TY  - JOUR
A1  - Fischer, Eric W.
A1  - Saalfrank, Peter
T1  - A thermofield-based multilayer multiconfigurational time-dependent Hartree approach to non-adiabatic quantum dynamics at finite temperature
T2  - The journal of chemical physics : bridges a gap between journals of physics and journals of chemistry
N2  - We introduce a thermofield-based formulation of the multilayer multiconfigurational time-dependent Hartree (MCTDH) method to study finite temperature effects on non-adiabatic quantum dynamics from a non-stochastic, wave function perspective. Our approach is based on the formal equivalence of bosonic many-body theory at zero temperature with a doubled number of degrees of freedom and the thermal quasi-particle representation of bosonic thermofield dynamics (TFD). This equivalence allows for a transfer of bosonic many-body MCTDH as introduced by Wang and Thoss to the finite temperature framework of thermal quasi-particle TFD. As an application, we study temperature effects on the ultrafast internal conversion dynamics in pyrazine. We show that finite temperature effects can be efficiently accounted for in the construction of multilayer expansions of thermofield states in the framework presented herein. Furthermore, we find our results to agree well with existing studies on the pyrazine model based on the pMCTDH method.
Y1  - 2021
UR  - https://publishup.uni-potsdam.de/frontdoor/index/index/docId/57592
SN  - 0021-9606
SN  - 1089-7690
VL  - 155
IS  - 13
PB  - American Institute of Physics
CY  - Melville
ER  -