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MO: Fachverband Molekülphysik
MO 15: MO Poster 3
MO 15.12: Poster
Mittwoch, 11. März 2020, 17:00–19:00, Empore Lichthof
A modified approach for simulating nonadiabatic dynamics via the generalized quantum master equation — Ellen Mulvihill1, •Alexander Schubert1,2,3, Xiang Sun4, Xing Gao1, Yudan Liu1, Barry D. Dunietz3, and Eitan Geva1 — 1University of Michigan, Ann Arbor, USA — 2Friedrich-Schiller Universität Jena, Germany — 3Kent State University, USA — 4New York University Shanghai, China
An approach for simulating nonadiabatic dynamics based on the Nakajima-Zwanzig generalized quantum master equation (GQME) is presented. Unlike the most common GQME-based approaches, the modified approach (M-GQME) does not require casting the overall Hamiltonian in a system-bath form, which is neither natural nor convenient in the case of the molecular Hamiltonian that governs the nonadiabatic dynamics. Within the M-GQME framework, the effect of the degrees of freedom of the environment on the time evolution of the reduced density operator is fully captured by a memory kernel superoperator. Two numerical implementations are presented, where the memory kernel is calculated either employing the Ehrenfest mean-field method [1] or via a combination of the mapping Hamiltonian (MH) approach and the linearized semi-classical (LSC) approximation [2]. Both approaches are demonstrated on a benchmark spin-boson model and shown to lead to significantly more accurate results than a direct application of the Ehrenfest method while being computationally more robust than other GQME-based approaches. [1] J.Chem.Phys.150, p.034101 (2019). [2] J.Chem.Phys.151, p.074103 (2019).