From 9b6c3de9b4c2e745ea134c9b80ba345689520c08 Mon Sep 17 00:00:00 2001 From: Charly Medrano Date: Mon, 27 Jun 2022 18:14:52 +0200 Subject: [PATCH 01/14] Add Abs. spectrum and laser for carbazole --- .../01_carbazole/spectrum/coords.gen | 24 ++ .../01_carbazole/spectrum/dftb_in.hsd_spec | 40 +++ docs/_figures/elecdynamics/tutorial/PDI.png | Bin 0 -> 328050 bytes .../elecdynamics/tutorial/carbazole.png | Bin 0 -> 200068 bytes .../tutorial/molpopul-carbazole.png | Bin 0 -> 213448 bytes .../tutorial/spec-nm-carbazole.png | Bin 0 -> 16763 bytes .../tutorial/specs-comparison-damp.png | Bin 0 -> 25895 bytes docs/conf.py | 1 + docs/electronicdynamics/tutorial.rst | 228 ++++++++++++++++++ 9 files changed, 293 insertions(+) create mode 100644 docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/spectrum/coords.gen create mode 100644 docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/spectrum/dftb_in.hsd_spec create mode 100644 docs/_figures/elecdynamics/tutorial/PDI.png create mode 100644 docs/_figures/elecdynamics/tutorial/carbazole.png create mode 100644 docs/_figures/elecdynamics/tutorial/molpopul-carbazole.png create mode 100644 docs/_figures/elecdynamics/tutorial/spec-nm-carbazole.png create mode 100644 docs/_figures/elecdynamics/tutorial/specs-comparison-damp.png create mode 100644 docs/electronicdynamics/tutorial.rst diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/spectrum/coords.gen b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/spectrum/coords.gen new file mode 100644 index 00000000..ee4238d8 --- /dev/null +++ b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/spectrum/coords.gen @@ -0,0 +1,24 @@ +22 C +C H N + 1 1 -5.1728644000E-01 -7.2571119000E-01 5.5846500000E-03 + 2 1 8.5078177000E-01 -1.1301429800E+00 2.0378600000E-03 + 3 1 1.2261304100E+00 -2.4865873900E+00 -1.5372900000E-03 + 4 1 1.9994598000E-01 -3.4347336900E+00 -4.3233500000E-03 + 5 2 2.2839472400E+00 -2.7882631200E+00 -3.3389800000E-03 + 6 1 -1.1562943300E+00 -3.0498598500E+00 -2.9476600000E-03 + 7 2 4.5464746000E-01 -4.5055579500E+00 -8.7991900000E-03 + 8 1 -1.5299440000E+00 -1.7037797500E+00 2.9104100000E-03 + 9 2 -1.9330937600E+00 -3.8293745100E+00 -7.3501000000E-03 + 10 2 -2.5921016000E+00 -1.4158925700E+00 3.5784700000E-03 + 11 1 -5.1730828000E-01 7.2567935000E-01 5.8213800000E-03 + 12 1 8.5080047000E-01 1.1301031400E+00 0.0000000000E+00 + 13 3 1.6513735600E+00 -1.0210000000E-05 0.0000000000E+00 + 14 1 -1.5297530300E+00 1.7038648900E+00 8.4112200000E-03 + 15 1 -1.1559873900E+00 3.0499477100E+00 1.8125700000E-03 + 16 2 -2.5920072900E+00 1.4162563500E+00 1.4849170000E-02 + 17 1 2.0031694000E-01 3.4347032300E+00 -7.4452800000E-03 + 18 2 -1.9327718800E+00 3.8294924100E+00 2.8904500000E-03 + 19 1 1.2263781800E+00 2.4864970000E+00 -7.6315500000E-03 + 20 2 2.2841771200E+00 2.7882250200E+00 -1.4735950000E-02 + 21 2 4.5487270000E-01 4.5055017500E+00 -1.5258710000E-02 + 22 2 2.6797365300E+00 -1.0210000000E-05 -4.1508500000E-03 diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/spectrum/dftb_in.hsd_spec b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/spectrum/dftb_in.hsd_spec new file mode 100644 index 00000000..1e246bb0 --- /dev/null +++ b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/spectrum/dftb_in.hsd_spec @@ -0,0 +1,40 @@ +Geometry = GenFormat { + <<< "coords.gen" +} + +Driver = {} + +Hamiltonian = DFTB { + SCC = Yes + SCCTolerance = 1e-7 + MaxAngularMomentum = { + C = "p" + H = "s" + N = "p" + } + SlaterKosterFiles = Type2FileNames { + Prefix = "../../mio-1-1/" + Separator = "-" + Suffix = ".skf" + } +} + + ElectronDynamics = { + Steps = #define the time window + TimeStep [au] = #resolution of the spectrum + Perturbation = Kick { #must be a kick (Dirac delta) + PolarizationDirection = #desired direction/s + } + FieldStrength [v/a] = #Field strength of the perturbation + } + + +InputVersion = 21.2 + + +Parallel { + # Allow OMP threads explicitely to test for hybrid parallelisation with + # MPI-binary. 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For a list of options available for each theme, see the diff --git a/docs/electronicdynamics/tutorial.rst b/docs/electronicdynamics/tutorial.rst new file mode 100644 index 00000000..84db020c --- /dev/null +++ b/docs/electronicdynamics/tutorial.rst @@ -0,0 +1,228 @@ +.. highlight:: none + +*********************************************************************** +Tutorial first steps: Absorption spectra, analysis and charge transfer +*********************************************************************** + + +This is the tutorial presented in the DFTB+ school 2022 in Daresbury. The idea is to get used +to with the real-time TDDFTB method learning the basics of absorption spectra calculations and +photoinduced processes like charge transfer under irradiation. + +Spectra and analysis +==================== + +We will first calculate the absorption spectra of two different molecules and +analyse them using the tools provided by DFTB+. + +Calculation of the absorption spectrum of carbazole +--------------------------------------------------- + +We will calculate the absorption spectrum of the carbazole molecule + +1. Take a look at the input coordinates *coords.gen*. The *.gen* format + is the one used for DFTB+ code. In order to visualize the molecule, + you can use the ``gen2xyz`` script, provided in the installation of the + DFTB+ code, doing:: + + gen2xyz coords.gen + + This will generate a *coords.xyz* that you can open with VMD, Avogadro or + any other molecular visualization software of your choice. + + .. figure:: ../_figures/elecdynamics/tutorial/carbazole.png + :height: 30ex + :align: center + :alt: Carbazole molecule. + +2. Open the *dftb_in.hsd_spec* file. This is a template for the calculation + of the absorption spectrum. + + - Take a look at the ``ElectronDynamics`` block at the end of the file:: + + ElectronDynamics = { + Steps = #define the time window + TimeStep [au] = #resolution of the spectrum + Perturbation = Kick { #must be a kick (Dirac delta) + PolarizationDirection = #desired direction/s + } + FieldStrength [v/a] = #Field strength of the perturbation + } + + - The input variables to be considered for the calculation of the spectrum are four: + + * ``Steps`` (integer): the number of steps of the dynamics. It defines the time window and, + consequently, the energy window of the spectrum. The longer the dynamic, the lower the + energies that can be reached in the spectrum are (also afected by the timestep, of course). + Here, we will use 10000 steps. + * ``TimeStep`` (float): the time step in time units. Usually 0.2 a.u (0.0048 fs). + It defines the resolution of the spectrum. The smaller the time step, + the higher the resolution within the time window. + * ``Perturbation``: In this case we need a kick perturbation (Dirac delta) and we need to + specify the ``PolarizationDirection`` that could be *X*, *Y*, *Z* (if we are interested in + one particular direction) or *all* if we want to calculate the whole absorption spectrum. + Set it as *all*. + * ``FieldStrength`` (float): the field strength of the perturbation applied. For the + calculation of the absorption spectrum, it must be within the linear response regime, + i.e. usually 0.001 :math:`V/\AA`. + + - Complete the template file, copy it to *dftb_in.hsd* and run the calculation. + +3. Once the dynamics ended, we will have 3 components of the dynamical dipole moment + (*mux.dat*, *muy.dat*, *muz.dat*). We need to Fourier-transform these dipole components + in order to obtain the absorption spectrum of the molecule. To do this, we will use the + ``calc_timeprop_spectrum`` tool available after installation of DFTB+ under: + *dftbplus/tools/misc/*. In the folder + where you have the dipole files just type:: + + calc_timeprop_spectrum -d 4 -f 0.001 + + where the option -d is for the damping constant (in fs) applied to the dipole moment before transformation. + The option -f stands for the field strength (in V/AA) of the perturbation applied during dynamic. + +4. After running the script you will find two new files: *spec-nm.dat* and *spec-ev.dat* which are + the absorption spectra in nm and eV, respectively. Plot the spectrum file with the plotting tool + of your desire and look at the lower energy transitions. You should then see + an absorption spectrum similar to: + + .. figure:: ../_figures/elecdynamics/tutorial/spec-nm-carbazole.png + :width: 60% + :align: center + :alt: Absorption spectrum of carbazole molecule + + Absorption spectrum of carbazole molecule + +5. Change the damping constant for a higher value, recalculate the specctrum and plot both spectra + together. Which is the effect of the damping time in the spectrum? + Here it is an example of the same spectrum obtained before, calculated with + different values of the damping constant. + + .. figure:: ../_figures/elecdynamics/tutorial/specs-comparison-damp.png + :width: 60% + :align: center + :alt: Influence of the damping constant value ``d`` in the absorption spectrum. + + Influence of the damping constant value ``d`` in the absorption spectrum. + +Analysis of the absorption spectrum of carbazole +------------------------------------------------ + +We will consider a laser perturbation in tune with the lowest energy +transition of the molecule in order to study the photodynamic +process of absorption in this transition. In order to do this, we +need to know the energy of the lowest energy transition of +the molecule (look for it in the spectrum plotted in the previous calculation) +and calculate the direction of maximal polarization of the transition. + +1. Open the *dftb_in.hsd_laser* file. This is a template for the calculation + of a laser perturbation. + + - Take a look at the ``ElectronDynamics`` block at the end of the file:: + + ElectronDynamics = { + Steps = 10000 + TimeStep [au] = 0.2 + Perturbation = Laser{ # Laser type perturbation + LaserEnergy [nm] = # energy of interest + PolarizationDirection = # calculate with calc_timeprop_maxpoldir + } + FieldStrength [v/a] = 0.001 + Populations = Yes # to write populations during dynamic + } + + Now, the ``Perturbation`` type is a ``laser`` (and not anymore a ``kick``) + and we need to specify two parameters: + + * ``LaserEnergy`` (float): the energy of the applied laser that may be + the transition energy of interest. This value must be in energy units + like eV but also nm is possible. + * ``PolarizationDirection`` (vector): in the case of a laser, the + ``PolarizationDirection`` is 3-cartesian components vector in which the + laser will be applied. + + Also note that we turned on the ``Populations`` flag in order to write + the occupations during the dynamics. + +2. To complete the input template for the laser, we need to provide + the ``LaserEnergy`` and the ``PolarizationDirection`` of the laser. Based on + our previous calculated spectrum, calculate the direction of maximal + polarization of the lowest energy transition of the molecule. + + - Help: use the tool ``calc_timeprop_maxpoldir`` already available in + your installation (under: *dftbplus/tools/misc/*). To know how this + tool work the user can just type:: + + calc_timeprop_maxpoldir -h + + - Along which axes is the direction vector? How is this explained? + + - Hint: try to visualize the molecule and see how it is oriented with respect + to the cartesian axes. + + + Solution: If you choose the lower energy transition of carbazole you may do:: + + calc_timeprop_maxpoldir -10 -w 326 + + and you will obtain the following transition dipole vector:: + + PolarizationDirection = 0.99999221 0.00101174 -0.00381496 + + which is essentially paralel to the *X* cartesian direction + + +3. Prepare the input for the dynamics under a continuous laser perturbation. + Use the energy transition obtained from the spectrum as the ``LaserEnergy`` + and the vector obtained above as the ``PolarizationDirection`` of the + laser. + + - Why we should use this direction instead of any other? + +4. After the dynamics, take a look at the *mu.dat* file. + + - Is the dipole moment increasing linearly? + +5. Take a look at the *molpopul.dat* + generated. This file contains the populations projected on the GS orbitals during the dynamics. + + - Which orbitals are involved in the transition? + Help: you can plot the *molpopul.dat* file using xmgrace:: + + xmgrace -nxy molpopul.dat + + Look at the populations at y=2 (occupied orbitals in the GS basis) and find + which curves are decreasing during the dynamic. These are the orbitals + being depopulated. + Look at the populations at y=0 (unoccopied orbitals in the GS basis) and find + which curves are increasing during the dynamics. These are the orbitals + being populated. + +6. Let's generate those orbitals using ``waveplot`` + + - Look at the *waveplot_in.hsd_* template input file for waveplot: + + - Which files are needed? + - In which orbitals are we interested? + + - After editing and completing this file, just rename it to *waveplot_in.hsd* and run + ``waveplot`` using your current installed version that probably is at:: + + $HOME/dftbplus/_build/app/waveplot/waveplot + + - After running waveplot, a number of files would be generated starting with "wp-1-1". + +7. Let's plot these orbitals: + + - Open the cube files that correspond to the HOMO and LUMO and plot them as an isosurface. + (For a tutorial on the [Basics of VMD](https://www.ks.uiuc.edu/Training/SumSchool/materials/sources/tutorials/01-vmd-tutorial/html/node2.html) and/or plotting an [isosurface](https://www.ks.uiuc.edu/Research/vmd/current/ug/node77.html) method please refer to the links.) + +Here we show a figure with the Populations obtained from the laser dynamics +and the orbitals involved in the transition. You should get something +similar in your calculations: + +.. figure:: ../_figures/elecdynamics/tutorial/molpopul-carbazole.png + :width: 60% + :align: center + :alt: molpopul1-carbazole + + (left)Populations vs time for the laser dynamics. (right) Orbitals involved + in the lower energy transition of the carbazole molecule. 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Really good for rapid examinations. `Download VESTA `_ Here we show a figure with the Populations obtained from the laser dynamics and the orbitals involved in the transition. You should get something From 9d959fa2ffa1283723973c5470f255f8cf5fceb8 Mon Sep 17 00:00:00 2001 From: Charly Medrano Date: Thu, 30 Jun 2022 17:09:53 +0200 Subject: [PATCH 03/14] Add charge transfer part --- .../{spectrum => 01_spectrum}/coords.gen | 0 .../dftb_in.hsd_spec | 0 .../01_carbazole/02_laser/coords.gen | 24 ++ .../01_carbazole/02_laser/dftb_in.hsd_laser | 50 +++++ .../01_carbazole/02_laser/waveplot_in.hsd_ | 29 +++ .../01_aggregate_spec/coords.gen | 85 +++++++ .../01_aggregate_spec/dftb_in.hsd_spec | 41 ++++ .../02_aggregate_CT/calc_timeprop_charges.py | 50 +++++ .../02_aggregate_CT/coords.gen | 85 +++++++ .../02_aggregate_CT/dftb_in.hsd_pulse | 49 ++++ .../elecdynamics/tutorial/PDI+carbazole.png | Bin 0 -> 91003 bytes docs/_figures/elecdynamics/tutorial/PDI.png | Bin 328050 -> 228652 bytes .../elecdynamics/tutorial/charge-vs-time.png | Bin 0 -> 20717 bytes .../elecdynamics/tutorial/molpopul-CT.png | Bin 0 -> 19898 bytes .../tutorial/specs-compar-A+D.png | Bin 0 -> 23956 bytes docs/electronicdynamics/tutorial.rst | 211 +++++++++++++++++- 16 files changed, 623 insertions(+), 1 deletion(-) rename docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/{spectrum => 01_spectrum}/coords.gen (100%) rename docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/{spectrum => 01_spectrum}/dftb_in.hsd_spec (100%) create mode 100644 docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/coords.gen create mode 100644 docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/dftb_in.hsd_laser create mode 100644 docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/waveplot_in.hsd_ create mode 100644 docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/coords.gen create mode 100644 docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/dftb_in.hsd_spec create mode 100755 docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/calc_timeprop_charges.py create mode 100644 docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/coords.gen create mode 100644 docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/dftb_in.hsd_pulse create mode 100644 docs/_figures/elecdynamics/tutorial/PDI+carbazole.png create mode 100644 docs/_figures/elecdynamics/tutorial/charge-vs-time.png create mode 100644 docs/_figures/elecdynamics/tutorial/molpopul-CT.png create mode 100644 docs/_figures/elecdynamics/tutorial/specs-compar-A+D.png diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/spectrum/coords.gen b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/01_spectrum/coords.gen similarity index 100% rename from docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/spectrum/coords.gen rename to docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/01_spectrum/coords.gen diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/spectrum/dftb_in.hsd_spec b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/01_spectrum/dftb_in.hsd_spec similarity index 100% rename from docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/spectrum/dftb_in.hsd_spec rename to docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/01_spectrum/dftb_in.hsd_spec diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/coords.gen b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/coords.gen new file mode 100644 index 00000000..ee4238d8 --- /dev/null +++ b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/coords.gen @@ -0,0 +1,24 @@ +22 C +C H N + 1 1 -5.1728644000E-01 -7.2571119000E-01 5.5846500000E-03 + 2 1 8.5078177000E-01 -1.1301429800E+00 2.0378600000E-03 + 3 1 1.2261304100E+00 -2.4865873900E+00 -1.5372900000E-03 + 4 1 1.9994598000E-01 -3.4347336900E+00 -4.3233500000E-03 + 5 2 2.2839472400E+00 -2.7882631200E+00 -3.3389800000E-03 + 6 1 -1.1562943300E+00 -3.0498598500E+00 -2.9476600000E-03 + 7 2 4.5464746000E-01 -4.5055579500E+00 -8.7991900000E-03 + 8 1 -1.5299440000E+00 -1.7037797500E+00 2.9104100000E-03 + 9 2 -1.9330937600E+00 -3.8293745100E+00 -7.3501000000E-03 + 10 2 -2.5921016000E+00 -1.4158925700E+00 3.5784700000E-03 + 11 1 -5.1730828000E-01 7.2567935000E-01 5.8213800000E-03 + 12 1 8.5080047000E-01 1.1301031400E+00 0.0000000000E+00 + 13 3 1.6513735600E+00 -1.0210000000E-05 0.0000000000E+00 + 14 1 -1.5297530300E+00 1.7038648900E+00 8.4112200000E-03 + 15 1 -1.1559873900E+00 3.0499477100E+00 1.8125700000E-03 + 16 2 -2.5920072900E+00 1.4162563500E+00 1.4849170000E-02 + 17 1 2.0031694000E-01 3.4347032300E+00 -7.4452800000E-03 + 18 2 -1.9327718800E+00 3.8294924100E+00 2.8904500000E-03 + 19 1 1.2263781800E+00 2.4864970000E+00 -7.6315500000E-03 + 20 2 2.2841771200E+00 2.7882250200E+00 -1.4735950000E-02 + 21 2 4.5487270000E-01 4.5055017500E+00 -1.5258710000E-02 + 22 2 2.6797365300E+00 -1.0210000000E-05 -4.1508500000E-03 diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/dftb_in.hsd_laser b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/dftb_in.hsd_laser new file mode 100644 index 00000000..d1ed1796 --- /dev/null +++ b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/dftb_in.hsd_laser @@ -0,0 +1,50 @@ +Geometry = GenFormat { + <<< "coords.gen" +} + +Driver = {} + +Hamiltonian = DFTB { + SCC = Yes + SCCTolerance = 1e-7 + MaxAngularMomentum = { + C = "p" + H = "s" + N = "p" + } + SlaterKosterFiles = Type2FileNames { + Prefix = "../../mio-1-1/" + Separator = "-" + Suffix = ".skf" + } +} + + ElectronDynamics = { + Steps = 10000 + TimeStep [au] = 0.2 + Perturbation = Laser{ # Laser type perturbation + PolarizationDirection = # calculate with calc_timeprop_maxpoldir + LaserEnergy [ev] = # energy of interest + } + FieldStrength [v/a] = 0.001 + Populations = Yes # to write populations during dynamic + } + +Options { + WriteDetailedXML = Yes # needed for waveplot +} + +Analysis { + WriteEigenvectors = Yes # needed for waveplot +} + + +InputVersion = 21.2 + + +Parallel { + # Allow OMP threads explicitely to test for hybrid parallelisation with + # MPI-binary. (Check the manual before using this in production runs!) + UseOmpThreads = Yes +} + diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/waveplot_in.hsd_ b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/waveplot_in.hsd_ new file mode 100644 index 00000000..c66315a9 --- /dev/null +++ b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/waveplot_in.hsd_ @@ -0,0 +1,29 @@ +# General options + +Options { + RealComponent = Yes # Plot real component of the wavefunction + PlottedSpins = 1 -1 + PlottedLevels = ### Levels (Orbitals) to plot + PlottedRegion = OptimalCuboid {} # Region to plot + + NrOfPoints = 50 50 50 # Number of grid points in each direction + NrOfCachedGrids = -1 # Nr of cached grids (speeds up things) + Verbose = Yes # Wanna see a lot of messages? +} + +DetailedXml = "detailed.xml" # File containing the detailed xml output + # of DFTB+ +EigenvecBin = "eigenvec.bin" # File cointaining the binary eigenvecs + # Both files must be asked for the user in the + # input for DFTB+ calculation (they are not default + # printed) + + +# Definition of the basis +Basis { + Resolution = 0.01 + # Including mio-1-1.hsd. (If you use a set, which depends on other sets, + # the wfc.*.hsd files for each required set must be included in a similar + # way.) + <<+ "./.hsd" ### Path for Wave function coeffiecients for waveplot +} diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/coords.gen b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/coords.gen new file mode 100644 index 00000000..8cc5e96a --- /dev/null +++ b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/coords.gen @@ -0,0 +1,85 @@ +83 C +H C O N + 1 1 -7.5120000000E+00 -8.6200000000E-01 -6.3900000000E-01 + 2 1 -7.5140000000E+00 9.0200000000E-01 -5.6500000000E-01 + 3 2 -7.1380000000E+00 -2.0000000000E-03 -3.8000000000E-02 + 4 3 -5.7070000000E+00 -2.2740000000E+00 1.2000000000E-02 + 5 4 -5.6920000000E+00 1.0000000000E-03 -3.2000000000E-02 + 6 2 -5.0880000000E+00 -1.2620000000E+00 -2.0000000000E-03 + 7 3 -5.7050000000E+00 2.2760000000E+00 2.4000000000E-02 + 8 2 -5.0890000000E+00 1.2640000000E+00 4.0000000000E-03 + 9 2 -3.5790000000E+00 -1.2240000000E+00 -2.0000000000E-03 + 10 2 -2.8730000000E+00 -2.4250000000E+00 -1.0000000000E-03 + 11 1 -3.4320000000E+00 -3.3710000000E+00 -1.0000000000E-03 + 12 2 -3.5790000000E+00 1.2240000000E+00 3.0000000000E-03 + 13 2 -2.8570000000E+00 0.0000000000E+00 0.0000000000E+00 + 14 2 -1.4710000000E+00 -2.4370000000E+00 -1.0000000000E-03 + 15 2 -2.8730000000E+00 2.4250000000E+00 8.0000000000E-03 + 16 2 -1.4290000000E+00 0.0000000000E+00 0.0000000000E+00 + 17 1 -3.4320000000E+00 3.3710000000E+00 1.2000000000E-02 + 18 2 -7.3100000000E-01 -1.2480000000E+00 -1.0000000000E-03 + 19 1 -9.5900000000E-01 -3.4080000000E+00 -1.0000000000E-03 + 20 2 -1.4720000000E+00 2.4370000000E+00 7.0000000000E-03 + 21 2 -7.3100000000E-01 1.2480000000E+00 2.0000000000E-03 + 22 2 7.3100000000E-01 -1.2480000000E+00 0.0000000000E+00 + 23 1 7.3970000000E+00 -1.0140000000E+00 -1.8860000000E+00 + 24 2 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1.0881470000E+01 -1.6829100000E+00 -3.0233600000E+00 + 75 2 7.9344700000E+00 -4.5149100000E+00 -1.5243600000E+00 + 76 1 9.6784700000E+00 -3.5860100000E+00 -3.4893600000E+00 + 77 1 7.5764700000E+00 -5.3839100000E+00 -2.0933600000E+00 + 78 1 7.5784700000E+00 -3.6149100000E+00 -2.0473600000E+00 + 79 1 1.5091470000E+01 -6.8291000000E-01 -3.0063600000E+00 + 80 2 1.4309470000E+01 -1.4539100000E+00 -3.0113600000E+00 + 81 2 1.2959470000E+01 -1.0630100000E+00 -3.0163600000E+00 + 82 1 1.2712470000E+01 7.0900000000E-03 -3.0173600000E+00 + 83 1 7.5833600000E+00 -4.5407800000E+00 -5.1394000000E-01 diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/dftb_in.hsd_spec b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/dftb_in.hsd_spec new file mode 100644 index 00000000..ae4c9cdc --- /dev/null +++ b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/dftb_in.hsd_spec @@ -0,0 +1,41 @@ +Geometry = GenFormat { + <<< "coords.gen" +} + +Driver = {} + +Hamiltonian = DFTB { + SCC = Yes + SCCTolerance = 1e-7 + MaxAngularMomentum = { + C = "p" + H = "s" + N = "p" + O = "p" + } + SlaterKosterFiles = Type2FileNames { + Prefix = "../../mio-1-1/" + Separator = "-" + Suffix = ".skf" + } +} + + ElectronDynamics = { + Steps = 10000 #define the time window + TimeStep [au] = 0.2 #resolution of the spectrum + Perturbation = Kick { #must be a kick (Dirac delta) + PolarizationDirection = "all" #desired direction/s + } + FieldStrength [v/a] = 0.001 #Field strength of the perturbation + } + + +InputVersion = 21.2 + + +Parallel { + # Allow OMP threads explicitely to test for hybrid parallelisation with + # MPI-binary. (Check the manual before using this in production runs!) + UseOmpThreads = Yes +} + diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/calc_timeprop_charges.py b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/calc_timeprop_charges.py new file mode 100755 index 00000000..bc2f0266 --- /dev/null +++ b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/calc_timeprop_charges.py @@ -0,0 +1,50 @@ +#!