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Peer-reviewedCC BYThe journal of physical chemistry letters

Limits of Memory-Assisted Coherence in Cavity-Embedded Molecules.

  1. 1School of Chemistry, Pharmacy and Pharmacology, University of East Anglia, Norwich Research Park, NorwichNR4 7TJ, United Kingdom.
  2. 2Department of Physics and Astronomy and Thomas Young Centre, University College London, Gower Street, LondonWC1E 6BT, United Kingdom.
  3. 3School of Engineering, Mathematics and Physics, University of East Anglia, Norwich Research Park, NorwichNR4 7TJ, United Kingdom.

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.

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BibTeX
@article{kinslow2026limits,
  title = {{Limits of Memory-Assisted Coherence in Cavity-Embedded Molecules.}},
  author = {Joshua C Kinslow and Ben S Humphries and Dale Green and Magnus O Borgh and Garth A Jones},
  journal = {The journal of physical chemistry letters},
  year = {2026},
  month = oct,
  doi = {10.1021/acs.jpclett.6c02396},
  url = {https://europepmc.org/article/MED/42918228},
  note = {CC BY},
}
RIS
TY  - JOUR
TI  - Limits of Memory-Assisted Coherence in Cavity-Embedded Molecules.
AU  - Joshua C Kinslow
AU  - Ben S Humphries
AU  - Dale Green
AU  - Magnus O Borgh
AU  - Garth A Jones
PY  - 2026
DA  - 2026/10/01
JO  - The journal of physical chemistry letters
DO  - 10.1021/acs.jpclett.6c02396
UR  - https://europepmc.org/article/MED/42918228
AB  - 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.
SN  - 1948-7185
ER  -