How to correct Ehrenfest nonadiabatic dynamics in open quantum systems: Ehrenfest plus random force (E + <i>σ</i>) dynamics
One key challenge in the study of nonadiabatic dynamics in open quantum systems is to balance computational efficiency and accuracy. Although Ehrenfest dynamics (ED) is computationally efficient and well-suited for large complex systems, ED often yields inaccurate results. To address these limitations, we improve the accuracy of the traditional ED by adding a random force (E + σ). In this work, the construction of random forces is considered in Markovian and non-Markovian scenarios, and we ensure the dynamics satisfy the detailed balance in both scenarios. By comparing our E + σ with existing methods such as the electronic friction model and surface hopping, we furthermore validate its reliability. In addition, the E + σ model still retains the high efficiency of ED and does not incur much additional computation. We believe that this method provides an alternative to accurately describe the mixed quantum-classical dynamics in open quantum systems, particularly for large complex systems.
Authors
- Wenjie Dou (ORCID: https://orcid.org/0000-0001-5410-6183)
- Jingqi Chen (ORCID: https://orcid.org/0000-0002-8046-2197)
- Joonho Lee (ORCID: https://orcid.org/0000-0002-9667-1081)
Institutions
- Harvard University (US)
- Westlake University (CN)
- Institute of Natural Science (KP)
Publication Details
- Journal
- The Journal of Chemical Physics
- Published
- 2025-01-23
- DOI
- https://doi.org/10.1063/5.0245114
- Citations
- 2
- Primary Topic
- Spectroscopy and Quantum Chemical Studies
- Type
- article
- Field-Weighted Citation Impact
- 2.49
Funders
- National Natural Science Foundation of China
- Natural Science Foundation of Zhejiang Province