/usr/bin/env python3 + +''' +Charge per fragment of DFTB+ TD data +''' + +import sys +import optparse +import numpy as np + +USAGE = """usage: %prog -l ii:jj,ll:mm + +Reads output from TD calculation with external laser and produces net charges per fragment +(subtracting value at time = 0). + +Needs qsvst.dat file present in working directory.""" + +def main(): + parser = optparse.OptionParser(usage=USAGE) + parser.add_option("-l", "--list", type='str', action="store", dest="at_list", + help="list of atom indices starting from 1 (initial and final index separated by colons, ranges separated by commas)") + + (options, args) = parser.parse_args() + + print(options.at_list) + list_ranges = options.at_list.split(',') + nfrag = len(list_ranges) #number of fragments + idx_ini = np.zeros(nfrag, dtype=int) + idx_end = np.zeros(nfrag, dtype=int) + for ii, ir in enumerate(list_ranges): + ini_end = ir.split(':') + idx_ini[ii] = int(ini_end[0]) - 1 # because first index is 0 + idx_end[ii] = int(ini_end[1]) - 1 + + qsdata = np.genfromtxt('qsvst.dat') + time = qsdata[:,0] + natoms = qsdata.shape[1] - 2 + print ('Number of atoms = {}'.format(natoms)) + if any(idx_ini > natoms) or any(idx_end) > natoms+1: + print('List ranges above total number of atoms = {}'.format(natoms)) + sys.exit() + + for ii in range(nfrag): #sum of the atomic charges inside each fragment + print ('Fragment {}: from atom {} till {}'.format(ii, idx_ini[ii]+1, idx_end[ii]+1)) + q_fragment = qsdata[:,2+idx_ini[ii]:2+idx_end[ii]+1].sum(axis=1) + np.savetxt("charge_frag%s.dat"%(ii+1), np.column_stack((time, q_fragment-q_fragment[0]))) + +if __name__ == "__main__": + main() + diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/coords.gen b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/coords.gen new file mode 100644 index 00000000..8cc5e96a --- /dev/null +++ b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/coords.gen @@ -0,0 +1,85 @@ +83 C +H C O N + 1 1 -7.5120000000E+00 -8.6200000000E-01 -6.3900000000E-01 + 2 1 -7.5140000000E+00 9.0200000000E-01 -5.6500000000E-01 + 3 2 -7.1380000000E+00 -2.0000000000E-03 -3.8000000000E-02 + 4 3 -5.7070000000E+00 -2.2740000000E+00 1.2000000000E-02 + 5 4 -5.6920000000E+00 1.0000000000E-03 -3.2000000000E-02 + 6 2 -5.0880000000E+00 -1.2620000000E+00 -2.0000000000E-03 + 7 3 -5.7050000000E+00 2.2760000000E+00 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1.0881470000E+01 -1.6829100000E+00 -3.0233600000E+00 + 75 2 7.9344700000E+00 -4.5149100000E+00 -1.5243600000E+00 + 76 1 9.6784700000E+00 -3.5860100000E+00 -3.4893600000E+00 + 77 1 7.5764700000E+00 -5.3839100000E+00 -2.0933600000E+00 + 78 1 7.5784700000E+00 -3.6149100000E+00 -2.0473600000E+00 + 79 1 1.5091470000E+01 -6.8291000000E-01 -3.0063600000E+00 + 80 2 1.4309470000E+01 -1.4539100000E+00 -3.0113600000E+00 + 81 2 1.2959470000E+01 -1.0630100000E+00 -3.0163600000E+00 + 82 1 1.2712470000E+01 7.0900000000E-03 -3.0173600000E+00 + 83 1 7.5833600000E+00 -4.5407800000E+00 -5.1394000000E-01 diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/dftb_in.hsd_pulse b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/dftb_in.hsd_pulse new file mode 100644 index 00000000..94a27706 --- /dev/null +++ b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/dftb_in.hsd_pulse @@ -0,0 +1,49 @@ +Geometry = GenFormat { + <<< "coords.gen" +} + +Driver = {} + +Hamiltonian = DFTB { + SCC = Yes + SCCTolerance = 1e-7 + MaxAngularMomentum = { + C = "p" + H = "s" + N = "p" + O = "p" + } + SlaterKosterFiles = Type2FileNames { + Prefix = "../../../mio-1-1/" + Separator = "-" + Suffix = ".skf" + } +} + + ElectronDynamics = { + Steps = 20000 + TimeStep [au] = 0.2 + Perturbation = Laser{ + PolarizationDirection = #calculate with calc_timeprop_maxpoldir + #for the energy of interest + LaserEnergy [nm] = + } + EnvelopeShape = Sin2{ #envelope shape type + Time1 [fs] = 30.0 #pulse duration (assuming Time0 = 0, by default) + } + FieldStrength [v/a] = 0.02 #field strength bigger than spectrum case (0.001) + WriteEnergyAndCharges = Yes + Populations = Yes + } + +Options { + WriteDetailedXML = Yes #needed for waveplot +} + +Analysis { + WriteEigenvectors = Yes #needed for waveplot +} + +InputVersion = 21.2 + + diff --git a/docs/_figures/elecdynamics/tutorial/PDI+carbazole.png 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zK^mP3j5fg0Da2k1Ot-#^qix~xtM^LR&a5+^8zwR)HgGX-P{q5yoorqn; z5(LA+S(`{FHDU6UbqEJj6ThD6PsCbKd57B-_WOKEtW4YIS;z>G#Gj0;-c4Z{y1ocjfJOL`h>JI?wYFT`edbhEC7ZOyh5`e@c(AxwThT~=Wai}+Y!prBs7Xd!ww~P z>-j%jph{f?Bxq#LP3>I{R(@L!n7zCsec36lVct9T*MmhC^)ow|(p~BAHeyZ}RvjS% jBmXn<`TuVS&EHk4=EIv%KAf9B?M+wPK&u$~ApHLTXXvpo literal 0 HcmV?d00001 diff --git a/docs/electronicdynamics/tutorial.rst b/docs/electronicdynamics/tutorial.rst index 763f30d0..74cbcd51 100644 --- a/docs/electronicdynamics/tutorial.rst +++ b/docs/electronicdynamics/tutorial.rst @@ -18,6 +18,8 @@ analyse them using the tools provided by DFTB+. Calculation of the absorption spectrum of carbazole --------------------------------------------------- +[Input: `recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/01_spectrum`] + We will calculate the absorption spectrum of the carbazole molecule 1. Take a look at the input coordinates *coords.gen*. The *.gen* format @@ -107,6 +109,8 @@ We will calculate the absorption spectrum of the carbazole molecule Analysis of the absorption spectrum of carbazole ------------------------------------------------ +[Input: `recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser`] + We will consider a laser perturbation in tune with the lowest energy transition of the molecule in order to study the photodynamic process of absorption in this transition. In order to do this, we @@ -173,7 +177,6 @@ and calculate the direction of maximal polarization of the transition. which is essentially paralel to the *X* cartesian direction (because of the molecules orientation with respect to the cartesian axes) - 3. Prepare the input for the dynamics under a continuous laser perturbation. Use the energy transition obtained from the spectrum as the ``LaserEnergy`` and the vector obtained above as the ``PolarizationDirection`` of the @@ -255,3 +258,209 @@ similar in your calculations: (left)Populations vs time for the laser dynamics. (right) Orbitals involved in the lower energy transition of the carbazole molecule. + + +Now is your turn! Calculation of PDI absorption spectrum +-------------------------------------------------------- + +[Input: `recipes/electronicdynamics/tutorial/01_spectra_and_laser/02_PDI/] + +We will repeat the workflow used for the carbazole molecule with a new +molecule, PDI. + +1. Based on the calculations that you ran before. + + - Calculate the absorption spectrum with a proper *dftb_in.hsd* input file. + - Find the lowest energy transition. + - Study the excitation process using a laser tuned with the transition. + - Obtain the orbitals involved in the transition using waveplot and plot them. + +Here we leave some figures from our calculations that could be useful to +compare with your own calculations of this section: + +.. figure:: ../_figures/elecdynamics/tutorial/PDI.png + :width: 60% + :align: center + :alt: PDI + + \(a\) Absorption spectrum of the PDI molecule.\(b\) PDI molecule structure.\(c\) Dipole + moment components vs time during a laser dynamics at 548 nm (note that in + this case the dipole moment in the *X* direction increases linearly).\(d\) Populations + vs time for the laser dynamics.\(e\) Orbitals involved in the transition. + +Photoinduced charge transfer +============================ + +Calculate the absorption spectrum of the Donor-acceptor aggregate +----------------------------------------------------------------- + +[Input: `recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/`] + +1. Take a look at the input coordinates *coords.xyz* (you can open it using avogadro, +jmol, vmd, VESTA, etc). + +.. figure:: ../_figures/elecdynamics/tutorial/PDI+carbazole.png + :width: 60% + :align: center + :alt: PDI+carbazole aggregate + + PDI+carbazole derivatives aggregate + +It is an aggregate of the previous molecules analysed in which the carbazole and +PDI derivative act as donor and acceptor of electrons, respectively. + + - Convert the coordinates into *gen* format (use the ``xyz2gen`` script) and + calculate the absorption spectrum using the *dftb_in.hsd_spec* as a template + for the input (copy this file or rename it as *dftb_in.hsd*). + Note that after the electron dynamics, you will need (as before) to run the + Fourier transform of the induced dipole moment of the system (using the + ``calc_timeprop_spectrum`` tool) in order to obtain the spectrum. + +2. Compare the calculated spectrum with the individual ones (you can use the spectra + calculated before or recalculate them from these derivatives). Is there + relevant differences? + + .. figure:: ../_figures/elecdynamics/tutorial/specs-compar-A+D.png + :width: 60% + :align: center + :alt: A+D spectrum + + Absorption spectrum of the PDI+carbazole derivatives aggregate. + +3. We are interested in the dynamics upon ilumination of the acceptor molecule. For such + puropose, we will perform a laser dynamic in next step and for it, we need to calculate + the transition dipole direction of the absorption band at ~530 nm. Calculate this vector + using the `calc_timeprop_maxpoldir` tool. You shold obtain something similar to:: + + PolarizationDirection = -0.99977920 0.01776644 0.01122075 + + which is essentially the *X* direction (since the PDI molecule axis is + paralel to the *X* axis in the coordinates). + +Laser dynamics on the donor-acceptor aggregate for charge transfer +------------------------------------------------------------------ + +[Input: `recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/`] + +1. With the transition dipole moment vector calculated previously, prepare + your input for a laser-driven electron dynamics in tune with the acceptor (PDI) + lowest energy excitation. Use the *dftb_in.hsd_pulse* as a template. Note + that this time we add an envelope function to the laser perturbation in order + to mimick a laser pulse:: + + ElectronDynamics = { + Steps = 20000 + TimeStep [au] = 0.2 + Perturbation = Laser{ + PolarizationDirection = #calculate with calc_timeprop_maxpoldir + #for the energy of interest + LaserEnergy [nm] = + } + EnvelopeShape = Sin2{ #envelope shape type + Time1 [fs] = 30.0 #pulse duration (assuming Time0 = 0, by default) + } + FieldStrength [v/a] = 0.02 #field strength bigger than spectrum case (0.001) + WriteEnergyAndCharges = Yes + Populations = Yes + } + + Now in the ElectronDynamics we added the Sin2 ``EnvelopeShape`` with + a duration of 30 fs starting at the beginning of the dynamics. We will + ask the code also to print the populations during dynamics to study the + mechanism of charge transfer. Complete the input template filling the + ``PolarizationDirection`` and ``LaserEnergy`` obtained before and run the + code (don't forget to rename the template to *dftb_in.hsd*). + +2. After running the electron dynamics, let inspect what give us de *qsvst.dat* + file:: + + # time (fs) | total net charge (e) | charge (atom_1) (e) | ... | charge (atom_N) (e)| + 0.000000000000000 -0.000000000000055 0.075753114169209 0.077680106829215 ... + 0.241888432650500 -0.000000000000048 0.075753940652948 0.077680933651269 ... + 0.483776865301000 -0.000000000000049 0.075758821681684 0.077685768802125 ... + + The first column of the file is the time and the second one is the total net charge + of the system at each time step (which should keep near to zero). After that, we + have one column for every atom charge at each time step (summing a total of N columns + being N the number of atoms in the system). + Making use of the file *qsvst.dat* one may potencially get information + about partial charges moving during dynamics. If you are interested in what is + happening with the charge of one molecule in your system, then you could sum the + atom charges corresponding to that molecule (or part) of the system at each time + and get some insights. + +3. As we are interested in the charge transfer between both molecules after the pulse + we want to process the information contained in the *qsvst.dat* to obtain the total + charge of each molecule during the dynamics. For that, you could develope your own + script but we also provide you a simple script based on this case to get that + information. The provided tool ``calc_timeprop_charges.py`` will do the job. + Try:: + + ./calc_timeprop_charges.py --help + + to get info about how to use the script:: + + usage: calc_timeprop_charges.py -l ii:jj,ll:mm + + Reads output from TD calculation with external laser and produces net charges per fragment + (subtracting value at time = 0). + + Needs qsvst.dat file present in working directory. + + Options: + -h, --help show this help message and exit + -l AT_LIST, --list=AT_LIST + list of atom indices starting from 1 (initial and + final index separated by colons, ranges separated by + commas) + + You will have to define the ranges of atoms that correspond to each of + the two molecules. In our case, the PDI derivative is between atom 1 and 52 + and the carbazole derivative is between atom 53 and 83. Then, you may do:: + + ./calc_timeprop_charges.py -l 1:52,53:83 + + After runing the script, two files may be generated: *charge_frag1.dat* and + *charge_frag2.dat* with the corresponding charges of each defined fragment. + If you plot it you will something like: + + .. figure:: ../_figures/elecdynamics/tutorial/charge-vs-time.png + :width: 60% + :align: center + :alt: charge vs time + + Charge vs time for the accpetor and donor molecules. + + where it is clearly shown that during the dynamic the PDI molecule act as + an accpetor of electrons getting negative values, meanwhile the carbazole is + getting positive. This confirm the charge transfer upon ilumination. + If we follow the protocol from before, ploting the populations and searching + for the orbitals involved in the transition, we should be able to get some + insigths on the mechanism of the charge transfer (follow the steps in the + prevous sections). As it is shown in the figure: + + .. figure:: ../_figures/elecdynamics/tutorial/molpopul-CT.png + :width: 60% + :align: center + :alt: molpopul CT + + (left)Populations vs time for the pulse dynamics. (right) Orbitals involved + in the excitation during the dynamics. + + the orbitals involved in the excitation with the pulse are localized in the + PDI molecule, i.e. we can confirm that we are exciting the PDI molecule in + its own HOMO-LUMO transition (and not an HOMO-LUMO transition of the whole + system). Comparing with the previous figure of the charges dynamics, we can + also see that the CT process start just after a certain amount of electrons + are excited in the PDI molecule (more or less 30 fs, the duration of the pulse + used). So we could in principle divide the mechanism in two steps. The first + one, from 0 to ~30 fs where the PDI is beeing excited. The second step is the + charge transfer from the carbazole to the PDI once the last is already excited. + + + + + + + + From 23eaf3a37d92d3421b52d1f9ae699c4f59c5534e Mon Sep 17 00:00:00 2001 From: Charly Medrano Date: Thu, 30 Jun 2022 17:17:07 +0200 Subject: [PATCH 04/14] Fix figure pops --- .../elecdynamics/tutorial/molpopul-CT.png | Bin 19898 -> 183253 bytes docs/electronicdynamics/tutorial.rst | 2 ++ 2 files changed, 2 insertions(+) diff --git a/docs/_figures/elecdynamics/tutorial/molpopul-CT.png b/docs/_figures/elecdynamics/tutorial/molpopul-CT.png index 08ca2701361578d61498fad0cf82d4eb5188522a..4b29320407f48bf7a65e3738ae218599399fb46a 100644 GIT binary patch literal 183253 zcmeFZWmFv7wl<8@xVuAe4HDcfxVyUs8h3YhcL+|<1b2504#C~s;q86jbMANdzGHm9 z-k+yO)u`3AR@bVUYw9y+b%dh4BoaJ6JQx@llGIl*WiT+PS}-t(A^-&FOyG=B8t4G- zq%0`{Ry|301p4A`rYU7ECkI9cY6HNa!12ML{~7|?1;7dZyDb4u0|xnD=RwyAvjT(q z*BE)w@vo0IX#eXs|Mv))5B{&wpmX^U{~irhn-BT#Hbl{1KXZ@NCI=nhfM2zoKsUVj 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So we could in principle divide the mechanism in two steps. The first one, from 0 to ~30 fs where the PDI is beeing excited. The second step is the charge transfer from the carbazole to the PDI once the last is already excited. + + From 7584fd1a36fd47d776638d2cd661528fae555bcc Mon Sep 17 00:00:00 2001 From: Charly Medrano Date: Fri, 1 Jul 2022 14:59:16 +0200 Subject: [PATCH 05/14] Final fix and refs --- .../01_carbazole/01_spectrum/dftb_in.hsd_spec | 2 +- .../01_carbazole/02_laser/dftb_in.hsd_laser | 2 +- .../01_carbazole/02_laser/waveplot_in.hsd_ | 2 +- .../01_spectra_and_laser/02_PDI/coords.gen | 42 +++++++ .../01_aggregate_spec/dftb_in.hsd_spec | 2 +- .../02_aggregate_CT/dftb_in.hsd_pulse | 2 +- docs/electronicdynamics/index.rst | 1 + docs/electronicdynamics/tutorial.rst | 110 +++++++++++------- 8 files changed, 113 insertions(+), 50 deletions(-) create mode 100644 docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/02_PDI/coords.gen diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/01_spectrum/dftb_in.hsd_spec b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/01_spectrum/dftb_in.hsd_spec index 1e246bb0..cb31d61b 100644 --- a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/01_spectrum/dftb_in.hsd_spec +++ b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/01_spectrum/dftb_in.hsd_spec @@ -13,7 +13,7 @@ Hamiltonian = DFTB { N = "p" } SlaterKosterFiles = Type2FileNames { - Prefix = "../../mio-1-1/" + Prefix = "../../../../slakos/download/mio-1-1/" Separator = "-" Suffix = ".skf" } diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/dftb_in.hsd_laser b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/dftb_in.hsd_laser index d1ed1796..752094a3 100644 --- a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/dftb_in.hsd_laser +++ b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/dftb_in.hsd_laser @@ -13,7 +13,7 @@ Hamiltonian = DFTB { N = "p" } SlaterKosterFiles = Type2FileNames { - Prefix = "../../mio-1-1/" + Prefix = "../../../../slakos/download/mio-1-1/" Separator = "-" Suffix = ".skf" } diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/waveplot_in.hsd_ b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/waveplot_in.hsd_ index c66315a9..ce881875 100644 --- a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/waveplot_in.hsd_ +++ b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/waveplot_in.hsd_ @@ -25,5 +25,5 @@ Basis { # Including mio-1-1.hsd. (If you use a set, which depends on other sets, # the wfc.*.hsd files for each required set must be included in a similar # way.) - <<+ "./.hsd" ### Path for Wave function coeffiecients for waveplot + <<+ "../../../../slakos/wfc/wfc.mio-1-1.hsd" ### Path for Wave function coeffiecients for waveplot } diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/02_PDI/coords.gen b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/02_PDI/coords.gen new file mode 100644 index 00000000..6bb60f85 --- /dev/null +++ b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/02_PDI/coords.gen @@ -0,0 +1,42 @@ +40 C +C H N O + 1 1 -2.8702011600E+00 0.0000000000E+00 0.0000000000E+00 + 2 1 -1.4362663100E+00 0.0000000000E+00 1.3000000000E-07 + 3 1 -3.5889101500E+00 -1.2350464400E+00 -2.3000000000E-07 + 4 1 -2.8813199700E+00 -2.4379174600E+00 -2.1000000000E-07 + 5 1 -1.4787678500E+00 -2.4440123700E+00 1.1000000000E-07 + 6 1 -7.3366388000E-01 -1.2519893100E+00 3.1000000000E-07 + 7 1 -3.5889101500E+00 1.2350464400E+00 0.0000000000E+00 + 8 1 -2.8813199600E+00 2.4379174600E+00 5.0000000000E-08 + 9 1 -1.4787678400E+00 2.4440123900E+00 0.0000000000E+00 + 10 1 -7.3366389000E-01 1.2519893100E+00 2.0000000000E-08 + 11 1 7.3366387000E-01 -1.2519893000E+00 5.5000000000E-07 + 12 1 1.4362663200E+00 1.0000000000E-08 2.6000000000E-07 + 13 1 7.3366387000E-01 1.2519893100E+00 -7.0000000000E-08 + 14 1 1.4787678400E+00 -2.4440123700E+00 9.5000000000E-07 + 15 1 2.8813199500E+00 -2.4379174700E+00 9.2000000000E-07 + 16 1 3.5889101400E+00 -1.2350464400E+00 5.1000000000E-07 + 17 1 2.8702011700E+00 2.0000000000E-08 2.3000000000E-07 + 18 1 3.5889101600E+00 1.2350464500E+00 -1.2000000000E-07 + 19 1 2.8813199600E+00 2.4379174700E+00 -5.4000000000E-07 + 20 1 1.4787678400E+00 2.4440123700E+00 -5.2000000000E-07 + 21 2 -3.4335673000E+00 -3.3896396100E+00 -4.6000000000E-07 + 22 2 -9.7502556000E-01 -3.4212878700E+00 1.4000000000E-07 + 23 2 -3.4335673300E+00 3.3896396100E+00 9.0000000000E-08 + 24 2 -9.7502557000E-01 3.4212879000E+00 -4.0000000000E-08 + 25 2 9.7502555000E-01 -3.4212878600E+00 1.2900000000E-06 + 26 2 3.4335673000E+00 -3.3896396100E+00 1.2100000000E-06 + 27 2 9.7502554000E-01 3.4212878700E+00 -8.9000000000E-07 + 28 2 3.4335672900E+00 3.3896396300E+00 -8.6000000000E-07 + 29 1 -5.0766344400E+00 -1.2425131600E+00 -6.6000000000E-07 + 30 1 -5.0766344500E+00 1.2425131500E+00 -4.0000000000E-08 + 31 1 5.0766344400E+00 -1.2425131700E+00 2.2000000000E-07 + 32 1 5.0766344600E+00 1.2425131600E+00 -6.0000000000E-08 + 33 3 -5.7159981400E+00 0.0000000000E+00 -4.1000000000E-07 + 34 3 5.7159981500E+00 -1.0000000000E-08 6.0000000000E-08 + 35 4 -5.7484785000E+00 -2.2718608200E+00 -1.2300000000E-06 + 36 4 -5.7484785300E+00 2.2718608200E+00 2.2000000000E-07 + 37 4 5.7484785100E+00 -2.2718608300E+00 1.1000000000E-07 + 38 4 5.7484785500E+00 2.2718607900E+00 -1.6000000000E-07 + 39 2 -6.7494873900E+00 0.0000000000E+00 -5.7000000000E-07 + 40 2 6.7494873800E+00 -4.0000000000E-08 -2.0000000000E-08 diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/dftb_in.hsd_spec b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/dftb_in.hsd_spec index ae4c9cdc..6886a940 100644 --- a/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/dftb_in.hsd_spec +++ b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/dftb_in.hsd_spec @@ -14,7 +14,7 @@ Hamiltonian = DFTB { O = "p" } SlaterKosterFiles = Type2FileNames { - Prefix = "../../mio-1-1/" + Prefix = "../../../slakos/download/mio-1-1/" Separator = "-" Suffix = ".skf" } diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/dftb_in.hsd_pulse b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/dftb_in.hsd_pulse index 94a27706..d8af1e29 100644 --- a/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/dftb_in.hsd_pulse +++ b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/dftb_in.hsd_pulse @@ -14,7 +14,7 @@ Hamiltonian = DFTB { O = "p" } SlaterKosterFiles = Type2FileNames { - Prefix = "../../../mio-1-1/" + Prefix = "../../../slakos/download/mio-1-1/" Separator = "-" Suffix = ".skf" } diff --git a/docs/electronicdynamics/index.rst b/docs/electronicdynamics/index.rst index 1b1e9d87..03ef7aac 100644 --- a/docs/electronicdynamics/index.rst +++ b/docs/electronicdynamics/index.rst @@ -24,3 +24,4 @@ and driving of nuclear motion via electronic excitation. spectra.rst driving.rst ehrenfest.rst + tutorial.rst diff --git a/docs/electronicdynamics/tutorial.rst b/docs/electronicdynamics/tutorial.rst index 8388d85c..40e28c2c 100644 --- a/docs/electronicdynamics/tutorial.rst +++ b/docs/electronicdynamics/tutorial.rst @@ -37,6 +37,8 @@ We will calculate the absorption spectrum of the carbazole molecule :align: center :alt: Carbazole molecule. + Carbazole molecule + 2. Open the *dftb_in.hsd_spec* file. This is a template for the calculation of the absorption spectrum. @@ -55,15 +57,15 @@ We will calculate the absorption spectrum of the carbazole molecule * ``Steps`` (integer): the number of steps of the dynamics. It defines the time window and, consequently, the energy window of the spectrum. The longer the dynamic, the lower the - energies that can be reached in the spectrum are (also afected by the timestep, of course). + energies that can be reached in the spectrum (also afected by the ``TimeStep``, of course). Here, we will use 10000 steps. * ``TimeStep`` (float): the time step in time units. Usually 0.2 a.u (0.0048 fs). It defines the resolution of the spectrum. The smaller the time step, the higher the resolution within the time window. * ``Perturbation``: In this case we need a kick perturbation (Dirac delta) and we need to specify the ``PolarizationDirection`` that could be *X*, *Y*, *Z* (if we are interested in - one particular direction) or *all* if we want to calculate the whole absorption spectrum. - Set it as *all*. + one particular direction) or ``all`` if we want to calculate the whole absorption spectrum. + Set it as ``all``. * ``FieldStrength`` (float): the field strength of the perturbation applied. For the calculation of the absorption spectrum, it must be within the linear response regime, i.e. usually 0.001 :math:`V/\AA`. @@ -71,7 +73,7 @@ We will calculate the absorption spectrum of the carbazole molecule - Complete the template file, copy it to *dftb_in.hsd* and run the calculation. 3. Once the dynamics ended, we will have 3 components of the dynamical dipole moment - (*mux.dat*, *muy.dat*, *muz.dat*). We need to Fourier-transform these dipole components + (*mux.dat*, muy.dat, *muz.dat*). We need to average and Fourier-transform these dipole components in order to obtain the absorption spectrum of the molecule. To do this, we will use the ``calc_timeprop_spectrum`` tool available after installation of DFTB+ under: *dftbplus/tools/misc/*. In the folder @@ -80,7 +82,7 @@ We will calculate the absorption spectrum of the carbazole molecule calc_timeprop_spectrum -d 4 -f 0.001 where the option -d is for the damping constant (in fs) applied to the dipole moment before transformation. - The option -f stands for the field strength (in V/AA) of the perturbation applied during dynamic. + The option -f stands for the field strength (in :math:`V/\AA`) of the perturbation applied during dynamic. 4. After running the script you will find two new files: *spec-nm.dat* and *spec-ev.dat* which are the absorption spectra in nm and eV, respectively. Plot the spectrum file with the plotting tool @@ -141,13 +143,13 @@ and calculate the direction of maximal polarization of the transition. the transition energy of interest. This value must be in energy units like eV but also nm is possible. * ``PolarizationDirection`` (vector): in the case of a laser, the - ``PolarizationDirection`` is 3-cartesian components vector in which the + ``PolarizationDirection`` is a 3-cartesian components vector in which the laser will be applied. Note that we turned on the ``Populations`` flag in order to write the occupations during the dynamics. Also note that we are asking for the detailed xml and the eigenvectors with the ``WriteDetailedXML`` - and ``WriteEigenvectors`` flags. We will need them to plot the orbitals + and ``WriteEigenvectors`` options. We will need them to plot the orbitals with waveplot in the following sections. 2. To complete the input template for the laser, we need to provide @@ -233,7 +235,7 @@ and calculate the direction of maximal polarization of the transition. - In which orbitals are we interested? - After editing and completing this file, just rename it to *waveplot_in.hsd* and run - ``waveplot`` using your current installed version that probably is at:: + ``waveplot`` using your current installed version that would be at:: $HOME/dftbplus/_build/app/waveplot/waveplot @@ -252,7 +254,7 @@ and the orbitals involved in the transition. You should get something similar in your calculations: .. figure:: ../_figures/elecdynamics/tutorial/molpopul-carbazole.png - :width: 60% + :width: 100% :align: center :alt: molpopul1-carbazole @@ -263,7 +265,7 @@ similar in your calculations: Now is your turn! Calculation of PDI absorption spectrum -------------------------------------------------------- -[Input: `recipes/electronicdynamics/tutorial/01_spectra_and_laser/02_PDI/] +[Input: `recipes/electronicdynamics/tutorial/01_spectra_and_laser/02_PDI/``] We will repeat the workflow used for the carbazole molecule with a new molecule, PDI. @@ -279,7 +281,7 @@ Here we leave some figures from our calculations that could be useful to compare with your own calculations of this section: .. figure:: ../_figures/elecdynamics/tutorial/PDI.png - :width: 60% + :width: 100% :align: center :alt: PDI @@ -291,30 +293,29 @@ compare with your own calculations of this section: Photoinduced charge transfer ============================ -Calculate the absorption spectrum of the Donor-acceptor aggregate +Calculate the absorption spectrum of a Donor-acceptor aggregate ----------------------------------------------------------------- [Input: `recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/`] 1. Take a look at the input coordinates *coords.xyz* (you can open it using avogadro, -jmol, vmd, VESTA, etc). - -.. figure:: ../_figures/elecdynamics/tutorial/PDI+carbazole.png - :width: 60% - :align: center - :alt: PDI+carbazole aggregate + jmol, vmd, VESTA, etc). - PDI+carbazole derivatives aggregate + .. figure:: ../_figures/elecdynamics/tutorial/PDI+carbazole.png + :width: 60% + :align: center + :alt: PDI+carbazole aggregate -It is an aggregate of the previous molecules analysed in which the carbazole and -PDI derivative act as donor and acceptor of electrons, respectively. + PDI+carbazole derivatives aggregate - - Convert the coordinates into *gen* format (use the ``xyz2gen`` script) and - calculate the absorption spectrum using the *dftb_in.hsd_spec* as a template - for the input (copy this file or rename it as *dftb_in.hsd*). - Note that after the electron dynamics, you will need (as before) to run the - Fourier transform of the induced dipole moment of the system (using the - ``calc_timeprop_spectrum`` tool) in order to obtain the spectrum. + It is an aggregate of the previous molecules analysed in which the carbazole and + PDI derivatives act as donor and acceptor of electrons, respectively. + - Convert the coordinates into *gen* format (use the ``xyz2gen`` script) and + calculate the absorption spectrum using the *dftb_in.hsd_spec* as a template + for the input (copy this file or rename it as *dftb_in.hsd*). + Note that after the electron dynamics, you will need (as before) to run the + Fourier transform of the induced dipole moment of the system (using the + ``calc_timeprop_spectrum`` tool) in order to obtain the spectrum. 