Gaussian-based multiconfiguration time-dependent Hartree: A two-layer approach. III. Application to nonadiabatic dynamics in a charge transfer complex

In this paper, we report on first applications of the Two-Layer Gaussian-based Multi-Configuration Time-Dependent Hartree (2L-GMCTDH) method to nonadiabatic dynamics. Simulations of ultrafast, coherent charge transfer dynamics are performed for a two-state linear vibronic coupling model describing an oligothiophene-fullerene charge transfer complex, for system dimensions ranging from 20 to 100 modes. Different variants of the state-dependent 2L-GMCTDH propagation are assessed, notably single-set and multi-set versions, along with a third hybrid variant. It is shown that the method is suitable to perform accurate and efficient nonadiabatic dynamics simulations in many dimensions.