QuantumPatch Excitonic Preprocessing

WaNo

The Excitonic Preprocessing WaNo is used to compute microscopic input for TTA, TPQ/SPQ rates as well as Fluorescent and Phosphorescent properties for Lightforge. Most options in this WaNo are identical but slimmed down in comparison to the QuantumPatch WaNo.

General Tab Engines Tab Shells Tab

Input files and parameters

General

Morphology: Here you can either provide a full morphology e.g. from Deposit or single molecule cml files (e.g. the molecule.pdb from the Parametrizer module converted into cml via babel). Note that also for morphologies as input, environmental effects will not be taken into account, i.e. the molecules on which the computations are performed are extracted from the morphology for vaccum calculations. For sake of computational time, we recommend to run the ExcitonicPreprocessor module on single optimized molecules as described above. If you have sufficient computational resources available, you can take into account the impact of different molecular configurations in the thin film by computing excitonics on multiple molecules of each type in the morphology. See below how to do this.

All excitonic preprocessing steps run independently and can be enabled using the "enabled" triggers in each section. For a full-stack KMC simulation, all boxes should be checked.

Import your morphology in the General Settings->Morphology field and seperately enable each analysis: Fluorescent, Phosphorescent, TTA and TPQ/SPQ. Unless you have specific requirements leave all other options at their default. Note especially that only the Dalton engine is able to compute the quadratic response including spin-orbit coupling required for Phosphorescence. The specification of roots should also not be changed unless it is explicitly required to reach convergence. In the TPQ/SPQ field, you can specify if TPQ and SPQ rate input should be computed for quenching between Excitons and anions, Excitons with cations, or both.

Engines

Setup the engine settings here. In a default computation, only Turbomole and Dalton have to be configured. Especially consider Functional and Basis for the Turbomole calculations. You can find a description of QM engines here.

Due to the increased computational time of the excited states calculation, consider to increase the number of threads of Dalton and its memory. Note that Dalton only works for up to 16 threads. As QuantumPatch (on which the Excitonic Preprocessor is based) requires 1 master thread on the first node, the required number of CPUs per Node (in the Resources Tab in SimStack) needs to be higher than the threads assigned in the Engines tab.

For TPQ/SPQ we recommend to use Turbomole wb97x with def2-SVP and use N-1 threads, where N is the number of cores you can allocate in the resources tab (e.g. allocate 32 cores and set number of threads to 31) along with respective memory (e.g. 64GB for 31threads/32 cores).

Shells

In the shells tab you can define which molecules the excited state calculations will be conducted upon. For a single molecule cml or a pristine morphology from Deposit you can simply use the "Number of Molecules" option here to specify on how many molecules the excitated state computations should be conducted. For mixed morphologies, you need to specify at least one molecule per type via their IDs in the morphology using the "list of Molecule IDs" option in the dropdown. Then specify the Molecule IDs in the text field, e.g. "molstate.0: 101;205;707-720" to compute excitonic properties on molecules with IDs 101, 205 and all molecules with the IDs ranging from 707 to 720. You can identify respective IDs either manually in the structure.cml, or via a vizalization tool, e.g. Jmol. Please note that the IDs start counting at index 0, while visualization tools may start counting at 1 (as is the case for e.g. Jmol).

Outputs

Outputs are found in Analysis/excitonic_preprocessing/xxxx_results.yml, where xxxx is an identifier, for the given molecule species. The data is grouped in subsections and described in the sample output below. M_0 .. M_i are molecules 0 to i of the given type. If more than 1 molecule per type is calculated differences in ouput are only due to conformational differences (no environment included). N_TPQ, N_TTA, N_T1 and N_S1 are the respective number of excitations. For phosphorescence (triplets, N_T1), TTA and TPQ this number can be specified as "roots" in the EPP-WaNo. For singlets, N_S1 is hard coded at N_S1=5.

TPQ_anion
    TPQ_acceptor_energies
        M_0 .. M_i:     N_TPQ excitation energies of the anion in eV 
    TPQ_acceptor_radiative_lifetime
        M_0 .. M_i:     N_TPQ radiative lifetimes of the anion in s   
    TPQ_acceptor_transition_dipole
        M_0 .. M_i:     N_TPQx3 transition dipoles of anion excitations in au
TPQ_kation
    TPQ_acceptor_energies
        M_0 .. M_i:     N_TPQ excitation energies of the kation in eV
    TPQ_acceptor_radiative_lifetime
        M_0 .. M_i:     N_TPQ radiative lifetimes of the kation in s  
    TPQ_acceptor_transition_dipole
        M_0 .. M_i:     N_TPQx3 transition dipoles of kation excitations in au
TTA_acceptor_energies
    M_0 .. M_i:     N_TTA excitation energies from T1 to T_N in eV
TTA_acceptor_radiative_lifetime
    M_0 .. M_i:     N_TTA radiative lifetimes of T_N to T1 transitions in s
TTA_acceptor_transition_dipole
    M_0 .. M_i:     N_TTAx3 transition dipoles of T1 to T_N excitations in au
singlet_energies
    M_0 .. M_i:     N_S1 excitation energies from S0 to S1 in eV
singlet_oscillator_strength
    M_0 .. M_i:     N_S1 oscillator strength from S1 to S0 
singlet_radiative_lifetime
    M_0 .. M_i:     N_S1 radiative lifetimes from S1 to S0 in s
singlet_transition_dipole
    M_0 .. M_i:     N_S1x3 transition dipoles for S0 to S1 excitations in au
triplet_energies
    M_0 .. M_i:     N_T1 excitation energies from S0 to T1 in eV
triplet_oscillator_strength
    M_0 .. M_i:     N_T1 oscillator strength from T1 to S0 
triplet_radiative_lifetime
    M_0 .. M_i:     N_T1 radiative lifetimes from T1 to S0 in s
triplet_transition_dipole
    M_0 .. M_i:     N_T1x3x3 transition dipoles for S0 to T1_1,2,3 excitations in au

 

 

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