2. Compare the calculated spectrum with the individual ones (you can use the spectra calculated before or recalculate them from these derivatives). Is there @@ -325,12 +326,14 @@ PDI derivative act as donor and acceptor of electrons, respectively. :align: center :alt: A+D spectrum - Absorption spectrum of the PDI+carbazole derivatives aggregate. + Absorption spectrum of the PDI+carbazole derivatives aggregate (in black), + compared to the individual spectrum for the PDI moiety (in orange) and + the carbazole moiety (in red). 3. We are interested in the dynamics upon ilumination of the acceptor molecule. For such puropose, we will perform a laser dynamic in next step and for it, we need to calculate the transition dipole direction of the absorption band at ~530 nm. Calculate this vector - using the `calc_timeprop_maxpoldir` tool. You shold obtain something similar to:: + using the ``calc_timeprop_maxpoldir`` tool. You shold obtain something similar to:: PolarizationDirection = -0.99977920 0.01776644 0.01122075 @@ -352,32 +355,32 @@ Laser dynamics on the donor-acceptor aggregate for charge transfer Steps = 20000 TimeStep [au] = 0.2 Perturbation = Laser{ - PolarizationDirection = #calculate with calc_timeprop_maxpoldir - #for the energy of interest + PolarizationDirection = #calculate with calc_timeprop_maxpoldir + #for the energy of interest LaserEnergy [nm] = } - EnvelopeShape = Sin2{ #envelope shape type - Time1 [fs] = 30.0 #pulse duration (assuming Time0 = 0, by default) + EnvelopeShape = Sin2{ #envelope shape type + Time1 [fs] = 30.0 #pulse duration (assuming Time0 = 0, by default) } - FieldStrength [v/a] = 0.02 #field strength bigger than spectrum case (0.001) + FieldStrength [v/a] = 0.02 #field strength bigger than spectrum case (0.001) WriteEnergyAndCharges = Yes Populations = Yes } Now in the ElectronDynamics we added the Sin2 ``EnvelopeShape`` with a duration of 30 fs starting at the beginning of the dynamics. We will - ask the code also to print the populations during dynamics to study the + also ask the code to print the populations during dynamics to study the mechanism of charge transfer. Complete the input template filling the ``PolarizationDirection`` and ``LaserEnergy`` obtained before and run the code (don't forget to rename the template to *dftb_in.hsd*). -2. After running the electron dynamics, let inspect what give us de *qsvst.dat* +2. After running the electron dynamics, let inspect what give us the *qsvst.dat* file:: - # time (fs) | total net charge (e) | charge (atom_1) (e) | ... | charge (atom_N) (e)| - 0.000000000000000 -0.000000000000055 0.075753114169209 0.077680106829215 ... - 0.241888432650500 -0.000000000000048 0.075753940652948 0.077680933651269 ... - 0.483776865301000 -0.000000000000049 0.075758821681684 0.077685768802125 ... + #time (fs) | total net charge (e) | charge (atom_1) (e) | ... | charge (atom_N) (e)| + 0.000000000000000 -0.000000000000055 0.075753114169209 0.077680106829215 ... + 0.241888432650500 -0.000000000000048 0.075753940652948 0.077680933651269 ... + 0.483776865301000 -0.000000000000049 0.075758821681684 0.077685768802125 ... The first column of the file is the time and the second one is the total net charge of the system at each time step (which should keep near to zero). After that, we @@ -422,7 +425,7 @@ Laser dynamics on the donor-acceptor aggregate for charge transfer After runing the script, two files may be generated: *charge_frag1.dat* and *charge_frag2.dat* with the corresponding charges of each defined fragment. - If you plot it you will something like: + If you plot it you will get something like: .. figure:: ../_figures/elecdynamics/tutorial/charge-vs-time.png :width: 60% @@ -437,10 +440,10 @@ Laser dynamics on the donor-acceptor aggregate for charge transfer If we follow the protocol from before, ploting the populations and searching for the orbitals involved in the transition, we should be able to get some insigths on the mechanism of the charge transfer (follow the steps in the - prevous sections). As it is shown in the figure: + previous sections). As it is shown in the figure: .. figure:: ../_figures/elecdynamics/tutorial/molpopul-CT.png - :width: 60% + :width: 100% :align: center :alt: molpopul CT @@ -457,12 +460,29 @@ Laser dynamics on the donor-acceptor aggregate for charge transfer one, from 0 to ~30 fs where the PDI is beeing excited. The second step is the charge transfer from the carbazole to the PDI once the last is already excited. +We hope that this tutorial would be helpful for those interested in get into the real-time TDDFTB +method using ``DFTB+``. Of course, this is just the beginning and there are much more possibilities +to do in terms of studyng optical properties and photoinduced processes within this approach in many +different scenarios and materials like *graphene nanoribbons*, *plasmonic nanoparticles*, *glod nanoclusters*, +*semiconductor nanoparticles* and *organic solar cells*. As an inspiration, we give you some references of +the last works performed with this method in ``DFTB+``: - +**Fano Resonance and Incoherent Interlayer Excitons in Molecular van der Waals Heterostructures.** Lien-Medrano, C. R., Bonafé, F. P., Yam, C. Y., Palma, C.-A., Sánchez, C. G., & Frauenheim, T. (2022). Nano Letters, 22(3), 911–917. `https://doi.org/10.1021/acs.nanolett.1c03441 `_ - +**Dynamical evolution of the Schottky barrier as a determinant contribution to electron-hole pair stabilization and photocatalysis of plasmon-induced hot carriers.** Berdakin, M., Soldano, G., Bonafé, F. P., Liubov, V., Aradi, B., Frauenheim, T., & Sánchez, C. G. (2022). Nanoscale, 14(7), 2816–2825. `https://doi.org/10.1039/d1nr04699c `_ + +**Photoinduced charge-transfer in chromophore-labeled gold nanoclusters: quantum evidence of the critical role of ligands and vibronic couplings.** Domínguez-Castro, A., Lien-Medrano, C. R., Maghrebi, K., Messaoudi, S., Frauenheim, T., & Fihey, A. (2021). Nanoscale, 13(14), 6786–6797. `https://doi.org/10.1039/D1NR00213A `_ + +**Interplay between Intra- And Interband Transitions Associated with the Plasmon-Induced Hot Carrier Generation Process in Silver and Gold Nanoclusters.** Berdakin, M., Douglas-Gallardo, O. A., & Sánchez, C. G. (2020). Journal of Physical Chemistry C, 1631–1639. `https://doi.org/10.1021/acs.jpcc.9b10871 `_ + +**Plasmon-induced hot-carrier generation differences in gold and silver nanoclusters.** Douglas-Gallardo, O. A., Berdakin, M., Frauenheim, T., & Sánchez, C. G. (2019). Nanoscale, 11(17), 8604–8615. `https://doi.org/10.1039/c9nr01352k `_ +**Trap-Door-Like Irreversible Photoinduced Charge Transfer in a Donor-Acceptor Complex.** Medrano, C. R., & Sánchez, C. G. (2018). Journal of Physical Chemistry Letters, 9(12), 3517–3524. `https://doi.org/10.1021/acs.jpclett.8b01043 `_ +**Quantum efficiency of the photo-induced electronic transfer in dye–TiO 2 complexes.** Marquez, D. M., & Sánchez, C. G. (2018). Physical Chemistry Chemical Physics, 20(41), 26280–26287. `https://doi.org/10.1039/C8CP04625E `_ +**Characterization of ZnO as substrate for DSSC.** Mansilla Wettstein, C., & Sánchez, C. G. (2018). Physical Chemistry Chemical Physics, 20(34), 21910–21916. `https://doi.org/10.1039/C8CP01709C `_ +**Plasmon-driven sub-picosecond breathing of metal nanoparticles.** Bonafé, F. P., Aradi, B., Guan, M., Douglas-Gallardo, O. A., Lian, C., Meng, S., Frauenheim, T., & Sánchez, C. G. (2017). Nanoscale, 9(34), 12391–12397. `https://doi.org/10.1039/C7NR04536K `_ +**Photoinduced charge-transfer dynamics simulations in noncovalently bonded molecular aggregates.** Medrano, C. R., Oviedo, M. B., & Sánchez, C. G. (2016). Physical Chemistry Chemical Physics, 18(22), 14840–14849. `https://doi.org/10.1039/c6cp00231e `_ From b073f85cde60420ec426fb069dbb9f48aa1e19be Mon Sep 17 00:00:00 2001 From: Charly Medrano Date: Mon, 27 Jun 2022 18:14:52 +0200 Subject: [PATCH 06/14] Add Abs. spectrum and laser for carbazole --- .../01_carbazole/spectrum/coords.gen | 24 ++ .../01_carbazole/spectrum/dftb_in.hsd_spec | 40 +++ docs/_figures/elecdynamics/tutorial/PDI.png | Bin 0 -> 328050 bytes .../elecdynamics/tutorial/carbazole.png | Bin 0 -> 200068 bytes .../tutorial/molpopul-carbazole.png | Bin 0 -> 213448 bytes .../tutorial/spec-nm-carbazole.png | Bin 0 -> 16763 bytes .../tutorial/specs-comparison-damp.png | Bin 0 -> 25895 bytes docs/electronicdynamics/tutorial.rst | 228 ++++++++++++++++++ 8 files changed, 292 insertions(+) create mode 100644 docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/spectrum/coords.gen create mode 100644 docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/spectrum/dftb_in.hsd_spec create mode 100644 docs/_figures/elecdynamics/tutorial/PDI.png create mode 100644 docs/_figures/elecdynamics/tutorial/carbazole.png create mode 100644 docs/_figures/elecdynamics/tutorial/molpopul-carbazole.png create mode 100644 docs/_figures/elecdynamics/tutorial/spec-nm-carbazole.png create mode 100644 docs/_figures/elecdynamics/tutorial/specs-comparison-damp.png create mode 100644 docs/electronicdynamics/tutorial.rst diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/spectrum/coords.gen b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/spectrum/coords.gen new file mode 100644 index 00000000..ee4238d8 --- /dev/null +++ b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/spectrum/coords.gen @@ -0,0 +1,24 @@ +22 C +C H N + 1 1 -5.1728644000E-01 -7.2571119000E-01 5.5846500000E-03 + 2 1 8.5078177000E-01 -1.1301429800E+00 2.0378600000E-03 + 3 1 1.2261304100E+00 -2.4865873900E+00 -1.5372900000E-03 + 4 1 1.9994598000E-01 -3.4347336900E+00 -4.3233500000E-03 + 5 2 2.2839472400E+00 -2.7882631200E+00 -3.3389800000E-03 + 6 1 -1.1562943300E+00 -3.0498598500E+00 -2.9476600000E-03 + 7 2 4.5464746000E-01 -4.5055579500E+00 -8.7991900000E-03 + 8 1 -1.5299440000E+00 -1.7037797500E+00 2.9104100000E-03 + 9 2 -1.9330937600E+00 -3.8293745100E+00 -7.3501000000E-03 + 10 2 -2.5921016000E+00 -1.4158925700E+00 3.5784700000E-03 + 11 1 -5.1730828000E-01 7.2567935000E-01 5.8213800000E-03 + 12 1 8.5080047000E-01 1.1301031400E+00 0.0000000000E+00 + 13 3 1.6513735600E+00 -1.0210000000E-05 0.0000000000E+00 + 14 1 -1.5297530300E+00 1.7038648900E+00 8.4112200000E-03 + 15 1 -1.1559873900E+00 3.0499477100E+00 1.8125700000E-03 + 16 2 -2.5920072900E+00 1.4162563500E+00 1.4849170000E-02 + 17 1 2.0031694000E-01 3.4347032300E+00 -7.4452800000E-03 + 18 2 -1.9327718800E+00 3.8294924100E+00 2.8904500000E-03 + 19 1 1.2263781800E+00 2.4864970000E+00 -7.6315500000E-03 + 20 2 2.2841771200E+00 2.7882250200E+00 -1.4735950000E-02 + 21 2 4.5487270000E-01 4.5055017500E+00 -1.5258710000E-02 + 22 2 2.6797365300E+00 -1.0210000000E-05 -4.1508500000E-03 diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/spectrum/dftb_in.hsd_spec b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/spectrum/dftb_in.hsd_spec new file mode 100644 index 00000000..1e246bb0 --- /dev/null +++ b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/spectrum/dftb_in.hsd_spec @@ -0,0 +1,40 @@ +Geometry = GenFormat { + <<< "coords.gen" +} + +Driver = {} + +Hamiltonian = DFTB { + SCC = Yes + SCCTolerance = 1e-7 + MaxAngularMomentum = { + C = "p" + H = "s" + N = "p" + } + SlaterKosterFiles = Type2FileNames { + Prefix = "../../mio-1-1/" + Separator = "-" + Suffix = ".skf" + } +} + + ElectronDynamics = { + Steps = #define the time window + TimeStep [au] = #resolution of the spectrum + Perturbation = Kick { #must be a kick (Dirac delta) + PolarizationDirection = #desired direction/s + } + FieldStrength [v/a] = #Field strength of the perturbation + } + + +InputVersion = 21.2 + + +Parallel { + # Allow OMP threads explicitely to test for hybrid parallelisation with + # MPI-binary. 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The idea is to get used +to with the real-time TDDFTB method learning the basics of absorption spectra calculations and +photoinduced processes like charge transfer under irradiation. + +Spectra and analysis +==================== + +We will first calculate the absorption spectra of two different molecules and +analyse them using the tools provided by DFTB+. + +Calculation of the absorption spectrum of carbazole +--------------------------------------------------- + +We will calculate the absorption spectrum of the carbazole molecule + +1. Take a look at the input coordinates *coords.gen*. The *.gen* format + is the one used for DFTB+ code. In order to visualize the molecule, + you can use the ``gen2xyz`` script, provided in the installation of the + DFTB+ code, doing:: + + gen2xyz coords.gen + + This will generate a *coords.xyz* that you can open with VMD, Avogadro or + any other molecular visualization software of your choice. + + .. figure:: ../_figures/elecdynamics/tutorial/carbazole.png + :height: 30ex + :align: center + :alt: Carbazole molecule. + +2. Open the *dftb_in.hsd_spec* file. This is a template for the calculation + of the absorption spectrum. + + - Take a look at the ``ElectronDynamics`` block at the end of the file:: + + ElectronDynamics = { + Steps = #define the time window + TimeStep [au] = #resolution of the spectrum + Perturbation = Kick { #must be a kick (Dirac delta) + PolarizationDirection = #desired direction/s + } + FieldStrength [v/a] = #Field strength of the perturbation + } + + - The input variables to be considered for the calculation of the spectrum are four: + + * ``Steps`` (integer): the number of steps of the dynamics. It defines the time window and, + consequently, the energy window of the spectrum. The longer the dynamic, the lower the + energies that can be reached in the spectrum are (also afected by the timestep, of course). + Here, we will use 10000 steps. + * ``TimeStep`` (float): the time step in time units. Usually 0.2 a.u (0.0048 fs). + It defines the resolution of the spectrum. The smaller the time step, + the higher the resolution within the time window. + * ``Perturbation``: In this case we need a kick perturbation (Dirac delta) and we need to + specify the ``PolarizationDirection`` that could be *X*, *Y*, *Z* (if we are interested in + one particular direction) or *all* if we want to calculate the whole absorption spectrum. + Set it as *all*. + * ``FieldStrength`` (float): the field strength of the perturbation applied. For the + calculation of the absorption spectrum, it must be within the linear response regime, + i.e. usually 0.001 :math:`V/\AA`. + + - Complete the template file, copy it to *dftb_in.hsd* and run the calculation. + +3. Once the dynamics ended, we will have 3 components of the dynamical dipole moment + (*mux.dat*, *muy.dat*, *muz.dat*). We need to Fourier-transform these dipole components + in order to obtain the absorption spectrum of the molecule. To do this, we will use the + ``calc_timeprop_spectrum`` tool available after installation of DFTB+ under: + *dftbplus/tools/misc/*. In the folder + where you have the dipole files just type:: + + calc_timeprop_spectrum -d 4 -f 0.001 + + where the option -d is for the damping constant (in fs) applied to the dipole moment before transformation. + The option -f stands for the field strength (in V/AA) of the perturbation applied during dynamic. + +4. After running the script you will find two new files: *spec-nm.dat* and *spec-ev.dat* which are + the absorption spectra in nm and eV, respectively. Plot the spectrum file with the plotting tool + of your desire and look at the lower energy transitions. You should then see + an absorption spectrum similar to: + + .. figure:: ../_figures/elecdynamics/tutorial/spec-nm-carbazole.png + :width: 60% + :align: center + :alt: Absorption spectrum of carbazole molecule + + Absorption spectrum of carbazole molecule + +5. Change the damping constant for a higher value, recalculate the specctrum and plot both spectra + together. Which is the effect of the damping time in the spectrum? + Here it is an example of the same spectrum obtained before, calculated with + different values of the damping constant. + + .. figure:: ../_figures/elecdynamics/tutorial/specs-comparison-damp.png + :width: 60% + :align: center + :alt: Influence of the damping constant value ``d`` in the absorption spectrum. + + Influence of the damping constant value ``d`` in the absorption spectrum. + +Analysis of the absorption spectrum of carbazole +------------------------------------------------ + +We will consider a laser perturbation in tune with the lowest energy +transition of the molecule in order to study the photodynamic +process of absorption in this transition. In order to do this, we +need to know the energy of the lowest energy transition of +the molecule (look for it in the spectrum plotted in the previous calculation) +and calculate the direction of maximal polarization of the transition. + +1. Open the *dftb_in.hsd_laser* file. This is a template for the calculation + of a laser perturbation. + + - Take a look at the ``ElectronDynamics`` block at the end of the file:: + + ElectronDynamics = { + Steps = 10000 + TimeStep [au] = 0.2 + Perturbation = Laser{ # Laser type perturbation + LaserEnergy [nm] = # energy of interest + PolarizationDirection = # calculate with calc_timeprop_maxpoldir + } + FieldStrength [v/a] = 0.001 + Populations = Yes # to write populations during dynamic + } + + Now, the ``Perturbation`` type is a ``laser`` (and not anymore a ``kick``) + and we need to specify two parameters: + + * ``LaserEnergy`` (float): the energy of the applied laser that may be + the transition energy of interest. This value must be in energy units + like eV but also nm is possible. + * ``PolarizationDirection`` (vector): in the case of a laser, the + ``PolarizationDirection`` is 3-cartesian components vector in which the + laser will be applied. + + Also note that we turned on the ``Populations`` flag in order to write + the occupations during the dynamics. + +2. To complete the input template for the laser, we need to provide + the ``LaserEnergy`` and the ``PolarizationDirection`` of the laser. Based on + our previous calculated spectrum, calculate the direction of maximal + polarization of the lowest energy transition of the molecule. + + - Help: use the tool ``calc_timeprop_maxpoldir`` already available in + your installation (under: *dftbplus/tools/misc/*). To know how this + tool work the user can just type:: + + calc_timeprop_maxpoldir -h + + - Along which axes is the direction vector? How is this explained? + + - Hint: try to visualize the molecule and see how it is oriented with respect + to the cartesian axes. + + + Solution: If you choose the lower energy transition of carbazole you may do:: + + calc_timeprop_maxpoldir -10 -w 326 + + and you will obtain the following transition dipole vector:: + + PolarizationDirection = 0.99999221 0.00101174 -0.00381496 + + which is essentially paralel to the *X* cartesian direction + + +3. Prepare the input for the dynamics under a continuous laser perturbation. + Use the energy transition obtained from the spectrum as the ``LaserEnergy`` + and the vector obtained above as the ``PolarizationDirection`` of the + laser. + + - Why we should use this direction instead of any other? + +4. After the dynamics, take a look at the *mu.dat* file. + + - Is the dipole moment increasing linearly? + +5. Take a look at the *molpopul.dat* + generated. This file contains the populations projected on the GS orbitals during the dynamics. + + - Which orbitals are involved in the transition? + Help: you can plot the *molpopul.dat* file using xmgrace:: + + xmgrace -nxy molpopul.dat + + Look at the populations at y=2 (occupied orbitals in the GS basis) and find + which curves are decreasing during the dynamic. These are the orbitals + being depopulated. + Look at the populations at y=0 (unoccopied orbitals in the GS basis) and find + which curves are increasing during the dynamics. These are the orbitals + being populated. + +6. Let's generate those orbitals using ``waveplot`` + + - Look at the *waveplot_in.hsd_* template input file for waveplot: + + - Which files are needed? + - In which orbitals are we interested? + + - After editing and completing this file, just rename it to *waveplot_in.hsd* and run + ``waveplot`` using your current installed version that probably is at:: + + $HOME/dftbplus/_build/app/waveplot/waveplot + + - After running waveplot, a number of files would be generated starting with "wp-1-1". + +7. Let's plot these orbitals: + + - Open the cube files that correspond to the HOMO and LUMO and plot them as an isosurface. + (For a tutorial on the [Basics of VMD](https://www.ks.uiuc.edu/Training/SumSchool/materials/sources/tutorials/01-vmd-tutorial/html/node2.html) and/or plotting an [isosurface](https://www.ks.uiuc.edu/Research/vmd/current/ug/node77.html) method please refer to the links.) + +Here we show a figure with the Populations obtained from the laser dynamics +and the orbitals involved in the transition. You should get something +similar in your calculations: + +.. figure:: ../_figures/elecdynamics/tutorial/molpopul-carbazole.png + :width: 60% + :align: center + :alt: molpopul1-carbazole + + (left)Populations vs time for the laser dynamics. (right) Orbitals involved + in the lower energy transition of the carbazole molecule. 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Really good for rapid examinations. `Download VESTA `_ Here we show a figure with the Populations obtained from the laser dynamics and the orbitals involved in the transition. You should get something From 25d90030552763a566d9d9dbe23759eafebefd61 Mon Sep 17 00:00:00 2001 From: Charly Medrano Date: Thu, 30 Jun 2022 17:09:53 +0200 Subject: [PATCH 08/14] Add charge transfer part --- .../{spectrum => 01_spectrum}/coords.gen | 0 .../dftb_in.hsd_spec | 0 .../01_carbazole/02_laser/coords.gen | 24 ++ .../01_carbazole/02_laser/dftb_in.hsd_laser | 50 +++++ .../01_carbazole/02_laser/waveplot_in.hsd_ | 29 +++ .../01_aggregate_spec/coords.gen | 85 +++++++ .../01_aggregate_spec/dftb_in.hsd_spec | 41 ++++ .../02_aggregate_CT/calc_timeprop_charges.py | 50 +++++ .../02_aggregate_CT/coords.gen | 85 +++++++ .../02_aggregate_CT/dftb_in.hsd_pulse | 49 ++++ .../elecdynamics/tutorial/PDI+carbazole.png | Bin 0 -> 91003 bytes docs/_figures/elecdynamics/tutorial/PDI.png | Bin 328050 -> 228652 bytes .../elecdynamics/tutorial/charge-vs-time.png | Bin 0 -> 20717 bytes .../elecdynamics/tutorial/molpopul-CT.png | Bin 0 -> 19898 bytes .../tutorial/specs-compar-A+D.png | Bin 0 -> 23956 bytes docs/electronicdynamics/tutorial.rst | 211 +++++++++++++++++- 16 files changed, 623 insertions(+), 1 deletion(-) rename docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/{spectrum => 01_spectrum}/coords.gen (100%) rename docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/{spectrum => 01_spectrum}/dftb_in.hsd_spec (100%) create mode 100644 docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/coords.gen create mode 100644 docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/dftb_in.hsd_laser create mode 100644 docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/waveplot_in.hsd_ create mode 100644 docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/coords.gen create mode 100644 docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/dftb_in.hsd_spec create mode 100755 docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/calc_timeprop_charges.py create mode 100644 docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/coords.gen create mode 100644 docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/dftb_in.hsd_pulse create mode 100644 docs/_figures/elecdynamics/tutorial/PDI+carbazole.png create mode 100644 docs/_figures/elecdynamics/tutorial/charge-vs-time.png create mode 100644 docs/_figures/elecdynamics/tutorial/molpopul-CT.png create mode 100644 docs/_figures/elecdynamics/tutorial/specs-compar-A+D.png diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/spectrum/coords.gen b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/01_spectrum/coords.gen similarity index 100% rename from docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/spectrum/coords.gen rename to docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/01_spectrum/coords.gen diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/spectrum/dftb_in.hsd_spec b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/01_spectrum/dftb_in.hsd_spec similarity index 100% rename from docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/spectrum/dftb_in.hsd_spec rename to docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/01_spectrum/dftb_in.hsd_spec diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/coords.gen b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/coords.gen new file mode 100644 index 00000000..ee4238d8 --- /dev/null +++ b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/coords.gen @@ -0,0 +1,24 @@ +22 C +C H N + 1 1 -5.1728644000E-01 -7.2571119000E-01 5.5846500000E-03 + 2 1 8.5078177000E-01 -1.1301429800E+00 2.0378600000E-03 + 3 1 1.2261304100E+00 -2.4865873900E+00 -1.5372900000E-03 + 4 1 1.9994598000E-01 -3.4347336900E+00 -4.3233500000E-03 + 5 2 2.2839472400E+00 -2.7882631200E+00 -3.3389800000E-03 + 6 1 -1.1562943300E+00 -3.0498598500E+00 -2.9476600000E-03 + 7 2 4.5464746000E-01 -4.5055579500E+00 -8.7991900000E-03 + 8 1 -1.5299440000E+00 -1.7037797500E+00 2.9104100000E-03 + 9 2 -1.9330937600E+00 -3.8293745100E+00 -7.3501000000E-03 + 10 2 -2.5921016000E+00 -1.4158925700E+00 3.5784700000E-03 + 11 1 -5.1730828000E-01 7.2567935000E-01 5.8213800000E-03 + 12 1 8.5080047000E-01 1.1301031400E+00 0.0000000000E+00 + 13 3 1.6513735600E+00 -1.0210000000E-05 0.0000000000E+00 + 14 1 -1.5297530300E+00 1.7038648900E+00 8.4112200000E-03 + 15 1 -1.1559873900E+00 3.0499477100E+00 1.8125700000E-03 + 16 2 -2.5920072900E+00 1.4162563500E+00 1.4849170000E-02 + 17 1 2.0031694000E-01 3.4347032300E+00 -7.4452800000E-03 + 18 2 -1.9327718800E+00 3.8294924100E+00 2.8904500000E-03 + 19 1 1.2263781800E+00 2.4864970000E+00 -7.6315500000E-03 + 20 2 2.2841771200E+00 2.7882250200E+00 -1.4735950000E-02 + 21 2 4.5487270000E-01 4.5055017500E+00 -1.5258710000E-02 + 22 2 2.6797365300E+00 -1.0210000000E-05 -4.1508500000E-03 diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/dftb_in.hsd_laser b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/dftb_in.hsd_laser new file mode 100644 index 00000000..d1ed1796 --- /dev/null +++ b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/dftb_in.hsd_laser @@ -0,0 +1,50 @@ +Geometry = GenFormat { + <<< "coords.gen" +} + +Driver = {} + +Hamiltonian = DFTB { + SCC = Yes + SCCTolerance = 1e-7 + MaxAngularMomentum = { + C = "p" + H = "s" + N = "p" + } + SlaterKosterFiles = Type2FileNames { + Prefix = "../../mio-1-1/" + Separator = "-" + Suffix = ".skf" + } +} + + ElectronDynamics = { + Steps = 10000 + TimeStep [au] = 0.2 + Perturbation = Laser{ # Laser type perturbation + PolarizationDirection = # calculate with calc_timeprop_maxpoldir + LaserEnergy [ev] = # energy of interest + } + FieldStrength [v/a] = 0.001 + Populations = Yes # to write populations during dynamic + } + +Options { + WriteDetailedXML = Yes # needed for waveplot +} + +Analysis { + WriteEigenvectors = Yes # needed for waveplot +} + + +InputVersion = 21.2 + + +Parallel { + # Allow OMP threads explicitely to test for hybrid parallelisation with + # MPI-binary. (Check the manual before using this in production runs!) + UseOmpThreads = Yes +} + diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/waveplot_in.hsd_ b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/waveplot_in.hsd_ new file mode 100644 index 00000000..c66315a9 --- /dev/null +++ b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/waveplot_in.hsd_ @@ -0,0 +1,29 @@ +# General options + +Options { + RealComponent = Yes # Plot real component of the wavefunction + PlottedSpins = 1 -1 + PlottedLevels = ### Levels (Orbitals) to plot + PlottedRegion = OptimalCuboid {} # Region to plot + + NrOfPoints = 50 50 50 # Number of grid points in each direction + NrOfCachedGrids = -1 # Nr of cached grids (speeds up things) + Verbose = Yes # Wanna see a lot of messages? +} + +DetailedXml = "detailed.xml" # File containing the detailed xml output + # of DFTB+ +EigenvecBin = "eigenvec.bin" # File cointaining the binary eigenvecs + # Both files must be asked for the user in the + # input for DFTB+ calculation (they are not default + # printed) + + +# Definition of the basis +Basis { + Resolution = 0.01 + # Including mio-1-1.hsd. (If you use a set, which depends on other sets, + # the wfc.