Multi-layer Gaussian-based multi-configuration time-dependent Hartree (ML-GMCTDH) simulations of ultrafast charge separation in a donor–acceptor complex

We report on first applications of the Multi-Layer Gaussian-based Multi-Configuration Time-Dependent Hartree (ML-GMCTDH) method [Römer et al., J. Chem. Phys. 138, 064106 (2013)] beyond its basic two-layer variant. The ML-GMCTDH scheme provides an embedding of a variationally evolving Gaussian wavepa...

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Bibliographic Details
Published in:The Journal of chemical physics 2021-04, Vol.154 (14), p.144106-144106
Main Authors: Di Maiolo, Francesco, Worth, Graham A., Burghardt, Irene
Format: Article
Language:English
Subjects:
Charge simulation
Charge transfer
Configurations
Coordination compounds
Coupling
First principles
Mathematical analysis
Multilayers
Tensors
Time dependence
Wave functions
Wave packets
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Summary:We report on first applications of the Multi-Layer Gaussian-based Multi-Configuration Time-Dependent Hartree (ML-GMCTDH) method [Römer et al., J. Chem. Phys. 138, 064106 (2013)] beyond its basic two-layer variant. The ML-GMCTDH scheme provides an embedding of a variationally evolving Gaussian wavepacket basis into a hierarchical tensor representation of the wavefunction. A first-principles parameterized model Hamiltonian for ultrafast non-adiabatic dynamics in an oligothiophene–fullerene charge transfer complex is employed, relying on a two-state linear vibronic coupling model that combines a distribution of tuning type modes with an intermolecular coordinate that also modulates the electronic coupling. Efficient ML-GMCTDH simulations are carried out for up to 300 vibrational modes using an implementation within the QUANTICS program. Excellent agreement with reference ML-MCTDH calculations is obtained.
ISSN:0021-9606
1089-7690
DOI:10.1063/5.0046933