Quantized Vibrational Relaxation from Stochastic Non-Markovian System-Bath Dynamics
In this contribution, we investigate the non-Markovian relaxation dynamics of a vibrating system in contact with a structured environment. Numerical simulations of the vibrational relaxation dynamics of an adsorbate coupled to a bath of phonons are performed using the stochastic multiconfiguration time-dependent Hartree method. Non-Markovian effects arise from the partitioning of the system-bath interaction into explicit and implicit contributions. It is shown that only a small number of explicit bath modes is sufficient to capture the short-time non-Markovian dynamics, and that imposing a "Markovian closure" of the weakly coupled explicit bath allows other physical regimes for the vibrational relaxation dynamics with distinctive signatures to be assessed.
Authors
- Roberto Marquardt (ORCID: https://orcid.org/0000-0002-2481-7117)
- Fabien Gatti (ORCID: https://orcid.org/0000-0002-5928-7427)
- Souvik Mandal (ORCID: https://orcid.org/0000-0003-0604-3135)
- Oussama Bindech (ORCID: https://orcid.org/0000-0002-5906-5779)
- Jean Christophe Tremblay (ORCID: https://orcid.org/0000-0001-8021-7063)
Institutions
- Centre National de la Recherche Scientifique (FR)
- Université de Bourgogne (FR)
- Université Paris-Saclay (FR)
- Institut des Sciences Moléculaires d'Orsay (FR)
- Laboratoire Interdisciplinaire Carnot de Bourgogne (FR)
- Laboratoire de Physique et Chimie Théoriques
- Université de Strasbourg (FR)
- Université de Lorraine (FR)
Publication Details
- Journal
- The Journal of Physical Chemistry B
- Published
- 2025-02-13
- DOI
- https://doi.org/10.1021/acs.jpcb.4c08189
- Primary Topic
- Spectroscopy and Quantum Chemical Studies
- Type
- article
- Field-Weighted Citation Impact
- 0.00
Funders
- Université de Lorraine
- Agence Nationale de la Recherche
- Université de Strasbourg
- Centre National de la Recherche Scientifique