*.hsd files for each required set must be included in a similar + # way.) + <<+ "./.hsd" ### Path for Wave function coeffiecients for waveplot +} diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/coords.gen b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/coords.gen new file mode 100644 index 00000000..8cc5e96a --- /dev/null +++ b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/coords.gen @@ -0,0 +1,85 @@ +83 C +H C O N + 1 1 -7.5120000000E+00 -8.6200000000E-01 -6.3900000000E-01 + 2 1 -7.5140000000E+00 9.0200000000E-01 -5.6500000000E-01 + 3 2 -7.1380000000E+00 -2.0000000000E-03 -3.8000000000E-02 + 4 3 -5.7070000000E+00 -2.2740000000E+00 1.2000000000E-02 + 5 4 -5.6920000000E+00 1.0000000000E-03 -3.2000000000E-02 + 6 2 -5.0880000000E+00 -1.2620000000E+00 -2.0000000000E-03 + 7 3 -5.7050000000E+00 2.2760000000E+00 2.4000000000E-02 + 8 2 -5.0890000000E+00 1.2640000000E+00 4.0000000000E-03 + 9 2 -3.5790000000E+00 -1.2240000000E+00 -2.0000000000E-03 + 10 2 -2.8730000000E+00 -2.4250000000E+00 -1.0000000000E-03 + 11 1 -3.4320000000E+00 -3.3710000000E+00 -1.0000000000E-03 + 12 2 -3.5790000000E+00 1.2240000000E+00 3.0000000000E-03 + 13 2 -2.8570000000E+00 0.0000000000E+00 0.0000000000E+00 + 14 2 -1.4710000000E+00 -2.4370000000E+00 -1.0000000000E-03 + 15 2 -2.8730000000E+00 2.4250000000E+00 8.0000000000E-03 + 16 2 -1.4290000000E+00 0.0000000000E+00 0.0000000000E+00 + 17 1 -3.4320000000E+00 3.3710000000E+00 1.2000000000E-02 + 18 2 -7.3100000000E-01 -1.2480000000E+00 -1.0000000000E-03 + 19 1 -9.5900000000E-01 -3.4080000000E+00 -1.0000000000E-03 + 20 2 -1.4720000000E+00 2.4370000000E+00 7.0000000000E-03 + 21 2 -7.3100000000E-01 1.2480000000E+00 2.0000000000E-03 + 22 2 7.3100000000E-01 -1.2480000000E+00 0.0000000000E+00 + 23 1 7.3970000000E+00 -1.0140000000E+00 -1.8860000000E+00 + 24 2 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1.0881470000E+01 -1.6829100000E+00 -3.0233600000E+00 + 75 2 7.9344700000E+00 -4.5149100000E+00 -1.5243600000E+00 + 76 1 9.6784700000E+00 -3.5860100000E+00 -3.4893600000E+00 + 77 1 7.5764700000E+00 -5.3839100000E+00 -2.0933600000E+00 + 78 1 7.5784700000E+00 -3.6149100000E+00 -2.0473600000E+00 + 79 1 1.5091470000E+01 -6.8291000000E-01 -3.0063600000E+00 + 80 2 1.4309470000E+01 -1.4539100000E+00 -3.0113600000E+00 + 81 2 1.2959470000E+01 -1.0630100000E+00 -3.0163600000E+00 + 82 1 1.2712470000E+01 7.0900000000E-03 -3.0173600000E+00 + 83 1 7.5833600000E+00 -4.5407800000E+00 -5.1394000000E-01 diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/dftb_in.hsd_spec b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/dftb_in.hsd_spec new file mode 100644 index 00000000..ae4c9cdc --- /dev/null +++ b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/dftb_in.hsd_spec @@ -0,0 +1,41 @@ +Geometry = GenFormat { + <<< "coords.gen" +} + +Driver = {} + +Hamiltonian = DFTB { + SCC = Yes + SCCTolerance = 1e-7 + MaxAngularMomentum = { + C = "p" + H = "s" + N = "p" + O = "p" + } + SlaterKosterFiles = Type2FileNames { + Prefix = "../../mio-1-1/" + Separator = "-" + Suffix = ".skf" + } +} + + ElectronDynamics = { + Steps = 10000 #define the time window + TimeStep [au] = 0.2 #resolution of the spectrum + Perturbation = Kick { #must be a kick (Dirac delta) + PolarizationDirection = "all" #desired direction/s + } + FieldStrength [v/a] = 0.001 #Field strength of the perturbation + } + + +InputVersion = 21.2 + + +Parallel { + # Allow OMP threads explicitely to test for hybrid parallelisation with + # MPI-binary. (Check the manual before using this in production runs!) + UseOmpThreads = Yes +} + diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/calc_timeprop_charges.py b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/calc_timeprop_charges.py new file mode 100755 index 00000000..bc2f0266 --- /dev/null +++ b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/calc_timeprop_charges.py @@ -0,0 +1,50 @@ +#!/usr/bin/env python3 + +''' +Charge per fragment of DFTB+ TD data +''' + +import sys +import optparse +import numpy as np + +USAGE = """usage: %prog -l ii:jj,ll:mm + +Reads output from TD calculation with external laser and produces net charges per fragment +(subtracting value at time = 0). + +Needs qsvst.dat file present in working directory.""" + +def main(): + parser = optparse.OptionParser(usage=USAGE) + parser.add_option("-l", "--list", type='str', action="store", dest="at_list", + help="list of atom indices starting from 1 (initial and final index separated by colons, ranges separated by commas)") + + (options, args) = parser.parse_args() + + print(options.at_list) + list_ranges = options.at_list.split(',') + nfrag = len(list_ranges) #number of fragments + idx_ini = np.zeros(nfrag, dtype=int) + idx_end = np.zeros(nfrag, dtype=int) + for ii, ir in enumerate(list_ranges): + ini_end = ir.split(':') + idx_ini[ii] = int(ini_end[0]) - 1 # because first index is 0 + idx_end[ii] = int(ini_end[1]) - 1 + + qsdata = np.genfromtxt('qsvst.dat') + time = qsdata[:,0] + natoms = qsdata.shape[1] - 2 + print ('Number of atoms = {}'.format(natoms)) + if any(idx_ini > natoms) or any(idx_end) > natoms+1: + print('List ranges above total number of atoms = {}'.format(natoms)) + sys.exit() + + for ii in range(nfrag): #sum of the atomic charges inside each fragment + print ('Fragment {}: from atom {} till {}'.format(ii, idx_ini[ii]+1, idx_end[ii]+1)) + q_fragment = qsdata[:,2+idx_ini[ii]:2+idx_end[ii]+1].sum(axis=1) + np.savetxt("charge_frag%s.dat"%(ii+1), np.column_stack((time, q_fragment-q_fragment[0]))) + +if __name__ == "__main__": + main() + diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/coords.gen b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/coords.gen new file mode 100644 index 00000000..8cc5e96a --- /dev/null +++ b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/coords.gen @@ -0,0 +1,85 @@ +83 C +H C O N + 1 1 -7.5120000000E+00 -8.6200000000E-01 -6.3900000000E-01 + 2 1 -7.5140000000E+00 9.0200000000E-01 -5.6500000000E-01 + 3 2 -7.1380000000E+00 -2.0000000000E-03 -3.8000000000E-02 + 4 3 -5.7070000000E+00 -2.2740000000E+00 1.2000000000E-02 + 5 4 -5.6920000000E+00 1.0000000000E-03 -3.2000000000E-02 + 6 2 -5.0880000000E+00 -1.2620000000E+00 -2.0000000000E-03 + 7 3 -5.7050000000E+00 2.2760000000E+00 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1.0881470000E+01 -1.6829100000E+00 -3.0233600000E+00 + 75 2 7.9344700000E+00 -4.5149100000E+00 -1.5243600000E+00 + 76 1 9.6784700000E+00 -3.5860100000E+00 -3.4893600000E+00 + 77 1 7.5764700000E+00 -5.3839100000E+00 -2.0933600000E+00 + 78 1 7.5784700000E+00 -3.6149100000E+00 -2.0473600000E+00 + 79 1 1.5091470000E+01 -6.8291000000E-01 -3.0063600000E+00 + 80 2 1.4309470000E+01 -1.4539100000E+00 -3.0113600000E+00 + 81 2 1.2959470000E+01 -1.0630100000E+00 -3.0163600000E+00 + 82 1 1.2712470000E+01 7.0900000000E-03 -3.0173600000E+00 + 83 1 7.5833600000E+00 -4.5407800000E+00 -5.1394000000E-01 diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/dftb_in.hsd_pulse b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/dftb_in.hsd_pulse new file mode 100644 index 00000000..94a27706 --- /dev/null +++ b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/dftb_in.hsd_pulse @@ -0,0 +1,49 @@ +Geometry = GenFormat { + <<< "coords.gen" +} + +Driver = {} + +Hamiltonian = DFTB { + SCC = Yes + SCCTolerance = 1e-7 + MaxAngularMomentum = { + C = "p" + H = "s" + N = "p" + O = "p" + } + SlaterKosterFiles = Type2FileNames { + Prefix = "../../../mio-1-1/" + Separator = "-" + Suffix = ".skf" + } +} + + ElectronDynamics = { + Steps = 20000 + TimeStep [au] = 0.2 + Perturbation = Laser{ + PolarizationDirection = #calculate with calc_timeprop_maxpoldir + #for the energy of interest + LaserEnergy [nm] = + } + EnvelopeShape = Sin2{ #envelope shape type + Time1 [fs] = 30.0 #pulse duration (assuming Time0 = 0, by default) + } + FieldStrength [v/a] = 0.02 #field strength bigger than spectrum case (0.001) + WriteEnergyAndCharges = Yes + Populations = Yes + } + +Options { + WriteDetailedXML = Yes #needed for waveplot +} + +Analysis { + WriteEigenvectors = Yes #needed for waveplot +} + +InputVersion = 21.2 + + diff --git a/docs/_figures/elecdynamics/tutorial/PDI+carbazole.png 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zK^mP3j5fg0Da2k1Ot-#^qix~xtM^LR&a5+^8zwR)HgGX-P{q5yoorqn; z5(LA+S(`{FHDU6UbqEJj6ThD6PsCbKd57B-_WOKEtW4YIS;z>G#Gj0;-c4Z{y1ocjfJOL`h>JI?wYFT`edbhEC7ZOyh5`e@c(AxwThT~=Wai}+Y!prBs7Xd!ww~P z>-j%jph{f?Bxq#LP3>I{R(@L!n7zCsec36lVct9T*MmhC^)ow|(p~BAHeyZ}RvjS% jBmXn<`TuVS&EHk4=EIv%KAf9B?M+wPK&u$~ApHLTXXvpo literal 0 HcmV?d00001 diff --git a/docs/electronicdynamics/tutorial.rst b/docs/electronicdynamics/tutorial.rst index 763f30d0..74cbcd51 100644 --- a/docs/electronicdynamics/tutorial.rst +++ b/docs/electronicdynamics/tutorial.rst @@ -18,6 +18,8 @@ analyse them using the tools provided by DFTB+. Calculation of the absorption spectrum of carbazole --------------------------------------------------- +[Input: `recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/01_spectrum`] + We will calculate the absorption spectrum of the carbazole molecule 1. Take a look at the input coordinates *coords.gen*. The *.gen* format @@ -107,6 +109,8 @@ We will calculate the absorption spectrum of the carbazole molecule Analysis of the absorption spectrum of carbazole ------------------------------------------------ +[Input: `recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser`] + We will consider a laser perturbation in tune with the lowest energy transition of the molecule in order to study the photodynamic process of absorption in this transition. In order to do this, we @@ -173,7 +177,6 @@ and calculate the direction of maximal polarization of the transition. which is essentially paralel to the *X* cartesian direction (because of the molecules orientation with respect to the cartesian axes) - 3. Prepare the input for the dynamics under a continuous laser perturbation. Use the energy transition obtained from the spectrum as the ``LaserEnergy`` and the vector obtained above as the ``PolarizationDirection`` of the @@ -255,3 +258,209 @@ similar in your calculations: (left)Populations vs time for the laser dynamics. (right) Orbitals involved in the lower energy transition of the carbazole molecule. + + +Now is your turn! Calculation of PDI absorption spectrum +-------------------------------------------------------- + +[Input: `recipes/electronicdynamics/tutorial/01_spectra_and_laser/02_PDI/] + +We will repeat the workflow used for the carbazole molecule with a new +molecule, PDI. + +1. Based on the calculations that you ran before. + + - Calculate the absorption spectrum with a proper *dftb_in.hsd* input file. + - Find the lowest energy transition. + - Study the excitation process using a laser tuned with the transition. + - Obtain the orbitals involved in the transition using waveplot and plot them. + +Here we leave some figures from our calculations that could be useful to +compare with your own calculations of this section: + +.. figure:: ../_figures/elecdynamics/tutorial/PDI.png + :width: 60% + :align: center + :alt: PDI + + \(a\) Absorption spectrum of the PDI molecule.\(b\) PDI molecule structure.\(c\) Dipole + moment components vs time during a laser dynamics at 548 nm (note that in + this case the dipole moment in the *X* direction increases linearly).\(d\) Populations + vs time for the laser dynamics.\(e\) Orbitals involved in the transition. + +Photoinduced charge transfer +============================ + +Calculate the absorption spectrum of the Donor-acceptor aggregate +----------------------------------------------------------------- + +[Input: `recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/`] + +1. Take a look at the input coordinates *coords.xyz* (you can open it using avogadro, +jmol, vmd, VESTA, etc). + +.. figure:: ../_figures/elecdynamics/tutorial/PDI+carbazole.png + :width: 60% + :align: center + :alt: PDI+carbazole aggregate + + PDI+carbazole derivatives aggregate + +It is an aggregate of the previous molecules analysed in which the carbazole and +PDI derivative act as donor and acceptor of electrons, respectively. + + - Convert the coordinates into *gen* format (use the ``xyz2gen`` script) and + calculate the absorption spectrum using the *dftb_in.hsd_spec* as a template + for the input (copy this file or rename it as *dftb_in.hsd*). + Note that after the electron dynamics, you will need (as before) to run the + Fourier transform of the induced dipole moment of the system (using the + ``calc_timeprop_spectrum`` tool) in order to obtain the spectrum. + +2. Compare the calculated spectrum with the individual ones (you can use the spectra + calculated before or recalculate them from these derivatives). Is there + relevant differences? + + .. figure:: ../_figures/elecdynamics/tutorial/specs-compar-A+D.png + :width: 60% + :align: center + :alt: A+D spectrum + + Absorption spectrum of the PDI+carbazole derivatives aggregate. + +3. We are interested in the dynamics upon ilumination of the acceptor molecule. For such + puropose, we will perform a laser dynamic in next step and for it, we need to calculate + the transition dipole direction of the absorption band at ~530 nm. Calculate this vector + using the `calc_timeprop_maxpoldir` tool. You shold obtain something similar to:: + + PolarizationDirection = -0.99977920 0.01776644 0.01122075 + + which is essentially the *X* direction (since the PDI molecule axis is + paralel to the *X* axis in the coordinates). + +Laser dynamics on the donor-acceptor aggregate for charge transfer +------------------------------------------------------------------ + +[Input: `recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/`] + +1. With the transition dipole moment vector calculated previously, prepare + your input for a laser-driven electron dynamics in tune with the acceptor (PDI) + lowest energy excitation. Use the *dftb_in.hsd_pulse* as a template. Note + that this time we add an envelope function to the laser perturbation in order + to mimick a laser pulse:: + + ElectronDynamics = { + Steps = 20000 + TimeStep [au] = 0.2 + Perturbation = Laser{ + PolarizationDirection = #calculate with calc_timeprop_maxpoldir + #for the energy of interest + LaserEnergy [nm] = + } + EnvelopeShape = Sin2{ #envelope shape type + Time1 [fs] = 30.0 #pulse duration (assuming Time0 = 0, by default) + } + FieldStrength [v/a] = 0.02 #field strength bigger than spectrum case (0.001) + WriteEnergyAndCharges = Yes + Populations = Yes + } + + Now in the ElectronDynamics we added the Sin2 ``EnvelopeShape`` with + a duration of 30 fs starting at the beginning of the dynamics. We will + ask the code also to print the populations during dynamics to study the + mechanism of charge transfer. Complete the input template filling the + ``PolarizationDirection`` and ``LaserEnergy`` obtained before and run the + code (don't forget to rename the template to *dftb_in.hsd*). + +2. After running the electron dynamics, let inspect what give us de *qsvst.dat* + file:: + + # time (fs) | total net charge (e) | charge (atom_1) (e) | ... | charge (atom_N) (e)| + 0.000000000000000 -0.000000000000055 0.075753114169209 0.077680106829215 ... + 0.241888432650500 -0.000000000000048 0.075753940652948 0.077680933651269 ... + 0.483776865301000 -0.000000000000049 0.075758821681684 0.077685768802125 ... + + The first column of the file is the time and the second one is the total net charge + of the system at each time step (which should keep near to zero). After that, we + have one column for every atom charge at each time step (summing a total of N columns + being N the number of atoms in the system). + Making use of the file *qsvst.dat* one may potencially get information + about partial charges moving during dynamics. If you are interested in what is + happening with the charge of one molecule in your system, then you could sum the + atom charges corresponding to that molecule (or part) of the system at each time + and get some insights. + +3. As we are interested in the charge transfer between both molecules after the pulse + we want to process the information contained in the *qsvst.dat* to obtain the total + charge of each molecule during the dynamics. For that, you could develope your own + script but we also provide you a simple script based on this case to get that + information. The provided tool ``calc_timeprop_charges.py`` will do the job. + Try:: + + ./calc_timeprop_charges.py --help + + to get info about how to use the script:: + + usage: calc_timeprop_charges.py -l ii:jj,ll:mm + + Reads output from TD calculation with external laser and produces net charges per fragment + (subtracting value at time = 0). + + Needs qsvst.dat file present in working directory. + + Options: + -h, --help show this help message and exit + -l AT_LIST, --list=AT_LIST + list of atom indices starting from 1 (initial and + final index separated by colons, ranges separated by + commas) + + You will have to define the ranges of atoms that correspond to each of + the two molecules. In our case, the PDI derivative is between atom 1 and 52 + and the carbazole derivative is between atom 53 and 83. Then, you may do:: + + ./calc_timeprop_charges.py -l 1:52,53:83 + + After runing the script, two files may be generated: *charge_frag1.dat* and + *charge_frag2.dat* with the corresponding charges of each defined fragment. + If you plot it you will something like: + + .. figure:: ../_figures/elecdynamics/tutorial/charge-vs-time.png + :width: 60% + :align: center + :alt: charge vs time + + Charge vs time for the accpetor and donor molecules. + + where it is clearly shown that during the dynamic the PDI molecule act as + an accpetor of electrons getting negative values, meanwhile the carbazole is + getting positive. This confirm the charge transfer upon ilumination. + If we follow the protocol from before, ploting the populations and searching + for the orbitals involved in the transition, we should be able to get some + insigths on the mechanism of the charge transfer (follow the steps in the + prevous sections). As it is shown in the figure: + + .. figure:: ../_figures/elecdynamics/tutorial/molpopul-CT.png + :width: 60% + :align: center + :alt: molpopul CT + + (left)Populations vs time for the pulse dynamics. (right) Orbitals involved + in the excitation during the dynamics. + + the orbitals involved in the excitation with the pulse are localized in the + PDI molecule, i.e. we can confirm that we are exciting the PDI molecule in + its own HOMO-LUMO transition (and not an HOMO-LUMO transition of the whole + system). Comparing with the previous figure of the charges dynamics, we can + also see that the CT process start just after a certain amount of electrons + are excited in the PDI molecule (more or less 30 fs, the duration of the pulse + used). So we could in principle divide the mechanism in two steps. The first + one, from 0 to ~30 fs where the PDI is beeing excited. The second step is the + charge transfer from the carbazole to the PDI once the last is already excited. + + + + + + + + From 231180bd936e3450b6d7a384026387e67981170e Mon Sep 17 00:00:00 2001 From: Charly Medrano Date: Thu, 30 Jun 2022 17:17:07 +0200 Subject: [PATCH 09/14] Fix figure pops --- .../elecdynamics/tutorial/molpopul-CT.png | Bin 19898 -> 183253 bytes docs/electronicdynamics/tutorial.rst | 2 ++ 2 files changed, 2 insertions(+) diff --git a/docs/_figures/elecdynamics/tutorial/molpopul-CT.png b/docs/_figures/elecdynamics/tutorial/molpopul-CT.png index 08ca2701361578d61498fad0cf82d4eb5188522a..4b29320407f48bf7a65e3738ae218599399fb46a 100644 GIT binary patch literal 183253 zcmeFZWmFv7wl<8@xVuAe4HDcfxVyUs8h3YhcL+|<1b2504#C~s;q86jbMANdzGHm9 z-k+yO)u`3AR@bVUYw9y+b%dh4BoaJ6JQx@llGIl*WiT+PS}-t(A^-&FOyG=B8t4G- zq%0`{Ry|301p4A`rYU7ECkI9cY6HNa!12ML{~7|?1;7dZyDb4u0|xnD=RwyAvjT(q z*BE)w@vo0IX#eXs|Mv))5B{&wpmX^U{~irhn-BT#Hbl{1KXZ@NCI=nhfM2zoKsUVj 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So we could in principle divide the mechanism in two steps. The first one, from 0 to ~30 fs where the PDI is beeing excited. The second step is the charge transfer from the carbazole to the PDI once the last is already excited. + + From eb03fe4279a9418a4d047e11e9d320d75c295706 Mon Sep 17 00:00:00 2001 From: Charly Medrano Date: Fri, 1 Jul 2022 14:59:16 +0200 Subject: [PATCH 10/14] Final fix and refs --- .../01_carbazole/01_spectrum/dftb_in.hsd_spec | 2 +- .../01_carbazole/02_laser/dftb_in.hsd_laser | 2 +- .../01_carbazole/02_laser/waveplot_in.hsd_ | 2 +- .../01_spectra_and_laser/02_PDI/coords.gen | 42 +++++++ .../01_aggregate_spec/dftb_in.hsd_spec | 2 +- .../02_aggregate_CT/dftb_in.hsd_pulse | 2 +- docs/electronicdynamics/index.rst | 1 + docs/electronicdynamics/tutorial.rst | 110 +++++++++++------- 8 files changed, 113 insertions(+), 50 deletions(-) create mode 100644 docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/02_PDI/coords.gen diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/01_spectrum/dftb_in.hsd_spec b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/01_spectrum/dftb_in.hsd_spec index 1e246bb0..cb31d61b 100644 --- a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/01_spectrum/dftb_in.hsd_spec +++ b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/01_spectrum/dftb_in.hsd_spec @@ -13,7 +13,7 @@ Hamiltonian = DFTB { N = "p" } SlaterKosterFiles = Type2FileNames { - Prefix = "../../mio-1-1/" + Prefix = "../../../../slakos/download/mio-1-1/" Separator = "-" Suffix = ".skf" } diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/dftb_in.hsd_laser b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/dftb_in.hsd_laser index d1ed1796..752094a3 100644 --- a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/dftb_in.hsd_laser +++ b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/dftb_in.hsd_laser @@ -13,7 +13,7 @@ Hamiltonian = DFTB { N = "p" } SlaterKosterFiles = Type2FileNames { - Prefix = "../../mio-1-1/" + Prefix = "../../../../slakos/download/mio-1-1/" Separator = "-" Suffix = ".skf" } diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/waveplot_in.hsd_ b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/waveplot_in.hsd_ index c66315a9..ce881875 100644 --- a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/waveplot_in.hsd_ +++ b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/waveplot_in.hsd_ @@ -25,5 +25,5 @@ Basis { # Including mio-1-1.hsd. (If you use a set, which depends on other sets, # the wfc.