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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…
Resonant vibrational strong coupling (VSC) between molecular vibrations and quantized field modes of low-frequency optical cavities constitutes the conceptual cornerstone of vibro-polaritonic chemistry. In this work, we theoretically…
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…
Polariton chemistry may provide a new means to control molecular reactivity, permitting remote, reversible modification of reaction energetics, kinetics, and product yields. A considerable body of experimental and theoretical work has…
Polaritons have gained significant attention for the tantalizing possibility of modifying chemical properties and dynamics by coupling molecules to resonant cavity modes to create hybrid light-matter quantum states. Herein, we implement the…
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…
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…
Recent experiments have revealed the profound effect of strong light-matter interactions in optical cavities on the electronic ground state of molecular systems. This phenomenon, known as vibrational strong coupling (VSC), can modify…
Polaritonic chemistry offers the possibility of modifying molecular properties and even influencing chemical reactivity through strong coupling between vibrational transitions and confined light modes in optical cavities. Despite…
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…
Strong coupling (SC) is a fundamental concept in physics that describes extreme interactions between light and matter. Recent experiments have demonstrated SC at the nanometer scale, where strongly confined polaritons, rather than photons,…
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…
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…
The strong coupling of an IR-active molecular transition with an optical mode of the cavity results in vibrational polaritons, which opens a new way to control chemical reactivity via confined electromagnetic fields of the cavity. In this…
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…
For a small fraction of hot CO2 molecules immersed in a liquid-phase CO2 thermal bath, classical cavity molecular dynamics simulations show that forming collective vibrational strong coupling (VSC) between the C=O asymmetric stretch of CO2…
Vibrational strong coupling can modify chemical reaction pathways in unconventional ways. Thus far, Fabry-Perot cavities formed by pairs of facing mirrors have been mostly utilized to achieve vibrational strong coupling. In this study, we…
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…
We study theoretically the quantum dynamics and spectroscopy of rovibrational polaritons formed in a model system composed of a single rovibrating diatomic molecule, which interacts with two degenerate, orthogonally polarized modes of an…
Recent experiments suggest that vibrational strong coupling (VSC) may significantly modify ground-state chemical reactions and their rates even without external pumping. The intrinsic mechanism of this "vacuum-field catalysis" remains…