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Recent advances in polaritonic chemistry suggest that chemical reactions can be controlled via collective vibrational strong coupling (VSC) in a cavity. In this fully analytical work, we demonstrate that the collective vibrations of a…

Quantum Physics · Physics 2025-04-15 Vasil Rokaj , Ilia Tutunnikov , H. R. Sadeghpour

Under vibrational strong coupling (VSC), the formation of molecular polaritons may significantly modify the photo-induced or thermal properties of molecules. In an effort to understand these intriguing modifications, both experimental and…

Chemical Physics · Physics 2022-04-07 Tao E. Li , Abraham Nitzan , Joseph E. Subotnik

Vibrational strong coupling (VSC) provides a novel means to modify chemical reactions and energy transfer pathways. To efficiently model chemical dynamics under VSC in the collective regime, herein a hybrid quantum mechanical/molecular…

Chemical Physics · Physics 2022-12-29 Tao E. Li , Sharon Hammes-Schiffer

Recent experiments have demonstrated that vibrational strong coupling (VSC) between molecular vibrations and the optical cavity field can modify vibrational energy transfer (VET) processes in molecular systems. However, the underlying…

Chemical Physics · Physics 2024-11-25 Qi Yu , Dong H. Zhang , Joel M. Bowman

In vibrational strong coupling (VSC), molecular vibrations strongly interact with the modes of an optical cavity to form hybrid light-matter states known as vibrational polaritons. Experiments show that the kinetics of thermally activated…

Quantum Physics · Physics 2021-05-04 Matthew Du , Jorge A. Campos-Gonzalez-Angulo , Joel Yuen-Zhou

We present a microscopic theory that aims to explain the vibrational strong coupling (VSC) modified reaction rate constant. The analytic theory is based on a mechanistic conjecture that cavity modes promote the transition from the ground…

Quantum Physics · Physics 2023-05-16 Wenxiang Ying , Michael A. D. Taylor , Pengfei Huo

In the regime of ensemble vibrational strong coupling (VSC), a macroscopic number $N$ of molecular transitions couple to each resonant cavity mode, yielding two hybrid light-matter (polariton) modes, and a reservoir of $N-1$ dark states…

Chemical Physics · Physics 2020-04-03 Jorge Campos-Gonzalez-Angulo , Raphael F. Ribeiro , Joel Yuen-Zhou

We theoretically demonstrate that chemical reaction rate constant can be significantly suppressed by coupling molecular vibrations with an optical cavity, exhibiting both the collective coupling effect and the cavity-frequency modification…

Chemical Physics · Physics 2022-01-26 Arkajit Mandal , Xinyang Li , Pengfei Huo

In this paper we develop quantum dynamical methods capable of treating the dynamics of chemically reacting systems in an optical cavity in the vibrationally strong-coupling (VSC) limit at finite temperatures and in the presence of a…

Quantum Physics · Physics 2025-02-11 Lachlan P. Lindoy , Arkajit Mandal , David R. Reichman

Understanding the mechanism of chemical reaction rate modulation by vibrational strong coupling (VSC) has been the focus of several recent studies. However, a definitive explanation for the mode-specificity of VSC still eludes us. In this…

Chemical Physics · Physics 2026-03-11 Subhadip Mondal , Atul Kumar , Srihari Keshavamurthy

Recent experiments have observed that the chemical and photophysical properties of molecules can be modified inside an optical Fabry-Perot microcavity under collective vibrational strong coupling (VSC) conditions, and such modification is…

Mesoscale and Nanoscale Physics · Physics 2021-03-09 Tao E. Li , Abraham Nitzan , Joseph E. Subotnik

We simulate vibrational strong (VSC) and ultrastrong coupling (V-USC) for liquid water with classical molecular dynamics simulations. When the cavity modes are resonantly coupled to the O-H stretch mode of liquid water, the infrared…

Chemical Physics · Physics 2020-07-21 Tao E. Li , Joseph E. Subotnik , Abraham Nitzan

Interaction between light and molecular vibrations leads to hybrid light-matter states called vibrational polaritons. Even though many intriguing phenomena have been predicted for single-molecule vibrational strong coupling (VSC), several…

Molecular polaritons, hybrid light-matter states resulting from strong cavity coupling of optical transitions, may provide a new route to guide chemical reactions. However, demonstrations of cavity-modified reactivity in clean benchmark…

Chemical Physics · Physics 2024-08-20 Liying Chen , Ashley P. Fidler , Alexander M. McKillop , Marissa L. Weichman

When molecular transitions strongly couple to photon modes, they form hybrid light-matter modes called polaritons. Collective vibrational strong coupling is a promising avenue for control of chemistry, but this can be deterred by the large…

Developing theoretical frameworks for vibrational strong coupling (VSC) beyond the single-mode approximation is crucial for a comprehensive understanding of experiments with planar Fabry-P\'erot cavities. Herein, a generalized cavity…

Chemical Physics · Physics 2024-06-18 Tao E. Li

Polaritons - hybrid light-matter states formed from the strong coupling of a bright molecular transition with a confined photonic mode - may offer new opportunities for optical control of molecular behavior. Vibrational strong coupling…

Chemical Physics · Physics 2025-11-19 Liying Chen , Alexander M. McKillop , Ashley P. Fidler , Marissa L. Weichman

The electromagnetic field in an optical cavity can dramatically modify and even control chemical reactivity via vibrational strong coupling (VSC). Since the typical vibration and cavity frequencies are considerably higher than thermal…

Quantum Physics · Physics 2021-09-29 Peiyun Yang , Jianshu Cao

Recent experiments of chemical reactions in optical cavities have shown great promise to alter and steer chemical reactions but still remain poorly understood theoretically. In particular the origin of resonant effects between the cavity…

Chemical Physics · Physics 2022-12-21 Derek S. Wang , Johannes Flick , Susanne F. Yelin

A quantum simulation of vibrational strong coupling (VSC) in the collective regime via thermostatted ring-polymer molecular dynamics (TRPMD) is reported. For a collection of liquid-phase water molecules resonantly coupled to a single…

Chemical Physics · Physics 2022-03-08 Tao E. Li , Abraham Nitzan , Sharon Hammes-Schiffer , Joseph E. Subotnik
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