*.hsd files for each required set must be included in a similar # way.) - <<+ "./.hsd" ### Path for Wave function coeffiecients for waveplot + <<+ "../../../../slakos/wfc/wfc.mio-1-1.hsd" ### Path for Wave function coeffiecients for waveplot } diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/02_PDI/coords.gen b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/02_PDI/coords.gen new file mode 100644 index 00000000..6bb60f85 --- /dev/null +++ b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/02_PDI/coords.gen @@ -0,0 +1,42 @@ +40 C +C H N O + 1 1 -2.8702011600E+00 0.0000000000E+00 0.0000000000E+00 + 2 1 -1.4362663100E+00 0.0000000000E+00 1.3000000000E-07 + 3 1 -3.5889101500E+00 -1.2350464400E+00 -2.3000000000E-07 + 4 1 -2.8813199700E+00 -2.4379174600E+00 -2.1000000000E-07 + 5 1 -1.4787678500E+00 -2.4440123700E+00 1.1000000000E-07 + 6 1 -7.3366388000E-01 -1.2519893100E+00 3.1000000000E-07 + 7 1 -3.5889101500E+00 1.2350464400E+00 0.0000000000E+00 + 8 1 -2.8813199600E+00 2.4379174600E+00 5.0000000000E-08 + 9 1 -1.4787678400E+00 2.4440123900E+00 0.0000000000E+00 + 10 1 -7.3366389000E-01 1.2519893100E+00 2.0000000000E-08 + 11 1 7.3366387000E-01 -1.2519893000E+00 5.5000000000E-07 + 12 1 1.4362663200E+00 1.0000000000E-08 2.6000000000E-07 + 13 1 7.3366387000E-01 1.2519893100E+00 -7.0000000000E-08 + 14 1 1.4787678400E+00 -2.4440123700E+00 9.5000000000E-07 + 15 1 2.8813199500E+00 -2.4379174700E+00 9.2000000000E-07 + 16 1 3.5889101400E+00 -1.2350464400E+00 5.1000000000E-07 + 17 1 2.8702011700E+00 2.0000000000E-08 2.3000000000E-07 + 18 1 3.5889101600E+00 1.2350464500E+00 -1.2000000000E-07 + 19 1 2.8813199600E+00 2.4379174700E+00 -5.4000000000E-07 + 20 1 1.4787678400E+00 2.4440123700E+00 -5.2000000000E-07 + 21 2 -3.4335673000E+00 -3.3896396100E+00 -4.6000000000E-07 + 22 2 -9.7502556000E-01 -3.4212878700E+00 1.4000000000E-07 + 23 2 -3.4335673300E+00 3.3896396100E+00 9.0000000000E-08 + 24 2 -9.7502557000E-01 3.4212879000E+00 -4.0000000000E-08 + 25 2 9.7502555000E-01 -3.4212878600E+00 1.2900000000E-06 + 26 2 3.4335673000E+00 -3.3896396100E+00 1.2100000000E-06 + 27 2 9.7502554000E-01 3.4212878700E+00 -8.9000000000E-07 + 28 2 3.4335672900E+00 3.3896396300E+00 -8.6000000000E-07 + 29 1 -5.0766344400E+00 -1.2425131600E+00 -6.6000000000E-07 + 30 1 -5.0766344500E+00 1.2425131500E+00 -4.0000000000E-08 + 31 1 5.0766344400E+00 -1.2425131700E+00 2.2000000000E-07 + 32 1 5.0766344600E+00 1.2425131600E+00 -6.0000000000E-08 + 33 3 -5.7159981400E+00 0.0000000000E+00 -4.1000000000E-07 + 34 3 5.7159981500E+00 -1.0000000000E-08 6.0000000000E-08 + 35 4 -5.7484785000E+00 -2.2718608200E+00 -1.2300000000E-06 + 36 4 -5.7484785300E+00 2.2718608200E+00 2.2000000000E-07 + 37 4 5.7484785100E+00 -2.2718608300E+00 1.1000000000E-07 + 38 4 5.7484785500E+00 2.2718607900E+00 -1.6000000000E-07 + 39 2 -6.7494873900E+00 0.0000000000E+00 -5.7000000000E-07 + 40 2 6.7494873800E+00 -4.0000000000E-08 -2.0000000000E-08 diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/dftb_in.hsd_spec b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/dftb_in.hsd_spec index ae4c9cdc..6886a940 100644 --- a/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/dftb_in.hsd_spec +++ b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/dftb_in.hsd_spec @@ -14,7 +14,7 @@ Hamiltonian = DFTB { O = "p" } SlaterKosterFiles = Type2FileNames { - Prefix = "../../mio-1-1/" + Prefix = "../../../slakos/download/mio-1-1/" Separator = "-" Suffix = ".skf" } diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/dftb_in.hsd_pulse b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/dftb_in.hsd_pulse index 94a27706..d8af1e29 100644 --- a/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/dftb_in.hsd_pulse +++ b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/dftb_in.hsd_pulse @@ -14,7 +14,7 @@ Hamiltonian = DFTB { O = "p" } SlaterKosterFiles = Type2FileNames { - Prefix = "../../../mio-1-1/" + Prefix = "../../../slakos/download/mio-1-1/" Separator = "-" Suffix = ".skf" } diff --git a/docs/electronicdynamics/index.rst b/docs/electronicdynamics/index.rst index 1b1e9d87..03ef7aac 100644 --- a/docs/electronicdynamics/index.rst +++ b/docs/electronicdynamics/index.rst @@ -24,3 +24,4 @@ and driving of nuclear motion via electronic excitation. spectra.rst driving.rst ehrenfest.rst + tutorial.rst diff --git a/docs/electronicdynamics/tutorial.rst b/docs/electronicdynamics/tutorial.rst index 8388d85c..40e28c2c 100644 --- a/docs/electronicdynamics/tutorial.rst +++ b/docs/electronicdynamics/tutorial.rst @@ -37,6 +37,8 @@ We will calculate the absorption spectrum of the carbazole molecule :align: center :alt: Carbazole molecule. + Carbazole molecule + 2. Open the *dftb_in.hsd_spec* file. This is a template for the calculation of the absorption spectrum. @@ -55,15 +57,15 @@ We will calculate the absorption spectrum of the carbazole molecule * ``Steps`` (integer): the number of steps of the dynamics. It defines the time window and, consequently, the energy window of the spectrum. The longer the dynamic, the lower the - energies that can be reached in the spectrum are (also afected by the timestep, of course). + energies that can be reached in the spectrum (also afected by the ``TimeStep``, of course). Here, we will use 10000 steps. * ``TimeStep`` (float): the time step in time units. Usually 0.2 a.u (0.0048 fs). It defines the resolution of the spectrum. The smaller the time step, the higher the resolution within the time window. * ``Perturbation``: In this case we need a kick perturbation (Dirac delta) and we need to specify the ``PolarizationDirection`` that could be *X*, *Y*, *Z* (if we are interested in - one particular direction) or *all* if we want to calculate the whole absorption spectrum. - Set it as *all*. + one particular direction) or ``all`` if we want to calculate the whole absorption spectrum. + Set it as ``all``. * ``FieldStrength`` (float): the field strength of the perturbation applied. For the calculation of the absorption spectrum, it must be within the linear response regime, i.e. usually 0.001 :math:`V/\AA`. @@ -71,7 +73,7 @@ We will calculate the absorption spectrum of the carbazole molecule - Complete the template file, copy it to *dftb_in.hsd* and run the calculation. 3. Once the dynamics ended, we will have 3 components of the dynamical dipole moment - (*mux.dat*, *muy.dat*, *muz.dat*). We need to Fourier-transform these dipole components + (*mux.dat*, muy.dat, *muz.dat*). We need to average and Fourier-transform these dipole components in order to obtain the absorption spectrum of the molecule. To do this, we will use the ``calc_timeprop_spectrum`` tool available after installation of DFTB+ under: *dftbplus/tools/misc/*. In the folder @@ -80,7 +82,7 @@ We will calculate the absorption spectrum of the carbazole molecule calc_timeprop_spectrum -d 4 -f 0.001 where the option -d is for the damping constant (in fs) applied to the dipole moment before transformation. - The option -f stands for the field strength (in V/AA) of the perturbation applied during dynamic. + The option -f stands for the field strength (in :math:`V/\AA`) of the perturbation applied during dynamic. 4. After running the script you will find two new files: *spec-nm.dat* and *spec-ev.dat* which are the absorption spectra in nm and eV, respectively. Plot the spectrum file with the plotting tool @@ -141,13 +143,13 @@ and calculate the direction of maximal polarization of the transition. the transition energy of interest. This value must be in energy units like eV but also nm is possible. * ``PolarizationDirection`` (vector): in the case of a laser, the - ``PolarizationDirection`` is 3-cartesian components vector in which the + ``PolarizationDirection`` is a 3-cartesian components vector in which the laser will be applied. Note that we turned on the ``Populations`` flag in order to write the occupations during the dynamics. Also note that we are asking for the detailed xml and the eigenvectors with the ``WriteDetailedXML`` - and ``WriteEigenvectors`` flags. We will need them to plot the orbitals + and ``WriteEigenvectors`` options. We will need them to plot the orbitals with waveplot in the following sections. 2. To complete the input template for the laser, we need to provide @@ -233,7 +235,7 @@ and calculate the direction of maximal polarization of the transition. - In which orbitals are we interested? - After editing and completing this file, just rename it to *waveplot_in.hsd* and run - ``waveplot`` using your current installed version that probably is at:: + ``waveplot`` using your current installed version that would be at:: $HOME/dftbplus/_build/app/waveplot/waveplot @@ -252,7 +254,7 @@ and the orbitals involved in the transition. You should get something similar in your calculations: .. figure:: ../_figures/elecdynamics/tutorial/molpopul-carbazole.png - :width: 60% + :width: 100% :align: center :alt: molpopul1-carbazole @@ -263,7 +265,7 @@ similar in your calculations: Now is your turn! Calculation of PDI absorption spectrum -------------------------------------------------------- -[Input: `recipes/electronicdynamics/tutorial/01_spectra_and_laser/02_PDI/] +[Input: `recipes/electronicdynamics/tutorial/01_spectra_and_laser/02_PDI/``] We will repeat the workflow used for the carbazole molecule with a new molecule, PDI. @@ -279,7 +281,7 @@ Here we leave some figures from our calculations that could be useful to compare with your own calculations of this section: .. figure:: ../_figures/elecdynamics/tutorial/PDI.png - :width: 60% + :width: 100% :align: center :alt: PDI @@ -291,30 +293,29 @@ compare with your own calculations of this section: Photoinduced charge transfer ============================ -Calculate the absorption spectrum of the Donor-acceptor aggregate +Calculate the absorption spectrum of a Donor-acceptor aggregate ----------------------------------------------------------------- [Input: `recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/`] 1. Take a look at the input coordinates *coords.xyz* (you can open it using avogadro, -jmol, vmd, VESTA, etc). - -.. figure:: ../_figures/elecdynamics/tutorial/PDI+carbazole.png - :width: 60% - :align: center - :alt: PDI+carbazole aggregate + jmol, vmd, VESTA, etc). - PDI+carbazole derivatives aggregate + .. figure:: ../_figures/elecdynamics/tutorial/PDI+carbazole.png + :width: 60% + :align: center + :alt: PDI+carbazole aggregate -It is an aggregate of the previous molecules analysed in which the carbazole and -PDI derivative act as donor and acceptor of electrons, respectively. + PDI+carbazole derivatives aggregate - - Convert the coordinates into *gen* format (use the ``xyz2gen`` script) and - calculate the absorption spectrum using the *dftb_in.hsd_spec* as a template - for the input (copy this file or rename it as *dftb_in.hsd*). - Note that after the electron dynamics, you will need (as before) to run the - Fourier transform of the induced dipole moment of the system (using the - ``calc_timeprop_spectrum`` tool) in order to obtain the spectrum. + It is an aggregate of the previous molecules analysed in which the carbazole and + PDI derivatives act as donor and acceptor of electrons, respectively. + - Convert the coordinates into *gen* format (use the ``xyz2gen`` script) and + calculate the absorption spectrum using the *dftb_in.hsd_spec* as a template + for the input (copy this file or rename it as *dftb_in.hsd*). + Note that after the electron dynamics, you will need (as before) to run the + Fourier transform of the induced dipole moment of the system (using the + ``calc_timeprop_spectrum`` tool) in order to obtain the spectrum. 2. Compare the calculated spectrum with the individual ones (you can use the spectra calculated before or recalculate them from these derivatives). Is there @@ -325,12 +326,14 @@ PDI derivative act as donor and acceptor of electrons, respectively. :align: center :alt: A+D spectrum - Absorption spectrum of the PDI+carbazole derivatives aggregate. + Absorption spectrum of the PDI+carbazole derivatives aggregate (in black), + compared to the individual spectrum for the PDI moiety (in orange) and + the carbazole moiety (in red). 3. We are interested in the dynamics upon ilumination of the acceptor molecule. For such puropose, we will perform a laser dynamic in next step and for it, we need to calculate the transition dipole direction of the absorption band at ~530 nm. Calculate this vector - using the `calc_timeprop_maxpoldir` tool. You shold obtain something similar to:: + using the ``calc_timeprop_maxpoldir`` tool. You shold obtain something similar to:: PolarizationDirection = -0.99977920 0.01776644 0.01122075 @@ -352,32 +355,32 @@ Laser dynamics on the donor-acceptor aggregate for charge transfer Steps = 20000 TimeStep [au] = 0.2 Perturbation = Laser{ - PolarizationDirection = #calculate with calc_timeprop_maxpoldir - #for the energy of interest + PolarizationDirection = #calculate with calc_timeprop_maxpoldir + #for the energy of interest LaserEnergy [nm] = } - EnvelopeShape = Sin2{ #envelope shape type - Time1 [fs] = 30.0 #pulse duration (assuming Time0 = 0, by default) + EnvelopeShape = Sin2{ #envelope shape type + Time1 [fs] = 30.0 #pulse duration (assuming Time0 = 0, by default) } - FieldStrength [v/a] = 0.02 #field strength bigger than spectrum case (0.001) + FieldStrength [v/a] = 0.02 #field strength bigger than spectrum case (0.001) WriteEnergyAndCharges = Yes Populations = Yes } Now in the ElectronDynamics we added the Sin2 ``EnvelopeShape`` with a duration of 30 fs starting at the beginning of the dynamics. We will - ask the code also to print the populations during dynamics to study the + also ask the code to print the populations during dynamics to study the mechanism of charge transfer. Complete the input template filling the ``PolarizationDirection`` and ``LaserEnergy`` obtained before and run the code (don't forget to rename the template to *dftb_in.hsd*). -2. After running the electron dynamics, let inspect what give us de *qsvst.dat* +2. After running the electron dynamics, let inspect what give us the *qsvst.dat* file:: - # time (fs) | total net charge (e) | charge (atom_1) (e) | ... | charge (atom_N) (e)| - 0.000000000000000 -0.000000000000055 0.075753114169209 0.077680106829215 ... - 0.241888432650500 -0.000000000000048 0.075753940652948 0.077680933651269 ... - 0.483776865301000 -0.000000000000049 0.075758821681684 0.077685768802125 ... + #time (fs) | total net charge (e) | charge (atom_1) (e) | ... | charge (atom_N) (e)| + 0.000000000000000 -0.000000000000055 0.075753114169209 0.077680106829215 ... + 0.241888432650500 -0.000000000000048 0.075753940652948 0.077680933651269 ... + 0.483776865301000 -0.000000000000049 0.075758821681684 0.077685768802125 ... The first column of the file is the time and the second one is the total net charge of the system at each time step (which should keep near to zero). After that, we @@ -422,7 +425,7 @@ Laser dynamics on the donor-acceptor aggregate for charge transfer After runing the script, two files may be generated: *charge_frag1.dat* and *charge_frag2.dat* with the corresponding charges of each defined fragment. - If you plot it you will something like: + If you plot it you will get something like: .. figure:: ../_figures/elecdynamics/tutorial/charge-vs-time.png :width: 60% @@ -437,10 +440,10 @@ Laser dynamics on the donor-acceptor aggregate for charge transfer If we follow the protocol from before, ploting the populations and searching for the orbitals involved in the transition, we should be able to get some insigths on the mechanism of the charge transfer (follow the steps in the - prevous sections). As it is shown in the figure: + previous sections). As it is shown in the figure: .. figure:: ../_figures/elecdynamics/tutorial/molpopul-CT.png - :width: 60% + :width: 100% :align: center :alt: molpopul CT @@ -457,12 +460,29 @@ Laser dynamics on the donor-acceptor aggregate for charge transfer one, from 0 to ~30 fs where the PDI is beeing excited. The second step is the charge transfer from the carbazole to the PDI once the last is already excited. +We hope that this tutorial would be helpful for those interested in get into the real-time TDDFTB +method using ``DFTB+``. Of course, this is just the beginning and there are much more possibilities +to do in terms of studyng optical properties and photoinduced processes within this approach in many +different scenarios and materials like *graphene nanoribbons*, *plasmonic nanoparticles*, *glod nanoclusters*, +*semiconductor nanoparticles* and *organic solar cells*. As an inspiration, we give you some references of +the last works performed with this method in ``DFTB+``: - +**Fano Resonance and Incoherent Interlayer Excitons in Molecular van der Waals Heterostructures.** Lien-Medrano, C. R., Bonafé, F. P., Yam, C. Y., Palma, C.-A., Sánchez, C. G., & Frauenheim, T. (2022). Nano Letters, 22(3), 911–917. `https://doi.org/10.1021/acs.nanolett.1c03441 `_ - +**Dynamical evolution of the Schottky barrier as a determinant contribution to electron-hole pair stabilization and photocatalysis of plasmon-induced hot carriers.** Berdakin, M., Soldano, G., Bonafé, F. P., Liubov, V., Aradi, B., Frauenheim, T., & Sánchez, C. G. (2022). Nanoscale, 14(7), 2816–2825. `https://doi.org/10.1039/d1nr04699c `_ + +**Photoinduced charge-transfer in chromophore-labeled gold nanoclusters: quantum evidence of the critical role of ligands and vibronic couplings.** Domínguez-Castro, A., Lien-Medrano, C. R., Maghrebi, K., Messaoudi, S., Frauenheim, T., & Fihey, A. (2021). Nanoscale, 13(14), 6786–6797. `https://doi.org/10.1039/D1NR00213A `_ + +**Interplay between Intra- And Interband Transitions Associated with the Plasmon-Induced Hot Carrier Generation Process in Silver and Gold Nanoclusters.** Berdakin, M., Douglas-Gallardo, O. A., & Sánchez, C. G. (2020). Journal of Physical Chemistry C, 1631–1639. `https://doi.org/10.1021/acs.jpcc.9b10871 `_ + +**Plasmon-induced hot-carrier generation differences in gold and silver nanoclusters.** Douglas-Gallardo, O. A., Berdakin, M., Frauenheim, T., & Sánchez, C. G. (2019). Nanoscale, 11(17), 8604–8615. `https://doi.org/10.1039/c9nr01352k `_ +**Trap-Door-Like Irreversible Photoinduced Charge Transfer in a Donor-Acceptor Complex.** Medrano, C. R., & Sánchez, C. G. (2018). Journal of Physical Chemistry Letters, 9(12), 3517–3524. `https://doi.org/10.1021/acs.jpclett.8b01043 `_ +**Quantum efficiency of the photo-induced electronic transfer in dye–TiO 2 complexes.** Marquez, D. M., & Sánchez, C. G. (2018). Physical Chemistry Chemical Physics, 20(41), 26280–26287. `https://doi.org/10.1039/C8CP04625E `_ +**Characterization of ZnO as substrate for DSSC.** Mansilla Wettstein, C., & Sánchez, C. G. (2018). Physical Chemistry Chemical Physics, 20(34), 21910–21916. `https://doi.org/10.1039/C8CP01709C `_ +**Plasmon-driven sub-picosecond breathing of metal nanoparticles.** Bonafé, F. P., Aradi, B., Guan, M., Douglas-Gallardo, O. A., Lian, C., Meng, S., Frauenheim, T., & Sánchez, C. G. (2017). Nanoscale, 9(34), 12391–12397. `https://doi.org/10.1039/C7NR04536K `_ +**Photoinduced charge-transfer dynamics simulations in noncovalently bonded molecular aggregates.** Medrano, C. R., Oviedo, M. B., & Sánchez, C. G. (2016). Physical Chemistry Chemical Physics, 18(22), 14840–14849. `https://doi.org/10.1039/c6cp00231e `_ From 019a9fd011fb6284db24b00f06b839408fc6a357 Mon Sep 17 00:00:00 2001 From: Franco Bonafe Date: Fri, 1 Jul 2022 17:49:30 +0200 Subject: [PATCH 11/14] Proof read and modify tutorial text --- docs/electronicdynamics/tutorial.rst | 225 +++++++++++---------------- 1 file changed, 92 insertions(+), 133 deletions(-) diff --git a/docs/electronicdynamics/tutorial.rst b/docs/electronicdynamics/tutorial.rst index 40e28c2c..3a981bf1 100644 --- a/docs/electronicdynamics/tutorial.rst +++ b/docs/electronicdynamics/tutorial.rst @@ -1,13 +1,12 @@ .. highlight:: none *********************************************************************** -Tutorial first steps: Absorption spectra, analysis and charge transfer +Tutorial: Absorption spectra, analysis and charge transfer *********************************************************************** -This is the tutorial presented in the DFTB+ school 2022 in Daresbury. The idea is to get used -to with the real-time TDDFTB method learning the basics of absorption spectra calculations and -photoinduced processes like charge transfer under irradiation. +This is the tutorial given at the DFTB+ School 2022 in Daresbury, UK. The idea is to get familiar +with the real-time TDDFTB method applied to molecules and molecular complexes, learning the basics of absorption spectra calculations and photoinduced processes such as charge transfer under laser irradiation. Spectra and analysis ==================== @@ -20,12 +19,12 @@ Calculation of the absorption spectrum of carbazole [Input: `recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/01_spectrum`] -We will calculate the absorption spectrum of the carbazole molecule +We will calculate the absorption spectrum of the carbazole molecule, following the procedure described in :ref:`sec-spectra`. 1. Take a look at the input coordinates *coords.gen*. The *.gen* format is the one used for DFTB+ code. In order to visualize the molecule, you can use the ``gen2xyz`` script, provided in the installation of the - DFTB+ code, doing:: + DFTB+ code, by running:: gen2xyz coords.gen @@ -45,35 +44,30 @@ We will calculate the absorption spectrum of the carbazole molecule - Take a look at the ``ElectronDynamics`` block at the end of the file:: ElectronDynamics = { - Steps = #define the time window - TimeStep [au] = #resolution of the spectrum - Perturbation = Kick { #must be a kick (Dirac delta) - PolarizationDirection = #desired direction/s + Steps = # defines the total simulation time + TimeStep [au] = # resolution of the spectrum + Perturbation = Kick { # external field is a kick (Dirac delta) + PolarizationDirection = # desired direction/s } - FieldStrength [v/a] = #Field strength of the perturbation + FieldStrength [v/a] = # field strength of the kick } - The input variables to be considered for the calculation of the spectrum are four: - * ``Steps`` (integer): the number of steps of the dynamics. It defines the time window and, - consequently, the energy window of the spectrum. The longer the dynamic, the lower the - energies that can be reached in the spectrum (also afected by the ``TimeStep``, of course). - Here, we will use 10000 steps. - * ``TimeStep`` (float): the time step in time units. Usually 0.2 a.u (0.0048 fs). - It defines the resolution of the spectrum. The smaller the time step, - the higher the resolution within the time window. - * ``Perturbation``: In this case we need a kick perturbation (Dirac delta) and we need to + * ``Steps`` (integer): the number of steps of the dynamics. The longer the dynamics, the lower the + energies that can be resolved in the spectrum (the total time is also afected by the ``TimeStep``, of course). Here, we will use 10000 steps. + * ``TimeStep`` (float): the time step in time units. Here we use 0.2 a.u (0.0048 fs), which is normally stable for simulations of a few tens of thousands of steps. In case there is instability in the dynamics, the time step shuld be decreased. + * ``Perturbation``: In this case we need a Dirac-delta perturbation (AKA kick) and we need to specify the ``PolarizationDirection`` that could be *X*, *Y*, *Z* (if we are interested in - one particular direction) or ``all`` if we want to calculate the whole absorption spectrum. - Set it as ``all``. + one particular direction) or ``all`` if we want to calculate the three kicks consequtively and then calculate the spherically-averaged spectrum, accounting for random molecular orientations. + Hence, we set it as ``all``. * ``FieldStrength`` (float): the field strength of the perturbation applied. For the calculation of the absorption spectrum, it must be within the linear response regime, - i.e. usually 0.001 :math:`V/\AA`. + i.e. usually 0.001 :math:`V/\AA` or lower. - Complete the template file, copy it to *dftb_in.hsd* and run the calculation. -3. Once the dynamics ended, we will have 3 components of the dynamical dipole moment - (*mux.dat*, muy.dat, *muz.dat*). We need to average and Fourier-transform these dipole components +3. Once the dynamics ends, we will have calculated the time-resolved dipole moment using 3 field polarization directions (*mux.dat*, muy.dat, *muz.dat*). We need to average and Fourier-transform (or the other way around, as these are linear operations) these dipole components in order to obtain the absorption spectrum of the molecule. To do this, we will use the ``calc_timeprop_spectrum`` tool available after installation of DFTB+ under: *dftbplus/tools/misc/*. In the folder @@ -81,12 +75,12 @@ We will calculate the absorption spectrum of the carbazole molecule calc_timeprop_spectrum -d 4 -f 0.001 - where the option -d is for the damping constant (in fs) applied to the dipole moment before transformation. - The option -f stands for the field strength (in :math:`V/\AA`) of the perturbation applied during dynamic. + where the option -d is for the damping constant (artificial lifetime, in fs), which is equivalent to convoluting each resonance with a Lorentzian in time domain. + The option -f is the field strength of the kick (in :math:`V/\AA`). applied during dynamics. 4. After running the script you will find two new files: *spec-nm.dat* and *spec-ev.dat* which are the absorption spectra in nm and eV, respectively. Plot the spectrum file with the plotting tool - of your desire and look at the lower energy transitions. You should then see + of your choice and look at the lowest energy transitions. You should then see an absorption spectrum similar to: .. figure:: ../_figures/elecdynamics/tutorial/spec-nm-carbazole.png @@ -97,8 +91,8 @@ We will calculate the absorption spectrum of the carbazole molecule Absorption spectrum of carbazole molecule 5. Change the damping constant for a higher value, recalculate the specctrum and plot both spectra - together. Which is the effect of the damping time in the spectrum? - Here it is an example of the same spectrum obtained before, calculated with + together. What is the effect of the damping time in the spectrum? + Here it is an example of the same spectrum calculated with different values of the damping constant. .. figure:: ../_figures/elecdynamics/tutorial/specs-comparison-damp.png @@ -108,17 +102,16 @@ We will calculate the absorption spectrum of the carbazole molecule Influence of the damping constant value ``d`` in the absorption spectrum. -Analysis of the absorption spectrum of carbazole ------------------------------------------------- +Analysis of the absorption spectrum of carbazole: driving the system with a laser +--------------------------------------------------------------------------------- [Input: `recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser`] We will consider a laser perturbation in tune with the lowest energy transition of the molecule in order to study the photodynamic process of absorption in this transition. In order to do this, we -need to know the energy of the lowest energy transition of -the molecule (look for it in the spectrum plotted in the previous calculation) -and calculate the direction of maximal polarization of the transition. +will follow the same procedure as described in :ref:`sec-driving`, +finding first the lowest energy transition of the molecule in the spectrum plotted in the previous calculation, and then calculating the direction of maximal polarization of the transition. 