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.
Verfasserangaben: | Eric W. FischerORCiDGND, Peter SaalfrankORCiDGND |
---|---|
DOI: | https://doi.org/10.1063/5.0064013 |
ISSN: | 0021-9606 |
ISSN: | 1089-7690 |
Pubmed ID: | https://pubmed.ncbi.nlm.nih.gov/34624972 |
Titel des übergeordneten Werks (Englisch): | The journal of chemical physics : bridges a gap between journals of physics and journals of chemistry |
Verlag: | American Institute of Physics |
Verlagsort: | Melville |
Publikationstyp: | Wissenschaftlicher Artikel |
Sprache: | Englisch |
Datum der Erstveröffentlichung: | 04.10.2021 |
Erscheinungsjahr: | 2021 |
Datum der Freischaltung: | 19.01.2023 |
Band: | 155 |
Ausgabe: | 13 |
Aufsatznummer: | 134109 |
Seitenanzahl: | 15 |
Fördernde Institution: | Deutsche Forschungsgemeinschaft (DFG) German Research Foundation (DFG) [Sa 547/9]; International Max Planck Research School for Elementary Processes in Physical Chemistry |
Organisationseinheiten: | Mathematisch-Naturwissenschaftliche Fakultät / Institut für Chemie |
DDC-Klassifikation: | 5 Naturwissenschaften und Mathematik / 53 Physik / 530 Physik |
5 Naturwissenschaften und Mathematik / 54 Chemie / 540 Chemie und zugeordnete Wissenschaften | |
Peer Review: | Referiert |
Lizenz (Deutsch): | CC-BY - Namensnennung 4.0 International |