相关论文: Quantum mechanical deconstruction of vibrational e…
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…
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…
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…
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…
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…
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…
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…
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…
A computational study of liquid water when the system is coupled with a (model) Fabry-Perot cavity is reported. At this end, the Cavity Born-Oppenheimer Molecular Dynamics approach proposed recently (Li et al., Proc. Nat. Acad. Sci. USA,…
Strong coupling between molecular excitations and quantized electromagnetic fields in optical cavities provides a powerful means to control the physical and chemical properties of molecular systems. Here, we study electron transfer (ET)…
One of the most popular subjects now being researched in molecular science is strong light-matter coupling. The introduction of vibrational strong coupling and the formation vibro-polaritonic states tend to modify chemical reactivity,…
We assess the cavity molecular dynamics method for the calculation of vibrational polariton spectra, using liquid water as a specific example. We begin by disputing a recent suggestion that nuclear quantum effects may lead to a broadening…
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…
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…
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,…
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…
Vibrational coupling is relevant not only for dissipation of excess energy after chemical reactions but also for elucidating molecular structure and dynamics. It is particularly important for OH stretch vibrational spectra of water, for…
In this paper, we study the role of collective vibrational motion in the phenomenon of electronic energy transfer (EET) along a chain of coupled electronic dipoles with varying excitation frequencies. Previous experimental work on EET in…
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…
Based on quantum-mechanical path-integral molecular dynamics simulations the impact of nuclear quantum effects on the vibrational and hydrogen bond dynamics in liquid water is investigated. The instantaneous fluctuations in the frequencies…