Limits of Memory-Assisted Coherence in Cavity-Embedded Molecules

Jones, Garth, Green, Dale ORCID: https://orcid.org/0000-0002-2549-0486, Kinslow, Joshua, Borgh, Magnus O. ORCID: https://orcid.org/0000-0003-4243-7051 and Humphries, Ben (2026) Limits of Memory-Assisted Coherence in Cavity-Embedded Molecules. The Journal of Physical Chemistry Letters, 17 (41). pp. 11723-11730. ISSN 1948-7185

[thumbnail of acs.jpclett.6c02396]
Preview
PDF (acs.jpclett.6c02396) - Published Version
Available under License Creative Commons Attribution.

Download (2MB) | Preview

Abstract

Strong light–matter coupling in optical cavities is being widely explored as a strategy for modifying molecular dynamics and enhancing coherence. At the same time, structured vibrational environments can exhibit non-Markovian memory that promotes information backflow and coherence revival. We investigate the competition between these effects in a vibronic molecular system strongly coupled to a lossy optical cavity. Using hierarchical equations of motion to treat structured vibrational baths, we quantify both system coherence and non-Markovianity via the l1 norm of coherence and the Breuer–Laine–Piilo measure, respectively. We find that cavity coupling enhances coherence in overdamped environments but can suppress memory-assisted coherence in resonant underdamped regimes, even in the absence of significant photon loss. This suppression arises from hybridization-induced modification of system–bath information flow. We demonstrate that cavity coupling does not universally protect coherence but establishes limits governed by the competition between vibrational recurrence time scales and polaritonic hybridization.

Item Type: Article
Uncontrolled Keywords: molecular dynamics, hybridization, cavities, quantum mechanics, polaritons,das to be completed ,/dt/atira/pure/keyword/DAStatement/das_to_be_completed
Faculty \ School: Faculty of Science > School of Chemistry, Pharmacy and Pharmacology
Faculty of Science > School of Engineering, Mathematics and Physics
Faculty of Science
UEA Research Groups: Faculty of Science > Research Groups > Physical Chemistry and Pharmaceutics
Faculty of Science > Research Groups > Quantum Matter
Depositing User: LivePure Connector
Date Deposited: 26 Oct 2026 17:01
Last Modified: 26 Oct 2026 17:01
URI: https://ueaeprints.uea.ac.uk/id/eprint/104853
DOI: 10.1021/acs.jpclett.6c02396

Downloads

Downloads per month over past year

Actions (login required)

View Item View Item