A thermofield-based multilayer multiconfigurational time-dependent Hartree approach to non-adiabatic quantum dynamics at finite temperature
- 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.
Author details: | Eric Wolfgang FischerORCiDGND, Peter SaalfrankORCiDGND |
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DOI: | https://doi.org/10.1063/5.0064013 |
ISSN: | 0021-9606 |
ISSN: | 1089-7690 |
Pubmed ID: | https://pubmed.ncbi.nlm.nih.gov/34624972 |
Title of parent work (English): | The journal of chemical physics : bridges a gap between journals of physics and journals of chemistry |
Publisher: | American Institute of Physics |
Place of publishing: | Melville |
Publication type: | Article |
Language: | English |
Date of first publication: | 2021/10/04 |
Publication year: | 2021 |
Release date: | 2023/01/19 |
Volume: | 155 |
Issue: | 13 |
Article number: | 134109 |
Number of pages: | 15 |
Funding institution: | Deutsche Forschungsgemeinschaft (DFG) German Research Foundation (DFG) [Sa 547/9]; International Max Planck Research School for Elementary Processes in Physical Chemistry |
Organizational units: | Mathematisch-Naturwissenschaftliche Fakultät / Institut für Chemie |
DDC classification: | 5 Naturwissenschaften und Mathematik / 53 Physik / 530 Physik |
5 Naturwissenschaften und Mathematik / 54 Chemie / 540 Chemie und zugeordnete Wissenschaften | |
Peer review: | Referiert |
License (German): | CC-BY - Namensnennung 4.0 International |