English
 
Help Privacy Policy Disclaimer
  Advanced SearchBrowse

Item

ITEM ACTIONSEXPORT

Released

Journal Article

Benchmarking Quasiclassical Mapping Hamiltonian Methods for Simulating Cavity-Modified Molecular Dynamics

MPS-Authors
/persons/resource/persons196584

Kelly,  A.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Department of Chemistry, Dalhousie University;

External Resource
Fulltext (public)
There are no public fulltexts stored in PuRe
Supplementary Material (public)
There is no public supplementary material available
Citation

Saller, M. A. C., Kelly, A., & Geva, E. (2021). Benchmarking Quasiclassical Mapping Hamiltonian Methods for Simulating Cavity-Modified Molecular Dynamics. The Journal of Physical Chemistry Letters, 12(12), 3163-3170. doi:10.1021/acs.jpclett.1c00158.


Cite as: http://hdl.handle.net/21.11116/0000-0008-6B69-B
Abstract
Recent experimental realizations of strong coupling between optical cavity modes and molecular matter placed inside the cavity have opened exciting new routes for controlling chemical processes. Simulating the cavity-modified dynamics of complex chemical systems calls for the development of accurate, flexible, and cost-effective approximate numerical methods that scale favorably with system size and complexity. In this Letter, we test the ability of quasiclassical mapping Hamiltonian methods to serve this purpose. We simulated the spontaneous emission dynamics of an atom confined to a microcavity via five different variations of the linearized semiclassical (LSC) method. Our main finding is that recently proposed LSC-based methods which use a modified form of the identity operator are reasonably accurate and perform significantly better than the Ehrenfest and standard LSC methods, without significantly increasing computational costs. These methods are therefore highly promising as a general purpose tool for simulating cavity-modified dynamics of complex chemical systems.