cboamd: A Machine Learning Molecular Dynamics Framework for Vibrational Strong Coupling
Abstract
Under vibrational strong coupling (VSC), molecular vibrations hybridize with an optical cavity mode to form polaritons, offering a route to modify chemical and material properties without external driving. In this work, we develop a machine-learning interatomic potential (MLIP) based framework to study VSC inside optical cavities. By using the cavity Born-Oppenheimer approximation and treating the photonic degrees of freedom as an effective electric field, we provide a framework that can describe VSC solely based on the electronic ground-state potential energy surfaces (PES), electronic dipole moment, and polarizability, all quantities obtained outside the cavity. We train PES, polarization, and polarizability models to drive the molecular dynamics (MD) simulations of systems under VSC. We demonstrate the approach for both a single CO2 molecule and liquid CO2, showing that the polarizability renormalizes the effective cavity resonance: at fixed cavity frequency this renormalization renders the Rabi splitting strongly asymmetric, while with renormalized cavity frequency the symmetric splitting is capped by polarizability screening. The collective Rabi splitting of the liquid is connected quantitatively to the single-molecule splitting involving the √(N/3) orientational enhancement and the local-field enhanced effective charges of the coupled vibration, while the equilibrium pair structure of the CO2 liquid remains unchanged. These simulations are the first MLIP-driven simulations of collective VSC in the condensed phase and open further pathways to the exploration of chemical effects under VSC.
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BibTeX
@misc{li2026cboamd,
title = {{cboamd: A Machine Learning Molecular Dynamics Framework for Vibrational Strong Coupling}},
author = {Yifan Li and Roberto Car and Johannes Flick},
howpublished = {arXiv},
year = {2026},
month = sep,
doi = {10.48550/arxiv.2609.22022},
eprint = {2609.22022},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2609.22022},
}
RIS
TY - UNPB
TI - cboamd: A Machine Learning Molecular Dynamics Framework for Vibrational Strong Coupling
AU - Yifan Li
AU - Roberto Car
AU - Johannes Flick
PY - 2026
DA - 2026/09/18
PB - arXiv
DO - 10.48550/arxiv.2609.22022
UR - https://arxiv.org/abs/2609.22022
AB - Under vibrational strong coupling (VSC), molecular vibrations hybridize with an optical cavity mode to form polaritons, offering a route to modify chemical and material properties without external driving. In this work, we develop a machine-learning interatomic potential (MLIP) based framework to study VSC inside optical cavities. By using the cavity Born-Oppenheimer approximation and treating the photonic degrees of freedom as an effective electric field, we provide a framework that can describe VSC solely based on the electronic ground-state potential energy surfaces (PES), electronic dipole moment, and polarizability, all quantities obtained outside the cavity. We train PES, polarization, and polarizability models to drive the molecular dynamics (MD) simulations of systems under VSC. We demonstrate the approach for both a single CO_2 molecule and liquid CO_2, showing that the polarizability renormalizes the effective cavity resonance: at fixed cavity frequency this renormalization renders the Rabi splitting strongly asymmetric, while with renormalized cavity frequency the symmetric splitting is capped by polarizability screening. The collective Rabi splitting of the liquid is connected quantitatively to the single-molecule splitting involving the √(N/3) orientational enhancement and the local-field enhanced effective charges of the coupled vibration, while the equilibrium pair structure of the CO_2 liquid remains unchanged. These simulations are the first MLIP-driven simulations of collective VSC in the condensed phase and open further pathways to the exploration of chemical effects under VSC.
ER -