Limits of Memory-Assisted Coherence in Cavity-Embedded Molecules

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.