2022/03/06 by Tao E. Li, Abraham Nitzan, Li, Tao E. +5 · 2 citations
Physics and Astronomy · #Chemical Physics (physics.chem-ph) #FOS: Physical sciences #Mechanical and Optical Resonators #Mesoscale and Nanoscale Physics (cond-mat.mes-hall) #Spectroscopy and Quantum Chemical Studies #Strong Light-Matter Interactions
paper · pdf · doi:10.48550/arxiv.2203.03001
openalex publication_date 2022/03/06 · openalex created_date 2025/10/10 · openalex updated_date 2026/08/01
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 lossless cavity mode, the simulation shows that, as compared with a fully classical calculation, the inclusion of nuclear and photonic quantum effects does not lead to a change in the Rabi splitting but does broaden polaritonic linewidths roughly by a factor of two. Moreover, under thermal equilibrium, both quantum and classical simulations predict that the static dielectric constant of liquid water is largely unchanged inside versus outside the cavity. This result disagrees with a recent experiment demonstrating that the static dielectric constant of liquid water can be resonantly enhanced under VSC, suggesting either limitations of our approach or perhaps other experimental factors that have not yet been explored.