1. Open the *dftb_in.hsd_laser* file. This is a template for the calculation of a laser perturbation. @@ -128,23 +121,21 @@ and calculate the direction of maximal polarization of the transition. ElectronDynamics = { Steps = 10000 TimeStep [au] = 0.2 - Perturbation = Laser{ # Laser type perturbation - LaserEnergy [nm] = # energy of interest - PolarizationDirection = # calculate with calc_timeprop_maxpoldir + Perturbation = Laser{ # laser type perturbation + LaserEnergy [nm] = # energy or wavelength of interest + PolarizationDirection = # to be calculated with calc_timeprop_maxpoldir } FieldStrength [v/a] = 0.001 - Populations = Yes # to write populations during dynamic + Populations = Yes # to write GS-MP projected populations during the dynamics } - Now, the ``Perturbation`` type is a ``laser`` (and not anymore a ``kick``) - and we need to specify two parameters: + Now, the ``Perturbation`` type is a continuous-wave ``laser``, for which we need to specify two parameters: * ``LaserEnergy`` (float): the energy of the applied laser that may be the transition energy of interest. This value must be in energy units - like eV but also nm is possible. + like eV but also a wavelength in nm is allowed. * ``PolarizationDirection`` (vector): in the case of a laser, the - ``PolarizationDirection`` is a 3-cartesian components vector in which the - laser will be applied. + ``PolarizationDirection`` is a 3-components vector. Note that we turned on the ``Populations`` flag in order to write the occupations during the dynamics. Also note that we are asking for @@ -163,7 +154,7 @@ and calculate the direction of maximal polarization of the transition. calc_timeprop_maxpoldir -h - - Along which axes is the direction vector? How is this explained? + - Along which axis/axes is the polarization of the molecule oriented? Why? - Hint: try to visualize the molecule and see how it is oriented with respect to the cartesian axes. @@ -174,46 +165,45 @@ and calculate the direction of maximal polarization of the transition. and you will obtain the following transition dipole vector:: - PolarizationDirection = 0.99999221 0.00101174 -0.00381496 + PolarizationDirection = 0.99999 0.00101 -0.003815 which is essentially paralel to the *X* cartesian direction (because of the molecules orientation with respect to the cartesian axes) 3. Prepare the input for the dynamics under a continuous laser perturbation. - Use the energy transition obtained from the spectrum as the ``LaserEnergy`` + Use the energy obtained from the spectrum as the ``LaserEnergy`` and the vector obtained above as the ``PolarizationDirection`` of the laser. - - Why we should use this direction instead of any other? + - Why we should use this laser polarization instead of any other? 4. After the dynamics, take a look at the *mu.dat* file. - Is the dipole moment increasing linearly? - .. figure:: ../_figures/elecdynamics/tutorial/mu-carbazole-components.png + .. figure:: ../_figures/ele.. _sec-driving:cdynamics/tutorial/mu-carbazole-components.png :width: 60% :align: center :alt: mu components Dipole moment components vs time for the laser dynamics. -5. Take a look at the *molpopul.dat* +5. Take a look at the *molpopul1.dat* file generated. This file contains the populations projected on the GS orbitals during the dynamics. - Which orbitals are involved in the transition? - Help: you can plot the *molpopul.dat* file using xmgrace:: + Help: you can plot the *molpopul1.dat* file using `xmgrace`:: xmgrace -nxy molpopul.dat - Look at the populations at y=2 (occupied orbitals in the GS basis) and find - which curves are decreasing during the dynamic. These are the orbitals + Look at the populations initially at y=2 (occupied orbitals in the GS basis) and find + which curves are decreasing over time, these are the orbitals being depopulated. - Look at the populations at y=0 (unoccopied orbitals in the GS basis) and find - which curves are increasing during the dynamics. These are the orbitals - being populated. + Look at the populations initially at y=0 (unoccopied orbitals in the GS basis) and find + the orbitals being populated over time. You could also check in the *band.out* file generated from the SCC - calculation the states numbers. In the near of the Fermi energy, you + calculation the states numbers. Close to the Fermi energy, you should see something like:: 29 -6.641 2.00000 @@ -226,7 +216,7 @@ and calculate the direction of maximal polarization of the transition. where it is clear that states 31 and 32 are the HOMO and LUMO of the molecule, respectively. -6. Let's generate those orbitals using ``waveplot`` +6. Let's visualize those orbitals using ``waveplot``. For a complete description please check :ref:`basics-waveplot`. - Look at the *waveplot_in.hsd_* template input file for waveplot: @@ -234,10 +224,8 @@ and calculate the direction of maximal polarization of the transition. - Which files are needed? - In which orbitals are we interested? - - After editing and completing this file, just rename it to *waveplot_in.hsd* and run - ``waveplot`` using your current installed version that would be at:: - - $HOME/dftbplus/_build/app/waveplot/waveplot + - After editing this file, just rename it to *waveplot_in.hsd* and run + ``waveplot`` using your current installed executable, which should be in the same installation directory as the `dftbplus` executable. - After running waveplot, a number of files would be generated starting with "wp-1-1". @@ -245,13 +233,12 @@ and calculate the direction of maximal polarization of the transition. - Open the cube files that correspond to the HOMO and LUMO and plot them as an isosurface. For that there are several software options. Particularly, we give here some links for VMD and VESTA: - For a tutorial on the `Basics of VMD `_ and/or plotting an `isosurface `_ method please refer to the links. - VESTA allows the user to open directly cube files showing the isosurface instantaneusly - with some default parameters. Really good for rapid examinations. `Download VESTA `_ + For a tutorial on the `Basics of VMD `_ and/or plotting an `isosurface `_ method please refer to these links. + `VESTA `_ allows the user to open directly cube files showing the isosurface immediately + with some default parameters, making it a really good option for quick inspections. -Here we show a figure with the Populations obtained from the laser dynamics -and the orbitals involved in the transition. You should get something -similar in your calculations: +As a reference, here are the populations obtained from the laser dynamics +and the orbitals involved in the transition: .. figure:: ../_figures/elecdynamics/tutorial/molpopul-carbazole.png :width: 100% @@ -262,23 +249,22 @@ similar in your calculations: in the lower energy transition of the carbazole molecule. -Now is your turn! Calculation of PDI absorption spectrum +Now it's your turn! Calculation of PDI absorption spectrum -------------------------------------------------------- [Input: `recipes/electronicdynamics/tutorial/01_spectra_and_laser/02_PDI/``] -We will repeat the workflow used for the carbazole molecule with a new +We will repeat the procedure used for the carbazole molecule with a new molecule, PDI. 1. Based on the calculations that you ran before. - Calculate the absorption spectrum with a proper *dftb_in.hsd* input file. - Find the lowest energy transition. - - Study the excitation process using a laser tuned with the transition. + - Apply a laser tuned with this transition. - Obtain the orbitals involved in the transition using waveplot and plot them. -Here we leave some figures from our calculations that could be useful to -compare with your own calculations of this section: +Reference results: .. figure:: ../_figures/elecdynamics/tutorial/PDI.png :width: 100% @@ -293,13 +279,12 @@ compare with your own calculations of this section: Photoinduced charge transfer ============================ -Calculate the absorption spectrum of a Donor-acceptor aggregate +Calculate the absorption spectrum of a donor-acceptor aggregate ----------------------------------------------------------------- [Input: `recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/`] -1. Take a look at the input coordinates *coords.xyz* (you can open it using avogadro, - jmol, vmd, VESTA, etc). +1. Visualize the coordinates file *coords.xyz* .. figure:: ../_figures/elecdynamics/tutorial/PDI+carbazole.png :width: 60% @@ -307,19 +292,15 @@ Calculate the absorption spectrum of a Donor-acceptor aggregate :alt: PDI+carbazole aggregate PDI+carbazole derivatives aggregate - - It is an aggregate of the previous molecules analysed in which the carbazole and +` + It is an aggregate of the two previous molecules, in which the carbazole and PDI derivatives act as donor and acceptor of electrons, respectively. - - Convert the coordinates into *gen* format (use the ``xyz2gen`` script) and + - Convert the coordinates into *gen* format (using the ``xyz2gen`` script) and calculate the absorption spectrum using the *dftb_in.hsd_spec* as a template for the input (copy this file or rename it as *dftb_in.hsd*). - Note that after the electron dynamics, you will need (as before) to run the - Fourier transform of the induced dipole moment of the system (using the - ``calc_timeprop_spectrum`` tool) in order to obtain the spectrum. 2. Compare the calculated spectrum with the individual ones (you can use the spectra - calculated before or recalculate them from these derivatives). Is there - relevant differences? + calculated before or recalculate them from these derivatives). For the comparison to be valid, you should use the same damping constant for all spectra. Are there relevant differences? .. figure:: ../_figures/elecdynamics/tutorial/specs-compar-A+D.png :width: 60% @@ -331,39 +312,37 @@ Calculate the absorption spectrum of a Donor-acceptor aggregate the carbazole moiety (in red). 3. We are interested in the dynamics upon ilumination of the acceptor molecule. For such - puropose, we will perform a laser dynamic in next step and for it, we need to calculate + puropose, we will perform a driven simulation in next step and for it, we need to calculate the transition dipole direction of the absorption band at ~530 nm. Calculate this vector using the ``calc_timeprop_maxpoldir`` tool. You shold obtain something similar to:: - PolarizationDirection = -0.99977920 0.01776644 0.01122075 + PolarizationDirection = -0.99977 0.01777 0.01122 which is essentially the *X* direction (since the PDI molecule axis is paralel to the *X* axis in the coordinates). -Laser dynamics on the donor-acceptor aggregate for charge transfer +Laser dynamics on the donor-acceptor aggregate and charge transfer ------------------------------------------------------------------ [Input: `recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/`] 1. With the transition dipole moment vector calculated previously, prepare - your input for a laser-driven electron dynamics in tune with the acceptor (PDI) + your input file for a laser-driven electron dynamics in tune with the acceptor (PDI) lowest energy excitation. Use the *dftb_in.hsd_pulse* as a template. Note that this time we add an envelope function to the laser perturbation in order - to mimick a laser pulse:: + to mimic a laser pulse:: ElectronDynamics = { Steps = 20000 TimeStep [au] = 0.2 Perturbation = Laser{ - PolarizationDirection = #calculate with calc_timeprop_maxpoldir - #for the energy of interest - LaserEnergy [nm] = + PolarizationDirection = # to be completed + LaserEnergy [nm] = # to be completed } - EnvelopeShape = Sin2{ #envelope shape type - Time1 [fs] = 30.0 #pulse duration (assuming Time0 = 0, by default) + EnvelopeShape = Sin2{ # envelope shape type + Time1 [fs] = 30.0 # pulse duration (by default the initial time is Time0 = 0) } - FieldStrength [v/a] = 0.02 #field strength bigger than spectrum case (0.001) - WriteEnergyAndCharges = Yes + FieldStrength [v/a] = 0.02 # larger field strength than the kick (0.001) to observe driven dynamics clearly Populations = Yes } @@ -374,7 +353,7 @@ Laser dynamics on the donor-acceptor aggregate for charge transfer ``PolarizationDirection`` and ``LaserEnergy`` obtained before and run the code (don't forget to rename the template to *dftb_in.hsd*). -2. After running the electron dynamics, let inspect what give us the *qsvst.dat* +2. After running the electron dynamics, let inspect the *qsvst.dat* file:: #time (fs) | total net charge (e) | charge (atom_1) (e) | ... | charge (atom_N) (e)| @@ -383,20 +362,15 @@ Laser dynamics on the donor-acceptor aggregate for charge transfer 0.483776865301000 -0.000000000000049 0.075758821681684 0.077685768802125 ... The first column of the file is the time and the second one is the total net charge - of the system at each time step (which should keep near to zero). After that, we - have one column for every atom charge at each time step (summing a total of N columns - being N the number of atoms in the system). + of the system at each time step (which should be always close to zero, within numerical error). After that, each column is the net atomic charge at each time step. Making use of the file *qsvst.dat* one may potencially get information - about partial charges moving during dynamics. If you are interested in what is - happening with the charge of one molecule in your system, then you could sum the - atom charges corresponding to that molecule (or part) of the system at each time - and get some insights. - -3. As we are interested in the charge transfer between both molecules after the pulse - we want to process the information contained in the *qsvst.dat* to obtain the total - charge of each molecule during the dynamics. For that, you could develope your own - script but we also provide you a simple script based on this case to get that - information. The provided tool ``calc_timeprop_charges.py`` will do the job. + about partial charge motion during dynamics. If you are interested in what is + happening with the charge of one molecule in your system, you can sum the + net atomic charges of the atoms of such a molecule to get the net molecular charge over time. + +3. As we are interested in the charge transfer between both molecules we want to analyse the net + charge of each molecule during the dynamics. For this purpose, you could write your own + script but we also provide you with a simple script which works fine for this case. The provided tool ``calc_timeprop_charges.py``, which you can find in the same directory as the template input file, will do the job. Try:: ./calc_timeprop_charges.py --help @@ -419,7 +393,7 @@ Laser dynamics on the donor-acceptor aggregate for charge transfer You will have to define the ranges of atoms that correspond to each of the two molecules. In our case, the PDI derivative is between atom 1 and 52 - and the carbazole derivative is between atom 53 and 83. Then, you may do:: + and the carbazole derivative is between atom 53 and 83. Then, you may run:: ./calc_timeprop_charges.py -l 1:52,53:83 @@ -434,9 +408,8 @@ Laser dynamics on the donor-acceptor aggregate for charge transfer Charge vs time for the accpetor and donor molecules. - where it is clearly shown that during the dynamic the PDI molecule act as - an accpetor of electrons getting negative values, meanwhile the carbazole is - getting positive. This confirm the charge transfer upon ilumination. + where it is clear that the PDI molecule act as + an acceptor of electrons (net charge goes negative), while the carbazole is donating electrons (net charge goes positive). If we follow the protocol from before, ploting the populations and searching for the orbitals involved in the transition, we should be able to get some insigths on the mechanism of the charge transfer (follow the steps in the @@ -447,25 +420,23 @@ Laser dynamics on the donor-acceptor aggregate for charge transfer :align: center :alt: molpopul CT - (left)Populations vs time for the pulse dynamics. (right) Orbitals involved + (left)Populations vs time for pulse-driven dynamics. (right) Orbitals involved in the excitation during the dynamics. the orbitals involved in the excitation with the pulse are localized in the PDI molecule, i.e. we can confirm that we are exciting the PDI molecule in its own HOMO-LUMO transition (and not an HOMO-LUMO transition of the whole system). Comparing with the previous figure of the charges dynamics, we can - also see that the CT process start just after a certain amount of electrons + also see that the CT process start after a certain amount of electrons are excited in the PDI molecule (more or less 30 fs, the duration of the pulse used). So we could in principle divide the mechanism in two steps. The first one, from 0 to ~30 fs where the PDI is beeing excited. The second step is the - charge transfer from the carbazole to the PDI once the last is already excited. + charge transfer from the carbazole to the PDI once the latter is already excited. -We hope that this tutorial would be helpful for those interested in get into the real-time TDDFTB -method using ``DFTB+``. Of course, this is just the beginning and there are much more possibilities -to do in terms of studyng optical properties and photoinduced processes within this approach in many -different scenarios and materials like *graphene nanoribbons*, *plasmonic nanoparticles*, *glod nanoclusters*, +We hope that this tutorial is helpful for those interested in get into the real-time TDDFTB +method using ``DFTB+``. Of course, these are just the basics and there are many more possibilities in terms of calculating optical properties and photoinduced processes within this approach for a wide range of materials and system like *graphene nanoribbons*, *plasmonic nanoparticles*, *glod nanoclusters*, *semiconductor nanoparticles* and *organic solar cells*. As an inspiration, we give you some references of -the last works performed with this method in ``DFTB+``: +recent works performed with this method in ``DFTB+``: **Fano Resonance and Incoherent Interlayer Excitons in Molecular van der Waals Heterostructures.** Lien-Medrano, C. R., Bonafé, F. P., Yam, C. Y., Palma, C.-A., Sánchez, C. G., & Frauenheim, T. (2022). Nano Letters, 22(3), 911–917. `https://doi.org/10.1021/acs.nanolett.1c03441 `_ @@ -473,16 +444,4 @@ the last works performed with this method in ``DFTB+``: **Photoinduced charge-transfer in chromophore-labeled gold nanoclusters: quantum evidence of the critical role of ligands and vibronic couplings.** Domínguez-Castro, A., Lien-Medrano, C. R., Maghrebi, K., Messaoudi, S., Frauenheim, T., & Fihey, A. (2021). Nanoscale, 13(14), 6786–6797. `https://doi.org/10.1039/D1NR00213A `_ -**Interplay between Intra- And Interband Transitions Associated with the Plasmon-Induced Hot Carrier Generation Process in Silver and Gold Nanoclusters.** Berdakin, M., Douglas-Gallardo, O. A., & Sánchez, C. G. (2020). Journal of Physical Chemistry C, 1631–1639. `https://doi.org/10.1021/acs.jpcc.9b10871 `_ - -**Plasmon-induced hot-carrier generation differences in gold and silver nanoclusters.** Douglas-Gallardo, O. A., Berdakin, M., Frauenheim, T., & Sánchez, C. G. (2019). Nanoscale, 11(17), 8604–8615. `https://doi.org/10.1039/c9nr01352k `_ - -**Trap-Door-Like Irreversible Photoinduced Charge Transfer in a Donor-Acceptor Complex.** Medrano, C. R., & Sánchez, C. G. (2018). Journal of Physical Chemistry Letters, 9(12), 3517–3524. `https://doi.org/10.1021/acs.jpclett.8b01043 `_ - -**Quantum efficiency of the photo-induced electronic transfer in dye–TiO 2 complexes.** Marquez, D. M., & Sánchez, C. G. (2018). Physical Chemistry Chemical Physics, 20(41), 26280–26287. `https://doi.org/10.1039/C8CP04625E `_ - -**Characterization of ZnO as substrate for DSSC.** Mansilla Wettstein, C., & Sánchez, C. G. (2018). Physical Chemistry Chemical Physics, 20(34), 21910–21916. `https://doi.org/10.1039/C8CP01709C `_ - **Plasmon-driven sub-picosecond breathing of metal nanoparticles.** Bonafé, F. P., Aradi, B., Guan, M., Douglas-Gallardo, O. A., Lian, C., Meng, S., Frauenheim, T., & Sánchez, C. G. (2017). Nanoscale, 9(34), 12391–12397. `https://doi.org/10.1039/C7NR04536K `_ - -**Photoinduced charge-transfer dynamics simulations in noncovalently bonded molecular aggregates.** Medrano, C. R., Oviedo, M. B., & Sánchez, C. G. (2016). Physical Chemistry Chemical Physics, 18(22), 14840–14849. `https://doi.org/10.1039/c6cp00231e `_ From 282842044c4dab18874f40d74d2c0da50f939d48 Mon Sep 17 00:00:00 2001 From: Charly Medrano Date: Mon, 4 Jul 2022 12:11:45 +0200 Subject: [PATCH 12/14] Add refs to figs and secs --- docs/electronicdynamics/driving.rst | 1 + docs/electronicdynamics/spectra.rst | 1 + docs/electronicdynamics/tutorial.rst | 82 ++++++++++++++++++---------- 3 files changed, 55 insertions(+), 29 deletions(-) diff --git a/docs/electronicdynamics/driving.rst b/docs/electronicdynamics/driving.rst index 4b48d17d..0b2fdbb9 100644 --- a/docs/electronicdynamics/driving.rst +++ b/docs/electronicdynamics/driving.rst @@ -1,4 +1,5 @@ .. highlight:: none +.. _sec-driving: ************************************************ Driving electronic dynamics with external fields diff --git a/docs/electronicdynamics/spectra.rst b/docs/electronicdynamics/spectra.rst index 76bfce08..d07b9402 100644 --- a/docs/electronicdynamics/spectra.rst +++ b/docs/electronicdynamics/spectra.rst @@ -1,4 +1,5 @@ .. highlight:: none +.. _sec-spectra: ******************************************** Calculation of electronic absorption spectra diff --git a/docs/electronicdynamics/tutorial.rst b/docs/electronicdynamics/tutorial.rst index 3a981bf1..a3838d7b 100644 --- a/docs/electronicdynamics/tutorial.rst +++ b/docs/electronicdynamics/tutorial.rst @@ -1,9 +1,8 @@ .. highlight:: none -*********************************************************************** -Tutorial: Absorption spectra, analysis and charge transfer -*********************************************************************** - +******************************************************************* +Tutorial: Photoinduced charge transfer in a donor-acceptor complex. +******************************************************************* This is the tutorial given at the DFTB+ School 2022 in Daresbury, UK. The idea is to get familiar with the real-time TDDFTB method applied to molecules and molecular complexes, learning the basics of absorption spectra calculations and photoinduced processes such as charge transfer under laser irradiation. @@ -22,15 +21,17 @@ Calculation of the absorption spectrum of carbazole We will calculate the absorption spectrum of the carbazole molecule, following the procedure described in :ref:`sec-spectra`. 1. Take a look at the input coordinates *coords.gen*. The *.gen* format - is the one used for DFTB+ code. In order to visualize the molecule, + is the one used for DFTB+ code (see section :ref:`gen_format` for more details). In order to visualize the molecule, you can use the ``gen2xyz`` script, provided in the installation of the DFTB+ code, by running:: gen2xyz coords.gen This will generate a *coords.xyz* that you can open with VMD, Avogadro or - any other molecular visualization software of your choice. + any other molecular visualization software of your choice. An image of the + carbazole molecule made with VMD is presented in :numref:`fig_carbazole`. + .. _fig_carbazole: .. figure:: ../_figures/elecdynamics/tutorial/carbazole.png :height: 30ex :align: center @@ -81,8 +82,9 @@ We will calculate the absorption spectrum of the carbazole molecule, following t 4. After running the script you will find two new files: *spec-nm.dat* and *spec-ev.dat* which are the absorption spectra in nm and eV, respectively. Plot the spectrum file with the plotting tool of your choice and look at the lowest energy transitions. You should then see - an absorption spectrum similar to: + an absorption spectrum similar to :numref:`fig_carbazole_spec`. + .. _fig_carbazole_spec: .. figure:: ../_figures/elecdynamics/tutorial/spec-nm-carbazole.png :width: 60% :align: center @@ -92,9 +94,10 @@ We will calculate the absorption spectrum of the carbazole molecule, following t 5. Change the damping constant for a higher value, recalculate the specctrum and plot both spectra together. What is the effect of the damping time in the spectrum? - Here it is an example of the same spectrum calculated with + In :numref:`fig_carbazole_spec_damp` can be seen the same spectrum calculated with different values of the damping constant. + .. _fig_carbazole_spec_damp: .. figure:: ../_figures/elecdynamics/tutorial/specs-comparison-damp.png :width: 60% :align: center @@ -177,11 +180,17 @@ finding first the lowest energy transition of the molecule in the spectrum plott - Why we should use this laser polarization instead of any other? -4. After the dynamics, take a look at the *mu.dat* file. +4. After the dynamics, take a look at the *mu.dat* file. You could plot the 3 + componets of the dipole moment by doing:: - - Is the dipole moment increasing linearly? + xmgrace -nxy mu.dat + + In :numref:`fig_carbazole_mu` the dipole moment is plotted. - .. figure:: ../_figures/ele.. _sec-driving:cdynamics/tutorial/mu-carbazole-components.png + - Is the dipole moment increasing linearly? + + .. _fig_carbazole_mu: + .. figure:: ../_figures/elecdynamics/tutorial/mu-carbazole-components.png :width: 60% :align: center :alt: mu components @@ -189,12 +198,18 @@ finding first the lowest energy transition of the molecule in the spectrum plott Dipole moment components vs time for the laser dynamics. 5. Take a look at the *molpopul1.dat* file - generated. This file contains the populations projected on the GS orbitals during the dynamics. + generated. This file contains the populations projected on the GS orbitals during the dynamics:: + + # GS molecular orbital populations, spin channel : 1 + #time (fs) | population (orb 1) | population (orb 2) | ... | population (orb N) | + 0.237050663997490 1.999999999825206 1.999999999780047 1.999999999771997 ... + 0.478939096647990 1.999999999978780 1.999999999983538 1.999999999962606 ... + 0.720827529298490 1.999999999870651 1.999999999913354 1.999999999904491 ... - Which orbitals are involved in the transition? Help: you can plot the *molpopul1.dat* file using `xmgrace`:: - xmgrace -nxy molpopul.dat + xmgrace -nxy molpopul1.dat Look at the populations initially at y=2 (occupied orbitals in the GS basis) and find which curves are decreasing over time, these are the orbitals @@ -216,10 +231,9 @@ finding first the lowest energy transition of the molecule in the spectrum plott where it is clear that states 31 and 32 are the HOMO and LUMO of the molecule, respectively. -6. Let's visualize those orbitals using ``waveplot``. For a complete description please check :ref:`basics-waveplot`. +6. Let's visualize those orbitals using ``waveplot``. For a complete description please check :ref:`sec-basics-waveplot`. - Look at the *waveplot_in.hsd_* template input file for waveplot: - - Which files are needed? - In which orbitals are we interested? @@ -237,9 +251,10 @@ finding first the lowest energy transition of the molecule in the spectrum plott `VESTA `_ allows the user to open directly cube files showing the isosurface immediately with some default parameters, making it a really good option for quick inspections. -As a reference, here are the populations obtained from the laser dynamics -and the orbitals involved in the transition: +As a reference, we plotted the populations obtained from the laser dynamics +and the orbitals involved in the transition in :numref:`fig_carbazole_pops`. +.. _fig_carbazole_pops: .. figure:: ../_figures/elecdynamics/tutorial/molpopul-carbazole.png :width: 100% :align: center @@ -250,7 +265,7 @@ and the orbitals involved in the transition: Now it's your turn! Calculation of PDI absorption spectrum --------------------------------------------------------- +---------------------------------------------------------- [Input: `recipes/electronicdynamics/tutorial/01_spectra_and_laser/02_PDI/``] @@ -264,8 +279,9 @@ molecule, PDI. - Apply a laser tuned with this transition. - Obtain the orbitals involved in the transition using waveplot and plot them. -Reference results: +The reference results are plotted in :numref:`fig_PDI` +.. _fig_PDI: .. figure:: ../_figures/elecdynamics/tutorial/PDI.png :width: 100% :align: center @@ -284,24 +300,29 @@ Calculate the absorption spectrum of a donor-acceptor aggregate [Input: `recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/`] -1. Visualize the coordinates file *coords.xyz* - +1. Visualize the coordinates file *coords.xyz*. + + .. _fig_aggregate: .. figure:: ../_figures/elecdynamics/tutorial/PDI+carbazole.png :width: 60% :align: center :alt: PDI+carbazole aggregate PDI+carbazole derivatives aggregate -` + It is an aggregate of the two previous molecules, in which the carbazole and PDI derivatives act as donor and acceptor of electrons, respectively. + - Convert the coordinates into *gen* format (using the ``xyz2gen`` script) and calculate the absorption spectrum using the *dftb_in.hsd_spec* as a template for the input (copy this file or rename it as *dftb_in.hsd*). 