Probing voltage-induced chemical reactions and anharmonicity with a confined vacuum light field

In this work, we present a proof-of-concept investigation of non-equilibrium chemical reaction dynamics at a molecule-electrode interface, driven out of equilibrium by an applied voltage bias and mediated by a confined, enhanced vacuum electromagnetic field inside an optical cavity. The coupled electron-vibration-photon system, together with the electrodes and a dissipative environment, is described within an open quantum system framework and solved using a numerically exact quantum dynamical approach. The reaction coordinate is modeled using a Morse potential, enabling explicit treatment of molecular anharmonicity and bond-breaking behavior. By varying the cavity frequency across the infrared regime to cover typical nuclear vibrational energies, we observe multiple resonant rate suppression features that emerge whenever the cavity mode is brought into resonance with a dipole-allowed vibrational transition along the anharmonic ladder up to the dissociation threshold. These findings open the door to extending polaritonic chemistry into genuinely non-equilibrium scenarios relevant to molecule-electrode interfaces. Moreover, building on these results, we further propose a multi-mode vibrational strong coupling strategy in which several cavity modes are individually matched to distinct vibrational transitions. This engineered multi-resonant cavity induces a stepwise vibrational ladder descending process that efficiently drains vibrational excited energy. The resulting cavity-assisted cooling suggests a potential route toward mitigating voltage-induced bond rupture and the long-standing instability issues of molecular junctions operating under high bias.

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Publication Details

Journal
The Journal of Chemical Physics
Published
2026-04-16
DOI
https://doi.org/10.1063/5.0324681
Primary Topic
Strong Light-Matter Interactions
Type
article
Field-Weighted Citation Impact
0.00

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article

Probing voltage-induced chemical reactions and anharmonicity with a confined vacuum light field

Yaling Ke
The Journal of Chemical Physics
Strong Light-Matter Interactions
article

Probing voltage-induced chemical reactions and anharmonicity with a confined vacuum light field

Yaling Ke
article en

Abstract

In this work, we present a proof-of-concept investigation of non-equilibrium chemical reaction dynamics at a molecule-electrode interface, driven out of equilibrium by an applied voltage bias and mediated by a confined, enhanced vacuum electromagnetic field inside an optical cavity. The coupled electron-vibration-photon system, together with the electrodes and a dissipative environment, is described within an open quantum system framework and solved using a numerically exact quantum dynamical approach. The reaction coordinate is modeled using a Morse potential, enabling explicit treatment of molecular anharmonicity and bond-breaking behavior. By varying the cavity frequency across the infrared regime to cover typical nuclear vibrational energies, we observe multiple resonant rate suppression features that emerge whenever the cavity mode is brought into resonance with a dipole-allowed vibrational transition along the anharmonic ladder up to the dissociation threshold. These findings open the door to extending polaritonic chemistry into genuinely non-equilibrium scenarios relevant to molecule-electrode interfaces. Moreover, building on these results, we further propose a multi-mode vibrational strong coupling strategy in which several cavity modes are individually matched to distinct vibrational transitions. This engineered multi-resonant cavity induces a stepwise vibrational ladder descending process that efficiently drains vibrational excited energy. The resulting cavity-assisted cooling suggests a potential route toward mitigating voltage-induced bond rupture and the long-standing instability issues of molecular junctions operating under high bias.

The Journal of Chemical PhysicsVol. 164(15)
ETH Zurich (CH)
Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung
Affordable and clean energy
Openalex Percentile: Top 11%
Strong Light-Matter Interactions
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