Vibrational energy pooling driven by collective light–matter coupling
Abstract
Concentrating vibrational energy from multiple molecules onto selected members of an ensemble is central to mode-selective chemistry and molecular energy transport. Yet established mechanisms of vibrational energy pooling (VEP) rely on molecular collisions or strong intermolecular interactions. Here we demonstrate that collective vibrational strong coupling (VSC) provides a distinct route to VEP, with the optical cavity serving as an energetic intermediary. State-resolved cavity quasi-classical trajectory simulations of bend-excited water molecules reveal that the cavity transiently stores and redistributes vibrational energy among spatially separated, noninteracting molecules, producing bend overtones and higher excited states that are absent under otherwise identical free-space conditions. The cavity-mediated energy pooling persists in ensembles containing up to 10,000 molecules, while the pooling yields vary nonmonotonically with both collective coupling strength and cavity detuning. These results show how delocalized vibrational polariton promotes mode-specific vibrational energy localization and identify collective coupling and spectral resonance as joint control parameters for nonequilibrium molecular energy flow.
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BibTeX
@misc{yu2026vibrational,
title = {{Vibrational energy pooling driven by collective light–matter coupling}},
author = {Qi Yu and Dong H. Zhang and Joel M. Bowman},
howpublished = {ChemRxiv},
year = {2026},
month = sep,
doi = {10.26434/chemrxiv.15008293/v1},
url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15008293/v1},
note = {CC BY},
}
RIS
TY - UNPB
TI - Vibrational energy pooling driven by collective light–matter coupling
AU - Qi Yu
AU - Dong H. Zhang
AU - Joel M. Bowman
PY - 2026
DA - 2026/09/04
PB - ChemRxiv
DO - 10.26434/chemrxiv.15008293/v1
UR - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15008293/v1
AB - Concentrating vibrational energy from multiple molecules onto selected members of an ensemble is central to mode-selective chemistry and molecular energy transport. Yet established mechanisms of vibrational energy pooling (VEP) rely on molecular collisions or strong intermolecular interactions. Here we demonstrate that collective vibrational strong coupling (VSC) provides a distinct route to VEP, with the optical cavity serving as an energetic intermediary. State-resolved cavity quasi-classical trajectory simulations of bend-excited water molecules reveal that the cavity transiently stores and redistributes vibrational energy among spatially separated, noninteracting molecules, producing bend overtones and higher excited states that are absent under otherwise identical free-space conditions. The cavity-mediated energy pooling persists in ensembles containing up to 10,000 molecules, while the pooling yields vary nonmonotonically with both collective coupling strength and cavity detuning. These results show how delocalized vibrational polariton promotes mode-specific vibrational energy localization and identify collective coupling and spectral resonance as joint control parameters for nonequilibrium molecular energy flow.
ER -