2. Compare the calculated spectrum with the individual ones (you can use the spectra - calculated before or recalculate them from these derivatives). For the comparison to be valid, you should use the same damping constant for all spectra. Are there relevant differences? - + calculated before or recalculate them from these derivatives). For the comparison to be valid, + you should use the same damping constant for all spectra. Are there relevant differences? + See :numref:`fig_specs_AD`. + + .. _fig_specs_AD: .. figure:: ../_figures/elecdynamics/tutorial/specs-compar-A+D.png :width: 60% :align: center @@ -315,8 +336,8 @@ Calculate the absorption spectrum of a donor-acceptor aggregate puropose, we will perform a driven simulation in next step and for it, we need to calculate the transition dipole direction of the absorption band at ~530 nm. Calculate this vector using the ``calc_timeprop_maxpoldir`` tool. You shold obtain something similar to:: - - PolarizationDirection = -0.99977 0.01777 0.01122 + + PolarizationDirection = -0.99977 0.01777 0.01122 which is essentially the *X* direction (since the PDI molecule axis is paralel to the *X* axis in the coordinates). @@ -399,8 +420,9 @@ Laser dynamics on the donor-acceptor aggregate and charge transfer After runing the script, two files may be generated: *charge_frag1.dat* and *charge_frag2.dat* with the corresponding charges of each defined fragment. - If you plot it you will get something like: - + If you plot it you will get something like in :numref:`fig_CT_AD`. + + .. _fig_CT_AD: .. figure:: ../_figures/elecdynamics/tutorial/charge-vs-time.png :width: 60% :align: center @@ -413,8 +435,9 @@ Laser dynamics on the donor-acceptor aggregate and charge transfer If we follow the protocol from before, ploting the populations and searching for the orbitals involved in the transition, we should be able to get some insigths on the mechanism of the charge transfer (follow the steps in the - previous sections). As it is shown in the figure: + previous sections). As it is shown in :numref:`fig_molpopul-CT`. + .. _fig_molpopul-CT: .. figure:: ../_figures/elecdynamics/tutorial/molpopul-CT.png :width: 100% :align: center @@ -445,3 +468,4 @@ recent works performed with this method in ``DFTB+``: **Photoinduced charge-transfer in chromophore-labeled gold nanoclusters: quantum evidence of the critical role of ligands and vibronic couplings.** Domínguez-Castro, A., Lien-Medrano, C. R., Maghrebi, K., Messaoudi, S., Frauenheim, T., & Fihey, A. (2021). Nanoscale, 13(14), 6786–6797. `https://doi.org/10.1039/D1NR00213A `_ **Plasmon-driven sub-picosecond breathing of metal nanoparticles.** Bonafé, F. P., Aradi, B., Guan, M., Douglas-Gallardo, O. A., Lian, C., Meng, S., Frauenheim, T., & Sánchez, C. G. (2017). Nanoscale, 9(34), 12391–12397. `https://doi.org/10.1039/C7NR04536K `_ + From 13999b1d71f2bbf9fcd2b3366e7cf5effd7c2e5a Mon Sep 17 00:00:00 2001 From: Charly Medrano Date: Wed, 13 Jul 2022 10:53:13 +0200 Subject: [PATCH 13/14] Add ref tutorial --- docs/electronicdynamics/tutorial.rst | 2 ++ 1 file changed, 2 insertions(+) diff --git a/docs/electronicdynamics/tutorial.rst b/docs/electronicdynamics/tutorial.rst index a3838d7b..0c2c019e 100644 --- a/docs/electronicdynamics/tutorial.rst +++ b/docs/electronicdynamics/tutorial.rst @@ -6,6 +6,8 @@ Tutorial: Photoinduced charge transfer in a donor-acceptor complex. This is the tutorial given at the DFTB+ School 2022 in Daresbury, UK. The idea is to get familiar with the real-time TDDFTB method applied to molecules and molecular complexes, learning the basics of absorption spectra calculations and photoinduced processes such as charge transfer under laser irradiation. +The tutorial is based on the following work: **Photoinduced charge-transfer dynamics simulations in noncovalently bonded molecular aggregates. +** Medrano, C. R., Oviedo, M. B., & Sánchez, C. G. (2016). Physical Chemistry Chemical Physics, 18(22), 14840–14849. `https://doi.org/10.1039/c6cp00231e `_ Spectra and analysis ==================== From 24252cf287c1b7c86ffed86b7c6576f5fa15471f Mon Sep 17 00:00:00 2001 From: =?UTF-8?q?B=C3=A1lint=20Aradi?= Date: Mon, 27 Feb 2023 23:36:45 +0100 Subject: [PATCH 14/14] Make formal changes --- .../electronicdynamics/driving/dftb_in.hsd | 58 ++-- .../electronicdynamics/ehrenfest/dftb_in.hsd | 58 ++-- .../electronicdynamics/spectrum/dftb_in.hsd | 53 ++-- .../01_carbazole/01_spectrum/dftb_in.hsd_spec | 55 ++-- .../01_carbazole/02_laser/dftb_in.hsd_laser | 65 ++-- .../01_aggregate_spec/dftb_in.hsd_spec | 57 ++-- .../02_aggregate_CT/dftb_in.hsd_pulse | 70 ++--- docs/electronicdynamics/driving.rst | 33 +- docs/electronicdynamics/ehrenfest.rst | 29 +- docs/electronicdynamics/introduction.rst | 6 +- docs/electronicdynamics/spectra.rst | 52 +--- docs/electronicdynamics/tutorial.rst | 282 +++++++++--------- 12 files changed, 361 insertions(+), 457 deletions(-) diff --git a/docs/_archives/recipes/electronicdynamics/driving/dftb_in.hsd b/docs/_archives/recipes/electronicdynamics/driving/dftb_in.hsd index 5fc92546..4e8930d4 100644 --- a/docs/_archives/recipes/electronicdynamics/driving/dftb_in.hsd +++ b/docs/_archives/recipes/electronicdynamics/driving/dftb_in.hsd @@ -1,39 +1,37 @@ InputVersion = 20.1 Geometry = GenFormat { - <<< "coords.gen" + <<< "coords.gen" } -Driver = {} - Hamiltonian = DFTB { - SCC = Yes - SCCTolerance = 1.0e-7 - SlaterKosterFiles = Type2FileNames { - Prefix = "../../slakos/download/3ob/3ob-3-1/" - Separator = "-" - Suffix = ".skf" - } - MaxAngularMomentum = { - Mg = "p" - C = "p" - N = "p" - O = "p" - H = "s" - } - Filling = Fermi { - Temperature [K] = 300 - } + Scc = Yes + SccTolerance = 1.0e-7 + SlaterKosterFiles = Type2FileNames { + Prefix = "../../slakos/download/3ob/3ob-3-1/" + Separator = "-" + Suffix = ".skf" + } + MaxAngularMomentum { + Mg = "p" + C = "p" + N = "p" + O = "p" + H = "s" + } + Filling = Fermi { + Temperature [K] = 300 + } } -ElectronDynamics = { - Steps = 60000 - TimeStep [au] = 0.2 - Perturbation = Laser { - PolarizationDirection = -0.08808129 0.99564018 -0.03069709 - LaserEnergy [eV] = 1.94944 - } - FieldStrength [V/A] = 0.0001 - Populations = Yes - WriteFrequency = 100 +ElectronDynamics { + Steps = 60000 + TimeStep [au] = 0.2 + Perturbation = Laser { + PolarizationDirection = -0.08808129 0.99564018 -0.03069709 + LaserEnergy [eV] = 1.94944 + } + FieldStrength [V/A] = 0.0001 + Populations = Yes + WriteFrequency = 100 } diff --git a/docs/_archives/recipes/electronicdynamics/ehrenfest/dftb_in.hsd b/docs/_archives/recipes/electronicdynamics/ehrenfest/dftb_in.hsd index 81b47344..b8010977 100644 --- a/docs/_archives/recipes/electronicdynamics/ehrenfest/dftb_in.hsd +++ b/docs/_archives/recipes/electronicdynamics/ehrenfest/dftb_in.hsd @@ -1,38 +1,38 @@ InputVersion = 20.1 Geometry = GenFormat { - <<< "coords.gen" + <<< "coords.gen" } Hamiltonian = DFTB { - SCC = Yes - SCCTolerance = 1.0E-9 - MaxAngularMomentum = { - C = "p" - H = "s" - } - Filling = Fermi { - Temperature [Kelvin] = 30 - } - SlaterKosterFiles = Type2FileNames { - Prefix = "../../slakos/download/3ob/3ob-3-1/" - Separator = "-" - Suffix = ".skf" - } + Scc = Yes + SccTolerance = 1.0E-9 + MaxAngularMomentum { + C = "p" + H = "s" + } + Filling = Fermi { + Temperature [Kelvin] = 30 + } + SlaterKosterFiles = Type2FileNames { + Prefix = "../../slakos/download/3ob/3ob-3-1/" + Separator = "-" + Suffix = ".skf" + } } -ElectronDynamics = { - Steps = 100000 - TimeStep [au] = 0.1 - Perturbation = Laser { - PolarizationDirection = 0.00000001 0.61419463 -0.78915459 - LaserEnergy [eV] = 6.834 - } - EnvelopeShape = Sin2 { - Time1 [fs] = 10.0 - } - FieldStrength [V/A] = 0.10 - IonDynamics = Yes - InitialTemperature [K] = 0.0 - Populations = Yes +ElectronDynamics { + Steps = 100000 + TimeStep [au] = 0.1 + Perturbation = Laser { + PolarizationDirection = 0.00000001 0.61419463 -0.78915459 + LaserEnergy [eV] = 6.834 + } + EnvelopeShape = Sin2 { + Time1 [fs] = 10.0 + } + FieldStrength [V/A] = 0.10 + IonDynamics = Yes + InitialTemperature [K] = 0.0 + Populations = Yes } diff --git a/docs/_archives/recipes/electronicdynamics/spectrum/dftb_in.hsd b/docs/_archives/recipes/electronicdynamics/spectrum/dftb_in.hsd index 2851ce86..302a35af 100644 --- a/docs/_archives/recipes/electronicdynamics/spectrum/dftb_in.hsd +++ b/docs/_archives/recipes/electronicdynamics/spectrum/dftb_in.hsd @@ -1,37 +1,36 @@ InputVersion = 20.1 Geometry = GenFormat { - <<< "coords.gen" + <<< "coords.gen" } -Driver = {} +Driver {} Hamiltonian = DFTB { - SCC = Yes - SCCTolerance = 1.0e-7 - SlaterKosterFiles = Type2FileNames { - Prefix = "../../slakos/download/3ob/3ob-3-1/" - Separator = "-" - Suffix = ".skf" - } - MaxAngularMomentum = { - Mg = "p" - C = "p" - N = "p" - O = "p" - H = "s" - } - Charge = 0.0 - Filling = Fermi { - Temperature [K] = 300 - } + Scc = Yes + SccTolerance = 1.0e-7 + SlaterKosterFiles = Type2FileNames { + Prefix = "../../slakos/download/3ob/3ob-3-1/" + Separator = "-" + Suffix = ".skf" + } + MaxAngularMomentum { + Mg = "p" + C = "p" + N = "p" + O = "p" + H = "s" + } + Filling = Fermi { + Temperature [K] = 300 + } } -ElectronDynamics = { - Steps = 20000 - TimeStep [au] = 0.2 - Perturbation = Kick { - PolarizationDirection = all - } - FieldStrength [V/A] = 0.001 +ElectronDynamics { + Steps = 20000 + TimeStep [au] = 0.2 + Perturbation = Kick { + PolarizationDirection = "all" + } + FieldStrength [V/A] = 0.001 } diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/01_spectrum/dftb_in.hsd_spec b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/01_spectrum/dftb_in.hsd_spec index cb31d61b..eafba6e4 100644 --- a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/01_spectrum/dftb_in.hsd_spec +++ b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/01_spectrum/dftb_in.hsd_spec @@ -1,40 +1,29 @@ +InputVersion = 21.2 + Geometry = GenFormat { - <<< "coords.gen" + <<< "coords.gen" } -Driver = {} - Hamiltonian = DFTB { - SCC = Yes - SCCTolerance = 1e-7 - MaxAngularMomentum = { - C = "p" - H = "s" - N = "p" - } - SlaterKosterFiles = Type2FileNames { - Prefix = "../../../../slakos/download/mio-1-1/" - Separator = "-" - Suffix = ".skf" - } + Scc = Yes + SccTolerance = 1e-7 + MaxAngularMomentum { + C = "p" + H = "s" + N = "p" + } + SlaterKosterFiles = Type2FileNames { + Prefix = "../../../../../slakos/download/mio/mio-1-1/" + Separator = "-" + Suffix = ".skf" + } } - ElectronDynamics = { - Steps = #define the time window - TimeStep [au] = #resolution of the spectrum - Perturbation = Kick { #must be a kick (Dirac delta) - PolarizationDirection = #desired direction/s - } - FieldStrength [v/a] = #Field strength of the perturbation - } - - -InputVersion = 21.2 - - -Parallel { - # Allow OMP threads explicitely to test for hybrid parallelisation with - # MPI-binary. (Check the manual before using this in production runs!) - UseOmpThreads = Yes +ElectronDynamics { + Steps = # define the time window + TimeStep [au] = # resolution of the spectrum + Perturbation = Kick { # must be a kick (Dirac delta) + PolarizationDirection = # desired direction/s + } + FieldStrength [V/A] = # field strength of the perturbation } - diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/dftb_in.hsd_laser b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/dftb_in.hsd_laser index 752094a3..dbacbfb9 100644 --- a/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/dftb_in.hsd_laser +++ b/docs/_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/dftb_in.hsd_laser @@ -1,50 +1,39 @@ +InputVersion = 21.2 + Geometry = GenFormat { - <<< "coords.gen" + <<< "coords.gen" } -Driver = {} - Hamiltonian = DFTB { - SCC = Yes - SCCTolerance = 1e-7 - MaxAngularMomentum = { - C = "p" - H = "s" - N = "p" - } - SlaterKosterFiles = Type2FileNames { - Prefix = "../../../../slakos/download/mio-1-1/" - Separator = "-" - Suffix = ".skf" - } + Scc = Yes + SccTolerance = 1e-7 + MaxAngularMomentum { + C = "p" + H = "s" + N = "p" + } + SlaterKosterFiles = Type2FileNames { + Prefix = "../../../../slakos/download/mio-1-1/" + Separator = "-" + Suffix = ".skf" + } } - ElectronDynamics = { - Steps = 10000 - TimeStep [au] = 0.2 - Perturbation = Laser{ # Laser type perturbation - PolarizationDirection = # calculate with calc_timeprop_maxpoldir - LaserEnergy [ev] = # energy of interest - } - FieldStrength [v/a] = 0.001 - Populations = Yes # to write populations during dynamic - } +ElectronDynamics { + Steps = 10000 + TimeStep [au] = 0.2 + Perturbation = Laser { # Laser type perturbation + PolarizationDirection = # calculate with calc_timeprop_maxpoldir + LaserEnergy [eV] = # energy of interest + } + FieldStrength [V/A] = 0.001 + Populations = Yes # to write GS-MP projected populations during dynamic +} Options { - WriteDetailedXML = Yes # needed for waveplot + WriteDetailedXml = Yes # needed for waveplot } Analysis { - WriteEigenvectors = Yes # needed for waveplot + WriteEigenvectors = Yes # needed for waveplot } - - -InputVersion = 21.2 - - -Parallel { - # Allow OMP threads explicitely to test for hybrid parallelisation with - # MPI-binary. (Check the manual before using this in production runs!) - UseOmpThreads = Yes -} - diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/dftb_in.hsd_spec b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/dftb_in.hsd_spec index 6886a940..9b88f2a8 100644 --- a/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/dftb_in.hsd_spec +++ b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/dftb_in.hsd_spec @@ -1,41 +1,30 @@ +InputVersion = 21.2 + Geometry = GenFormat { - <<< "coords.gen" + <<< "coords.gen" } -Driver = {} - Hamiltonian = DFTB { - SCC = Yes - SCCTolerance = 1e-7 - MaxAngularMomentum = { - C = "p" - H = "s" - N = "p" - O = "p" - } - SlaterKosterFiles = Type2FileNames { - Prefix = "../../../slakos/download/mio-1-1/" - Separator = "-" - Suffix = ".skf" - } + Scc = Yes + SccTolerance = 1e-7 + MaxAngularMomentum { + C = "p" + H = "s" + N = "p" + O = "p" + } + SlaterKosterFiles = Type2FileNames { + Prefix = "../../../slakos/download/mio-1-1/" + Separator = "-" + Suffix = ".skf" + } } - ElectronDynamics = { - Steps = 10000 #define the time window - TimeStep [au] = 0.2 #resolution of the spectrum - Perturbation = Kick { #must be a kick (Dirac delta) - PolarizationDirection = "all" #desired direction/s - } - FieldStrength [v/a] = 0.001 #Field strength of the perturbation - } - - -InputVersion = 21.2 - - -Parallel { - # Allow OMP threads explicitely to test for hybrid parallelisation with - # MPI-binary. (Check the manual before using this in production runs!) - UseOmpThreads = Yes +ElectronDynamics { + Steps = 10000 # define the time window + TimeStep [au] = 0.2 # resolution of the spectrum + Perturbation = Kick { # must be a kick (Dirac delta) + PolarizationDirection = "all" # desired direction/s + } + FieldStrength [V/A] = 0.001 # field strength of the perturbation } - diff --git a/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/dftb_in.hsd_pulse b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/dftb_in.hsd_pulse index d8af1e29..4c411214 100644 --- a/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/dftb_in.hsd_pulse +++ b/docs/_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/dftb_in.hsd_pulse @@ -1,49 +1,45 @@ +InputVersion = 21.2 + Geometry = GenFormat { - <<< "coords.gen" + <<< "coords.gen" } -Driver = {} - Hamiltonian = DFTB { - SCC = Yes - SCCTolerance = 1e-7 - MaxAngularMomentum = { - C = "p" - H = "s" - N = "p" - O = "p" - } - SlaterKosterFiles = Type2FileNames { - Prefix = "../../../slakos/download/mio-1-1/" - Separator = "-" - Suffix = ".skf" - } + Scc = Yes + SccTolerance = 1e-7 + MaxAngularMomentum { + C = "p" + H = "s" + N = "p" + O = "p" + } + SlaterKosterFiles = Type2FileNames { + Prefix = "../../../slakos/download/mio-1-1/" + Separator = "-" + Suffix = ".skf" + } } - ElectronDynamics = { - Steps = 20000 - TimeStep [au] = 0.2 - Perturbation = Laser{ - PolarizationDirection = #calculate with calc_timeprop_maxpoldir - #for the energy of interest - LaserEnergy [nm] = - } - EnvelopeShape = Sin2{ #envelope shape type - Time1 [fs] = 30.0 #pulse duration (assuming Time0 = 0, by default) - } - FieldStrength [v/a] = 0.02 #field strength bigger than spectrum case (0.001) - WriteEnergyAndCharges = Yes - Populations = Yes - } +ElectronDynamics { + Steps = 20000 + TimeStep [au] = 0.2 + Perturbation = Laser { + PolarizationDirection = # calculate with calc_timeprop_maxpoldir + # for the energy of interest + LaserEnergy [nm] = + } + EnvelopeShape = Sin2 { # envelope shape type + Time1 [fs] = 30.0 # pulse duration (assuming Time0 = 0, by default) + } + FieldStrength [V/A] = 0.02 # field strength bigger than spectrum case (0.001) + WriteEnergyAndCharges = Yes + Populations = Yes +} Options { - WriteDetailedXML = Yes #needed for waveplot + WriteDetailedXML = Yes # needed for waveplot } Analysis { - WriteEigenvectors = Yes #needed for waveplot + WriteEigenvectors = Yes # needed for waveplot } - -InputVersion = 21.2 - - diff --git a/docs/electronicdynamics/driving.rst b/docs/electronicdynamics/driving.rst index 0b2fdbb9..821e14c6 100644 --- a/docs/electronicdynamics/driving.rst +++ b/docs/electronicdynamics/driving.rst @@ -27,26 +27,19 @@ the eigenvector of the polarizability tensor at that energy that has the largest eigenvalue. It is equivalent to a principal axis of inertia in rigid body rotation. -Using the ``ElectronDynamics`` block that follows:: - - ElectronDynamics = { - Steps = 60000 - TimeStep [au] = 0.2 - Perturbation = Laser { - PolarizationDirection = -0.08808129 0.99564018 -0.03069709 - LaserEnergy [eV] = 1.94944 - } - FieldStrength [V/A] = 0.0001 - } +Using the ``ElectronDynamics`` block that follows: + +.. literalinclude:: ../_archives/recipes/electronicdynamics/driving/dftb_in.hsd + :lines: 27-37 We resonantly excite the Q band along the direction of its maximum polarizability. The obtained magnitude of the dipole moment as a function of time is shown in the following figure: - .. figure:: ../_figures/elecdynamics/muvst.png - :height: 40ex - :align: center - :alt: Dipole moment as a function of time. +.. figure:: ../_figures/elecdynamics/muvst.png + :height: 40ex + :align: center + :alt: Dipole moment as a function of time. An initial transient, the dipole moment maxima and minima grow in absolute value as a linear function of time after, confirming that the applied field is in @@ -61,11 +54,11 @@ Off-resonant excitation An *off resonance* excitation at 1.9 eV produces the following result for the dipole moment: - .. figure:: ../_figures/elecdynamics/muvst-oot.png - :height: 40ex - :align: center - :alt: Dipole moment as a function of time. - +.. figure:: ../_figures/elecdynamics/muvst-oot.png + :height: 40ex + :align: center + :alt: Dipole moment as a function of time. + showing characteristic *beats*, the frequency of which are related to the amount of *detuning*. The amplitude of the dipole moment change caused by the illumination is also much smaller that when the laser is *in tune* with the diff --git a/docs/electronicdynamics/ehrenfest.rst b/docs/electronicdynamics/ehrenfest.rst index bef0d182..ff93804f 100644 --- a/docs/electronicdynamics/ehrenfest.rst +++ b/docs/electronicdynamics/ehrenfest.rst @@ -24,23 +24,10 @@ Benzene example As an example of Ehrenfest dynamics, starting from the equilibrium geometry we can excite the lowest-lying :math:`\pi-\pi^*` excitation of a benzene molecule using a short laser pulse, and explicitly allow the ions to move. In this case, -the ``ElectronDynamics`` blocks is as follows:: +the ``ElectronDynamics`` blocks is as follows: - ElectronDynamics = { - Steps = 100000 - TimeStep [au] = 0.1 - Perturbation = Laser { - PolarizationDirection = 0.00000001 0.61419463 -0.78915459 - LaserEnergy [eV] = 6.834 # pi-pi* transition energy - } - EnvelopeShape = Sin2 { - Time1 [fs] = 10.0 # end-time of the pulse - } - FieldStrength [V/A] = 0.10 - IonDynamics = Yes - InitialTemperature [K] = 0.0 - Populations = Yes - } +.. literalinclude:: ../_archives/recipes/electronicdynamics/ehrenfest/dftb_in.hsd + :lines: 24-38 The keyword ``IonDynamics`` is set to ``Yes`` and for this example, we are starting with zero initial atomic velocities. The short, but strong, laser pulse @@ -49,11 +36,11 @@ electronic structure impulsively drives the nuclei to move. In the following figure, we plot the distances between neighbouring carbon atoms in the benzene ring: - .. figure:: ../_figures/elecdynamics/CC-dist.png - :height: 60ex - :align: center - :alt: Carbon-carbon distances for benzene following excitation by a laser - pulse. +.. figure:: ../_figures/elecdynamics/CC-dist.png + :height: 60ex + :align: center + :alt: Carbon-carbon distances for benzene following excitation by a laser + pulse. After the short excitation, all carbon atoms move in a *breathing* motion with all distances increasing and decreasing periodically. The breathing is not diff --git a/docs/electronicdynamics/introduction.rst b/docs/electronicdynamics/introduction.rst index 18d12e09..c0cec815 100644 --- a/docs/electronicdynamics/introduction.rst +++ b/docs/electronicdynamics/introduction.rst @@ -1,5 +1,5 @@ .. _sec-electrondynamics: - + ******************* Electronic dynamics ******************* @@ -37,7 +37,7 @@ The EOM for the density matrix is integrated using a Leapfrog scheme in which the density matrix at time :math:`t_{i+i}` is obtained from its value a t time :math:`t_{i-1}` and its derivative at time :math:`t_i`: - :math:`\rho_{i+1}=\rho_{i-1}+2\Delta t \dot{\rho}_i.` +.. math:: \rho_{i+1}=\rho_{i-1}+2\Delta t \dot{\rho}_i. The nuclear motion is integrated using a velocity Verlet algorithm. @@ -46,7 +46,7 @@ calculation of absorption spectra, to study the response to constant or pulsed excitation and even the simulation of pump-probe spectroscopy. All input related to electronic dynamics is located within the -*ElectronDynamics* block of the input file. Electron dynamics is run after +``ElectronDynamics`` block of the input file. Electron dynamics is run after ground state self consistency is achieved, with the possibility of reading previously converged charges for the ground state or the state of the time-evolving density matrix to continue time propagation. diff --git a/docs/electronicdynamics/spectra.rst b/docs/electronicdynamics/spectra.rst index d07b9402..29cbc51e 100644 --- a/docs/electronicdynamics/spectra.rst +++ b/docs/electronicdynamics/spectra.rst @@ -21,35 +21,9 @@ The input [Input: `recipes/electronicdynamics/spectrum/`] The following input can be used to calculate the absorption spectrum of -chlorophyll a:: - - Geometry = GenFormat { - <<< "coords.gen" - } - - Hamiltonian = DFTB { - SCC = Yes - SCCTolerance = 1.0e-7 - MaxAngularMomentum = { - Mg = "p" - C = "p" - N = "p" - O = "p" - H = "s" - } - Filling = Fermi { - Temperature [K] = 300 - } - } - - ElectronDynamics = { - Steps = 20000 - TimeStep [au] = 0.2 - Perturbation = Kick { - PolarizationDirection = all - } - FieldStrength [v/a] = 0.001 - } +chlorophyll a: + +.. literalinclude:: ../_archives/recipes/electronicdynamics/spectrum/dftb_in.hsd The optimised geometry is located in the *coords.gen* file. Note that for this example the long *phytol* chain present in the natural molecule has been @@ -58,11 +32,11 @@ influence on the absorption spectrum. For the calculation of absorption spectra, an initial kick of the system is made using a Dirac delta type perturbation. The input specifies that after the -initial perturbation of *Kick* type, twenty thousand steps of dynamics will be -executed using a time step of 0.2 atomic units. The *Kick* perturbation can be -applied in any of the Cartesian directions (*x*, *y* or *z*). The use of *all* -here in the input instructs the code to run three independent dynamic -calculations, one with an initial *Kick* in each Cartesian direction. +initial perturbation of ``Kick`` type, twenty thousand steps of dynamics will be +executed using a time step of 0.2 atomic units. The ``Kick`` perturbation can be +applied in any of the Cartesian directions (``x``, ``y`` or ``z``). The use of +``all`` here in the input instructs the code to run three independent dynamic +calculations, one with an initial ``Kick`` in each Cartesian direction. After self consistency has been achieved and the ground state density matrix is obtained, the perturbation is applied and then the propagation starts, the @@ -122,7 +96,7 @@ of induced dipole moment of the molecule in the presence of an external time dependent field (within the linear response range) is related to the Fourier transform of said field in the following manner: -:math:`\mathbf{mu}(\omega)=\overset\leftrightarrow{\alpha}(\omega)\mathbf{E}(\omega)` +.. math:: \mathbf{\mu}(\omega)=\overset\leftrightarrow{\alpha}(\omega)\,\mathbf{E}(\omega) since the Fourier transform of a Dirac delta is a constant at all frequencies, the polarizability tensor :math:`\overset\leftrightarrow{\alpha}(\omega)` can be @@ -147,10 +121,10 @@ equivalent to using a *windowing* function. The spectrum is located in the output files *spec-ev* and *spec-nm*. In this case the spectrum looks as follows: - .. figure:: ../_figures/elecdynamics/spectrum.png - :height: 40ex - :align: center - :alt: Absorption spectrum of chlorophyll a. +.. figure:: ../_figures/elecdynamics/spectrum.png + :height: 40ex + :align: center + :alt: Absorption spectrum of chlorophyll a. The band between 400 and 500 nm is called the Soret band and the one between 600 and 700 nm is the Q band. This band is the band that provides is responsible for diff --git a/docs/electronicdynamics/tutorial.rst b/docs/electronicdynamics/tutorial.rst index 0c2c019e..34fbd3ef 100644 --- a/docs/electronicdynamics/tutorial.rst +++ b/docs/electronicdynamics/tutorial.rst @@ -6,8 +6,8 @@ Tutorial: Photoinduced charge transfer in a donor-acceptor complex. This is the tutorial given at the DFTB+ School 2022 in Daresbury, UK. The idea is to get familiar with the real-time TDDFTB method applied to molecules and molecular complexes, learning the basics of absorption spectra calculations and photoinduced processes such as charge transfer under laser irradiation. -The tutorial is based on the following work: **Photoinduced charge-transfer dynamics simulations in noncovalently bonded molecular aggregates. -** Medrano, C. R., Oviedo, M. B., & Sánchez, C. G. (2016). Physical Chemistry Chemical Physics, 18(22), 14840–14849. `https://doi.org/10.1039/c6cp00231e `_ +The tutorial is based on the following work: **Photoinduced charge-transfer dynamics simulations in noncovalently bonded molecular aggregates.