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We study the collective behavior of molecules placed in an infrared (IR) microcavity, incorporating the local fluctuations, i.e., dynamical disorder. The cooperative feature in vibrational polaritons is shown to be dynamically eroded, due…

Quantum Physics · Physics 2018-06-19 Zhedong Zhang , Kai Wang , Zhenhuan Yi , Shaul Mukamel , Marlan O. Scully

The vibrational dynamics of adsorbate molecules in single-molecule junctions depend critically on the geometric structure and electronic interactions between molecule and substrate. Vibrations, excited mechanochemically or by external…

Mesoscale and Nanoscale Physics · Physics 2025-09-17 Lukas Hörmann , Reinhard J. Maurer

Understanding how the effectiveness of natural photosynthetic energy harvesting systems arises from the interplay between quantum coherence and environmental noise represents a significant challenge for quantum theory. Recently it has begun…

Biological Physics · Physics 2015-06-16 E. K. Irish , R. Gómez-Bombarelli , B. W. Lovett

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 votage bias and mediated by a confined, enhanced vacuum…

Chemical Physics · Physics 2025-12-15 Yaling Ke

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

The multiphonon quantum dynamics in laser-pumped cavity optomechanical samples containing a vibrating mirror is investigated. Especially, we focus on dispersive interaction regimes where the externally applied coherent field frequency…

Quantum Physics · Physics 2022-03-09 Mihai A. Macovei , Adriana Pálffy

We employ an exact quantum mechanical simulation technique to investigate a model of cavity-modified chemical reactions in the condensed phase. The model contains the coupling of the reaction coordinate to a generic solvent, cavity coupling…

Quantum Physics · Physics 2023-07-03 Lachlan P. Lindoy , Arkajit Mandal , David R. Reichman

We present a microscopic theory for nonlinear optical spectroscopy of N molecules in an optical cavity. A quantum Langevin analytical expression is derived for the time- and frequency-resolved signals accounting for arbitrary numbers of…

Quantum Physics · Physics 2023-03-29 Zhedong Zhang , Xiaoyu Nie , Dangyuan Lei , Shaul Mukame

We analytically tackle opto-vibronic interactions in molecular systems driven by either classical or quantum light fields. In particular, we examine a simple model of molecules with two relevant electronic levels, characterized by potential…

Quantum Physics · Physics 2024-02-28 Q. Zhang , M. Asjad , M. Reitz , C. Sommer , B. Gurlek , C. Genes

In the regime of strong coupling between molecular excitons and confined optical modes, the intra-molecular degrees of freedom are profoundly affected, leading to a reduced vibrational dressing of polaritons compared to bare electronically…

Mesoscale and Nanoscale Physics · Physics 2018-10-17 Javier del Pino , Florian A. Y. N. Schröder , Alex W. Chin , Johannes Feist , Francisco J. Garcia-Vidal

Experimental and theoretical evidence point out to the crucial role of specific resonant intramolecular vibrational modes in the interpretation of long-lived coherences observed in two-dimensional spectra of some natural and synthetic light…

Chemical Physics · Physics 2020-07-15 Leonardo F. Calderón , Leonardo A. Pachón

Molecular vibrations and their dynamics are of outstanding importance for electronic and thermal transport in nanoscale devices as well as for molecular catalysis. The vibrational dynamics of <100 molecules are studied through three-colour…

We consider an optomechanical system comprising a single cavity mode and a dense spectrum of acoustic modes and solve for the quantum dynamics of initial cavity mode Fock (i.e., photon number) superposition states and thermal acoustic…

Quantum Physics · Physics 2021-12-16 Qidong Xu , M. P. Blencowe

Ultrafast spectroscopies constitute a fundamental tool to investigate the dynamics of non-equilibrium many-body states in correlated materials. Two-pulses (pump-probe) experiments have shed new light on the interplay between high-energy…

Strongly Correlated Electrons · Physics 2016-09-01 Claudio Giannetti

We study the dynamics of a quantum dot embedded in a three-dimensional microcavity in the strong coupling regime in which the quantum dot exciton has an energy close to the frequency of a confined cavity mode. Under the continuous pumping…

Mesoscale and Nanoscale Physics · Physics 2009-11-10 J. I. Perea , D. Porras , C. Tejedor

Coherent dynamics of coupled molecules are effectively characterized by the two-dimensional (2D) electronic coherent spectroscopy. Depending on the coupling between electronic and vibrational states, oscillating signals of purely…

Chemical Physics · Physics 2013-10-17 Vytautas Butkus , Donatas Zigmantas , Darius Abramavicius , Leonas Valkunas

From the high vibrational dipolar strength offered by molecular liquids, we demonstrate that a molecular vibration can be ultra-strongly coupled to multiple IR cavity modes, with Rabi splittings reaching $24\%$ of the vibration frequencies.…

We investigate exciton transport through one-dimensional molecular aggregates interacting strongly with a cavity mode. Unlike several prior theoretical studies treating the monomers as simple two-level systems, exciton-vibration coupling is…

Mesoscale and Nanoscale Physics · Physics 2019-03-14 Jingyu Liu , Qing Zhao , Ning Wu

Realizing nonlinear coupling across space can enable new scientific and technological advances, including ultrafast operation and propagation of information in IR photonic circuitry, remote triggering or catalyzing of chemical reactions,…

Optics · Physics 2019-12-13 Jiaxi Wang , Bo Xiang , Wei Xiong

Excited-state vibrational dynamics in molecules can be studied by an electronically off-resonant Raman process induced by a probe pulse with variable delay with respect to an actinic pulse. We establish the connection between several…

Chemical Physics · Physics 2013-09-27 Konstantin E. Dorfman , Benjamin P. Fingerhut , Shaul Mukamel