** Medrano, C. R., Oviedo, M. B., & Sánchez, C. G. (2016). Physical Chemistry Chemical Physics, 18(22), 14840–14849. `https://doi.org/10.1039/c6cp00231e `_ + Spectra and analysis ==================== @@ -15,6 +15,7 @@ Spectra and analysis We will first calculate the absorption spectra of two different molecules and analyse them using the tools provided by DFTB+. + Calculation of the absorption spectrum of carbazole --------------------------------------------------- @@ -24,9 +25,9 @@ We will calculate the absorption spectrum of the carbazole molecule, following t 1. Take a look at the input coordinates *coords.gen*. The *.gen* format is the one used for DFTB+ code (see section :ref:`gen_format` for more details). In order to visualize the molecule, - you can use the ``gen2xyz`` script, provided in the installation of the + you can use the ``gen2xyz`` script, provided in the installation of the DFTB+ code, by running:: - + gen2xyz coords.gen This will generate a *coords.xyz* that you can open with VMD, Avogadro or @@ -44,42 +45,39 @@ We will calculate the absorption spectrum of the carbazole molecule, following t 2. Open the *dftb_in.hsd_spec* file. This is a template for the calculation of the absorption spectrum. - - Take a look at the ``ElectronDynamics`` block at the end of the file:: - - ElectronDynamics = { - Steps = # defines the total simulation time - TimeStep [au] = # resolution of the spectrum - Perturbation = Kick { # external field is a kick (Dirac delta) - PolarizationDirection = # desired direction/s - } - FieldStrength [v/a] = # field strength of the kick - } + - Take a look at the ``ElectronDynamics`` block at the end of the file: + + .. literalinclude:: ../_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/01_spectrum/dftb_in.hsd_spec + :lines: 22-29 - The input variables to be considered for the calculation of the spectrum are four: * ``Steps`` (integer): the number of steps of the dynamics. The longer the dynamics, the lower the energies that can be resolved in the spectrum (the total time is also afected by the ``TimeStep``, of course). Here, we will use 10000 steps. - * ``TimeStep`` (float): the time step in time units. Here we use 0.2 a.u (0.0048 fs), which is normally stable for simulations of a few tens of thousands of steps. In case there is instability in the dynamics, the time step shuld be decreased. - * ``Perturbation``: In this case we need a Dirac-delta perturbation (AKA kick) and we need to - specify the ``PolarizationDirection`` that could be *X*, *Y*, *Z* (if we are interested in + + * ``TimeStep`` (float): the time step in time units. Here we use 0.2 a.u (0.0048 fs), which is normally stable for simulations of a few tens of thousands of steps. In case there is instability in the dynamics, the time step shuld be decreased. + + * ``Perturbation``: In this case we need a Dirac-delta perturbation (AKA kick) and we need to + specify the ``PolarizationDirection`` that could be *X*, *Y*, *Z* (if we are interested in one particular direction) or ``all`` if we want to calculate the three kicks consequtively and then calculate the spherically-averaged spectrum, accounting for random molecular orientations. Hence, we set it as ``all``. + * ``FieldStrength`` (float): the field strength of the perturbation applied. For the calculation of the absorption spectrum, it must be within the linear response regime, - i.e. usually 0.001 :math:`V/\AA` or lower. + i.e. usually 0.001 :math:`V/Å` or lower. - Complete the template file, copy it to *dftb_in.hsd* and run the calculation. 3. Once the dynamics ends, we will have calculated the time-resolved dipole moment using 3 field polarization directions (*mux.dat*, muy.dat, *muz.dat*). We need to average and Fourier-transform (or the other way around, as these are linear operations) these dipole components in order to obtain the absorption spectrum of the molecule. To do this, we will use the - ``calc_timeprop_spectrum`` tool available after installation of DFTB+ under: + ``calc_timeprop_spectrum`` tool available after installation of DFTB+ under: *dftbplus/tools/misc/*. In the folder where you have the dipole files just type:: calc_timeprop_spectrum -d 4 -f 0.001 - where the option -d is for the damping constant (artificial lifetime, in fs), which is equivalent to convoluting each resonance with a Lorentzian in time domain. - The option -f is the field strength of the kick (in :math:`V/\AA`). applied during dynamics. + where the option ``-d`` is for the damping constant (artificial lifetime, in fs), which is equivalent to convoluting each resonance with a Lorentzian in time domain. + The option ``-f`` is the field strength of the kick (in :math:`V/Å`) applied during dynamics. 4. After running the script you will find two new files: *spec-nm.dat* and *spec-ev.dat* which are the absorption spectra in nm and eV, respectively. Plot the spectrum file with the plotting tool @@ -94,7 +92,7 @@ We will calculate the absorption spectrum of the carbazole molecule, following t Absorption spectrum of carbazole molecule -5. Change the damping constant for a higher value, recalculate the specctrum and plot both spectra +5. Change the damping constant for a higher value, recalculate the spectrum and plot both spectra together. What is the effect of the damping time in the spectrum? In :numref:`fig_carbazole_spec_damp` can be seen the same spectrum calculated with different values of the damping constant. @@ -107,6 +105,7 @@ We will calculate the absorption spectrum of the carbazole molecule, following t Influence of the damping constant value ``d`` in the absorption spectrum. + Analysis of the absorption spectrum of carbazole: driving the system with a laser --------------------------------------------------------------------------------- @@ -115,69 +114,62 @@ Analysis of the absorption spectrum of carbazole: driving the system with a lase We will consider a laser perturbation in tune with the lowest energy transition of the molecule in order to study the photodynamic process of absorption in this transition. In order to do this, we -will follow the same procedure as described in :ref:`sec-driving`, +will follow the same procedure as described in :ref:`sec-driving`, finding first the lowest energy transition of the molecule in the spectrum plotted in the previous calculation, and then calculating the direction of maximal polarization of the transition. 1. Open the *dftb_in.hsd_laser* file. This is a template for the calculation of a laser perturbation. - - Take a look at the ``ElectronDynamics`` block at the end of the file:: - - ElectronDynamics = { - Steps = 10000 - TimeStep [au] = 0.2 - Perturbation = Laser{ # laser type perturbation - LaserEnergy [nm] = # energy or wavelength of interest - PolarizationDirection = # to be calculated with calc_timeprop_maxpoldir - } - FieldStrength [v/a] = 0.001 - Populations = Yes # to write GS-MP projected populations during the dynamics - } + - Take a look at the ``ElectronDynamics`` block at the end of the file: + + .. literalinclude:: ../_archives/recipes/electronicdynamics/tutorial/01_spectra_and_laser/01_carbazole/02_laser/dftb_in.hsd_laser + :lines: 22-31 Now, the ``Perturbation`` type is a continuous-wave ``laser``, for which we need to specify two parameters: - - * ``LaserEnergy`` (float): the energy of the applied laser that may be - the transition energy of interest. This value must be in energy units - like eV but also a wavelength in nm is allowed. - * ``PolarizationDirection`` (vector): in the case of a laser, the - ``PolarizationDirection`` is a 3-components vector. + + * ``LaserEnergy`` (float): the energy of the applied laser that may be + the transition energy of interest. This value must be in energy units + like eV but also a wavelength in nm is allowed. + + * ``PolarizationDirection`` (vector): in the case of a laser, the + ``PolarizationDirection`` is a 3-components vector. Note that we turned on the ``Populations`` flag in order to write the occupations during the dynamics. Also note that we are asking for the detailed xml and the eigenvectors with the ``WriteDetailedXML`` and ``WriteEigenvectors`` options. We will need them to plot the orbitals - with waveplot in the following sections. + with waveplot in the following sections. 2. To complete the input template for the laser, we need to provide - the ``LaserEnergy`` and the ``PolarizationDirection`` of the laser. Based on - our previous calculated spectrum, calculate the direction of maximal + the ``LaserEnergy`` and the ``PolarizationDirection`` of the laser. Based on + our previous calculated spectrum, calculate the direction of maximal polarization of the lowest energy transition of the molecule. - Help: use the tool ``calc_timeprop_maxpoldir`` already available in your installation (under: *dftbplus/tools/misc/*). To know how this tool work the user can just type:: - calc_timeprop_maxpoldir -h + calc_timeprop_maxpoldir -h - Along which axis/axes is the polarization of the molecule oriented? Why? - + - Hint: try to visualize the molecule and see how it is oriented with respect to the cartesian axes. - - + Solution: If you choose the lower energy transition of carbazole you may do:: - - calc_timeprop_maxpoldir -10 -w 326 + + - Solution: If you choose the lower energy transition of carbazole you may do:: + + calc_timeprop_maxpoldir -10 -w 326 and you will obtain the following transition dipole vector:: - - PolarizationDirection = 0.99999 0.00101 -0.003815 + + PolarizationDirection = 0.99999 0.00101 -0.003815 which is essentially paralel to the *X* cartesian direction (because of the molecules orientation with respect to the cartesian axes) 3. Prepare the input for the dynamics under a continuous laser perturbation. Use the energy obtained from the spectrum as the ``LaserEnergy`` - and the vector obtained above as the ``PolarizationDirection`` of the + and the vector obtained above as the ``PolarizationDirection`` of the laser. - Why we should use this laser polarization instead of any other? @@ -190,7 +182,7 @@ finding first the lowest energy transition of the molecule in the spectrum plott In :numref:`fig_carbazole_mu` the dipole moment is plotted. - Is the dipole moment increasing linearly? - + .. _fig_carbazole_mu: .. figure:: ../_figures/elecdynamics/tutorial/mu-carbazole-components.png :width: 60% @@ -201,17 +193,17 @@ finding first the lowest energy transition of the molecule in the spectrum plott 5. Take a look at the *molpopul1.dat* file generated. This file contains the populations projected on the GS orbitals during the dynamics:: - - # GS molecular orbital populations, spin channel : 1 - #time (fs) | population (orb 1) | population (orb 2) | ... | population (orb N) | - 0.237050663997490 1.999999999825206 1.999999999780047 1.999999999771997 ... - 0.478939096647990 1.999999999978780 1.999999999983538 1.999999999962606 ... - 0.720827529298490 1.999999999870651 1.999999999913354 1.999999999904491 ... + + # GS molecular orbital populations, spin channel : 1 + #time (fs) | population (orb 1) | population (orb 2) | ... | population (orb N) | + 0.237050663997490 1.999999999825206 1.999999999780047 1.999999999771997 ... + 0.478939096647990 1.999999999978780 1.999999999983538 1.999999999962606 ... + 0.720827529298490 1.999999999870651 1.999999999913354 1.999999999904491 ... - Which orbitals are involved in the transition? Help: you can plot the *molpopul1.dat* file using `xmgrace`:: - xmgrace -nxy molpopul1.dat + xmgrace -nxy molpopul1.dat Look at the populations initially at y=2 (occupied orbitals in the GS basis) and find which curves are decreasing over time, these are the orbitals @@ -219,31 +211,32 @@ finding first the lowest energy transition of the molecule in the spectrum plott Look at the populations initially at y=0 (unoccopied orbitals in the GS basis) and find the orbitals being populated over time. - You could also check in the *band.out* file generated from the SCC - calculation the states numbers. Close to the Fermi energy, you + You could also check in the *band.out* file generated from the SCC + calculation the states numbers. Close to the Fermi energy, you should see something like:: - 29 -6.641 2.00000 - 30 -5.809 2.00000 - 31 -5.512 2.00000 #HOMO - 32 -1.983 0.00000 #LUMO - 33 -1.358 0.00000 - 34 -0.501 0.00000 + 29 -6.641 2.00000 + 30 -5.809 2.00000 + 31 -5.512 2.00000 #HOMO + 32 -1.983 0.00000 #LUMO + 33 -1.358 0.00000 + 34 -0.501 0.00000 - where it is clear that states 31 and 32 are the HOMO - and LUMO of the molecule, respectively. + where it is clear that states 31 and 32 are the HOMO + and LUMO of the molecule, respectively. 6. Let's visualize those orbitals using ``waveplot``. For a complete description please check :ref:`sec-basics-waveplot`. - - Look at the *waveplot_in.hsd_* template input file for waveplot: - - - Which files are needed? - - In which orbitals are we interested? + - Look at the *waveplot_in.hsd_* template input file for waveplot: + + - Which files are needed? - - After editing this file, just rename it to *waveplot_in.hsd* and run - ``waveplot`` using your current installed executable, which should be in the same installation directory as the `dftbplus` executable. + - In which orbitals are we interested? - - After running waveplot, a number of files would be generated starting with "wp-1-1". + - After editing this file, just rename it to *waveplot_in.hsd* and run + ``waveplot`` using your current installed executable, which should be in the same installation directory as the `dftbplus` executable. + + - After running waveplot, a number of files would be generated starting with "wp-1-1". 7. Let's plot these orbitals: @@ -262,12 +255,14 @@ and the orbitals involved in the transition in :numref:`fig_carbazole_pops`. :align: center :alt: molpopul1-carbazole - (left)Populations vs time for the laser dynamics. (right) Orbitals involved + (left) Populations vs time for the laser dynamics. (right) Orbitals involved in the lower energy transition of the carbazole molecule. +Now it's your turn! + -Now it's your turn! Calculation of PDI absorption spectrum ----------------------------------------------------------- +Calculation of PDI absorption spectrum +-------------------------------------- [Input: `recipes/electronicdynamics/tutorial/01_spectra_and_laser/02_PDI/``] @@ -276,12 +271,15 @@ molecule, PDI. 1. Based on the calculations that you ran before. - - Calculate the absorption spectrum with a proper *dftb_in.hsd* input file. - - Find the lowest energy transition. - - Apply a laser tuned with this transition. - - Obtain the orbitals involved in the transition using waveplot and plot them. + - Calculate the absorption spectrum with a proper *dftb_in.hsd* input file. + + - Find the lowest energy transition. + + - Apply a laser tuned with this transition. + + - Obtain the orbitals involved in the transition using waveplot and plot them. -The reference results are plotted in :numref:`fig_PDI` +The reference results are plotted in :numref:`fig_PDI` .. _fig_PDI: .. figure:: ../_figures/elecdynamics/tutorial/PDI.png @@ -289,10 +287,11 @@ The reference results are plotted in :numref:`fig_PDI` :align: center :alt: PDI - \(a\) Absorption spectrum of the PDI molecule.\(b\) PDI molecule structure.\(c\) Dipole - moment components vs time during a laser dynamics at 548 nm (note that in - this case the dipole moment in the *X* direction increases linearly).\(d\) Populations - vs time for the laser dynamics.\(e\) Orbitals involved in the transition. + \(a\) Absorption spectrum of the PDI molecule. \(b\) PDI molecule structure. \(c\) Dipole + moment components vs time during a laser dynamics at 548 nm (note that in + this case the dipole moment in the *X* direction increases linearly). \(d\) Populations + vs time for the laser dynamics. \(e\) Orbitals involved in the transition. + Photoinduced charge transfer ============================ @@ -303,7 +302,7 @@ Calculate the absorption spectrum of a donor-acceptor aggregate [Input: `recipes/electronicdynamics/tutorial/02_photoinduced_CT/01_aggregate_spec/`] 1. Visualize the coordinates file *coords.xyz*. - + .. _fig_aggregate: .. figure:: ../_figures/elecdynamics/tutorial/PDI+carbazole.png :width: 60% @@ -315,15 +314,15 @@ Calculate the absorption spectrum of a donor-acceptor aggregate It is an aggregate of the two previous molecules, in which the carbazole and PDI derivatives act as donor and acceptor of electrons, respectively. - - Convert the coordinates into *gen* format (using the ``xyz2gen`` script) and - calculate the absorption spectrum using the *dftb_in.hsd_spec* as a template - for the input (copy this file or rename it as *dftb_in.hsd*). + - Convert the coordinates into *gen* format (using the ``xyz2gen`` script) and + calculate the absorption spectrum using the *dftb_in.hsd_spec* as a template + for the input (copy this file or rename it as *dftb_in.hsd*). 2. Compare the calculated spectrum with the individual ones (you can use the spectra calculated before or recalculate them from these derivatives). For the comparison to be valid, you should use the same damping constant for all spectra. Are there relevant differences? See :numref:`fig_specs_AD`. - + .. _fig_specs_AD: .. figure:: ../_figures/elecdynamics/tutorial/specs-compar-A+D.png :width: 60% @@ -331,19 +330,20 @@ Calculate the absorption spectrum of a donor-acceptor aggregate :alt: A+D spectrum Absorption spectrum of the PDI+carbazole derivatives aggregate (in black), - compared to the individual spectrum for the PDI moiety (in orange) and + compared to the individual spectrum for the PDI moiety (in orange) and the carbazole moiety (in red). 3. We are interested in the dynamics upon ilumination of the acceptor molecule. For such puropose, we will perform a driven simulation in next step and for it, we need to calculate the transition dipole direction of the absorption band at ~530 nm. Calculate this vector using the ``calc_timeprop_maxpoldir`` tool. You shold obtain something similar to:: - - PolarizationDirection = -0.99977 0.01777 0.01122 - which is essentially the *X* direction (since the PDI molecule axis is + PolarizationDirection = -0.99977 0.01777 0.01122 + + which is essentially the *X* direction (since the PDI molecule axis is paralel to the *X* axis in the coordinates). + Laser dynamics on the donor-acceptor aggregate and charge transfer ------------------------------------------------------------------ @@ -353,77 +353,67 @@ Laser dynamics on the donor-acceptor aggregate and charge transfer your input file for a laser-driven electron dynamics in tune with the acceptor (PDI) lowest energy excitation. Use the *dftb_in.hsd_pulse* as a template. Note that this time we add an envelope function to the laser perturbation in order - to mimic a laser pulse:: - - ElectronDynamics = { - Steps = 20000 - TimeStep [au] = 0.2 - Perturbation = Laser{ - PolarizationDirection = # to be completed - LaserEnergy [nm] = # to be completed - } - EnvelopeShape = Sin2{ # envelope shape type - Time1 [fs] = 30.0 # pulse duration (by default the initial time is Time0 = 0) - } - FieldStrength [v/a] = 0.02 # larger field strength than the kick (0.001) to observe driven dynamics clearly - Populations = Yes - } - - Now in the ElectronDynamics we added the Sin2 ``EnvelopeShape`` with + to mimic a laser pulse: + + .. literalinclude:: ../_archives/recipes/electronicdynamics/tutorial/02_photoinduced_CT/02_aggregate_CT/dftb_in.hsd_pulse + :lines: 23-37 + + Now in the ElectronDynamics we added the ``Sin2`` ``EnvelopeShape`` with a duration of 30 fs starting at the beginning of the dynamics. We will also ask the code to print the populations during dynamics to study the - mechanism of charge transfer. Complete the input template filling the - ``PolarizationDirection`` and ``LaserEnergy`` obtained before and run the + mechanism of charge transfer. Complete the input template filling the + ``PolarizationDirection`` and ``LaserEnergy`` obtained before and run the code (don't forget to rename the template to *dftb_in.hsd*). 2. After running the electron dynamics, let inspect the *qsvst.dat* file:: - #time (fs) | total net charge (e) | charge (atom_1) (e) | ... | charge (atom_N) (e)| - 0.000000000000000 -0.000000000000055 0.075753114169209 0.077680106829215 ... - 0.241888432650500 -0.000000000000048 0.075753940652948 0.077680933651269 ... - 0.483776865301000 -0.000000000000049 0.075758821681684 0.077685768802125 ... + #time (fs) | total net charge (e) | charge (atom_1) (e) | ... | charge (atom_N) (e)| + 0.000000000000000 -0.000000000000055 0.075753114169209 0.077680106829215 ... + 0.241888432650500 -0.000000000000048 0.075753940652948 0.077680933651269 ... + 0.483776865301000 -0.000000000000049 0.075758821681684 0.077685768802125 ... The first column of the file is the time and the second one is the total net charge of the system at each time step (which should be always close to zero, within numerical error). After that, each column is the net atomic charge at each time step. Making use of the file *qsvst.dat* one may potencially get information - about partial charge motion during dynamics. If you are interested in what is + about partial charge motion during dynamics. If you are interested in what is happening with the charge of one molecule in your system, you can sum the net atomic charges of the atoms of such a molecule to get the net molecular charge over time. 3. As we are interested in the charge transfer between both molecules we want to analyse the net charge of each molecule during the dynamics. For this purpose, you could write your own script but we also provide you with a simple script which works fine for this case. The provided tool ``calc_timeprop_charges.py``, which you can find in the same directory as the template input file, will do the job. + Try:: - ./calc_timeprop_charges.py --help + ./calc_timeprop_charges.py --help + + to get info about how to use the script:: - to get info about how to use the script:: - - usage: calc_timeprop_charges.py -l ii:jj,ll:mm + usage: calc_timeprop_charges.py -l ii:jj,ll:mm - Reads output from TD calculation with external laser and produces net charges per fragment - (subtracting value at time = 0). + Reads output from TD calculation with external laser and produces net charges per fragment + (subtracting value at time = 0). - Needs qsvst.dat file present in working directory. + Needs qsvst.dat file present in working directory. - Options: - -h, --help show this help message and exit - -l AT_LIST, --list=AT_LIST - list of atom indices starting from 1 (initial and - final index separated by colons, ranges separated by - commas) + Options: + -h, --help show this help message and exit + -l AT_LIST, --list=AT_LIST + list of atom indices starting from 1 (initial and + final index separated by colons, ranges separated by + commas) - You will have to define the ranges of atoms that correspond to each of + You will have to define the ranges of atoms that correspond to each of the two molecules. In our case, the PDI derivative is between atom 1 and 52 and the carbazole derivative is between atom 53 and 83. Then, you may run:: - ./calc_timeprop_charges.py -l 1:52,53:83 + ./calc_timeprop_charges.py -l 1:52,53:83 After runing the script, two files may be generated: *charge_frag1.dat* and *charge_frag2.dat* with the corresponding charges of each defined fragment. If you plot it you will get something like in :numref:`fig_CT_AD`. - + .. _fig_CT_AD: .. figure:: ../_figures/elecdynamics/tutorial/charge-vs-time.png :width: 60% @@ -434,7 +424,8 @@ Laser dynamics on the donor-acceptor aggregate and charge transfer where it is clear that the PDI molecule act as an acceptor of electrons (net charge goes negative), while the carbazole is donating electrons (net charge goes positive). - If we follow the protocol from before, ploting the populations and searching + + If we follow the protocol from before, ploting the populations and searching for the orbitals involved in the transition, we should be able to get some insigths on the mechanism of the charge transfer (follow the steps in the previous sections). As it is shown in :numref:`fig_molpopul-CT`. @@ -447,11 +438,11 @@ Laser dynamics on the donor-acceptor aggregate and charge transfer (left)Populations vs time for pulse-driven dynamics. (right) Orbitals involved in the excitation during the dynamics. - + the orbitals involved in the excitation with the pulse are localized in the - PDI molecule, i.e. we can confirm that we are exciting the PDI molecule in - its own HOMO-LUMO transition (and not an HOMO-LUMO transition of the whole - system). Comparing with the previous figure of the charges dynamics, we can + PDI molecule, i.e. we can confirm that we are exciting the PDI molecule in + its own HOMO-LUMO transition (and not an HOMO-LUMO transition of the whole + system). Comparing with the previous figure of the charges dynamics, we can also see that the CT process start after a certain amount of electrons are excited in the PDI molecule (more or less 30 fs, the duration of the pulse used). So we could in principle divide the mechanism in two steps. The first @@ -461,7 +452,7 @@ Laser dynamics on the donor-acceptor aggregate and charge transfer We hope that this tutorial is helpful for those interested in get into the real-time TDDFTB method using ``DFTB+``. Of course, these are just the basics and there are many more possibilities in terms of calculating optical properties and photoinduced processes within this approach for a wide range of materials and system like *graphene nanoribbons*, *plasmonic nanoparticles*, *glod nanoclusters*, *semiconductor nanoparticles* and *organic solar cells*. As an inspiration, we give you some references of -recent works performed with this method in ``DFTB+``: +recent works performed with this method in ``DFTB+``: **Fano Resonance and Incoherent Interlayer Excitons in Molecular van der Waals Heterostructures.** Lien-Medrano, C. R., Bonafé, F. P., Yam, C. Y., Palma, C.-A., Sánchez, C. G., & Frauenheim, T. (2022). Nano Letters, 22(3), 911–917. `https://doi.org/10.1021/acs.nanolett.1c03441 `_ @@ -470,4 +461,3 @@ recent works performed with this method in ``DFTB+``: **Photoinduced charge-transfer in chromophore-labeled gold nanoclusters: quantum evidence of the critical role of ligands and vibronic couplings.** Domínguez-Castro, A., Lien-Medrano, C. R., Maghrebi, K., Messaoudi, S., Frauenheim, T., & Fihey, A. (2021). Nanoscale, 13(14), 6786–6797. `https://doi.org/10.1039/D1NR00213A `_ **Plasmon-driven sub-picosecond breathing of metal nanoparticles.** Bonafé, F. P., Aradi, B., Guan, M., Douglas-Gallardo, O. A., Lian, C., Meng, S., Frauenheim, T., & Sánchez, C. G. (2017). Nanoscale, 9(34), 12391–12397. `https://doi.org/10.1039/C7NR04536K `_ -