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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

Optical microcavities and metallic nanostructures have been shown to significantly modulate the dynamics and spectroscopic response of molecular systems. We present a study of the nonlinear optics of a model consisting of $N$ anharmonic…

Polaritons, mixed light-matter quasiparticles, undergo a transition to a condensed, macroscopically coherent state at low temperatures or high densities. Recent experiments show that coupling light to organic molecules inside a microcavity…

Quantum Gases · Physics 2014-03-06 Justyna A. Cwik , Sahinur Reja , Peter B. Littlewood , Jonathan Keeling

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

When the interaction between a molecular system and confined light modes in an optical or plasmonic cavity is strong enough to overcome the dissipative process, hybrid light-matter states (polaritons) become the fundamental excitations in…

Mesoscale and Nanoscale Physics · Physics 2020-01-08 Yu Zhang , Tammie Nelson , Sergei Tretiak

Nonadiabatic phenomena are investigated in the rovibrational motion of molecules confined in an infrared cavity. Conical intersections (CIs) between vibrational polaritons, similar to CIs between electronic polaritonic surfaces, are found.…

Quantum Physics · Physics 2021-02-24 Tamás Szidarovszky , Péter Badankó , Gábor J. Halász , Ágnes Vibók

A model designed to mimic the implications of the collective optical response of molecular ensembles in optical cavities on molecular vibronic dynamics is investigated. Strong molecule-radiation field coupling is often reached when a large…

Chemical Physics · Physics 2022-10-05 Bingyu Cui , Abraham Nitzan

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

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,…

Linear spectra of molecular polaritons formed by $N$ molecules coupled to a microcavity photon mode are usually well described by classical linear optics, raising the question of where the expected nonlinear effects in these strongly…

Quantum Physics · Physics 2024-11-19 Arghadip Koner , Joel Yuen-Zhou

A theoretical framework is presented for the computation of rovibrational polaritonic states of a molecule in a lossless infrared (IR) microcavity. In the proposed approach the quantum treatment of the rotational and vibrational motion of…

Chemical Physics · Physics 2023-10-30 Tamás Szidarovszky

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

There is growing interest in using strongly coupled organic microcavities to tune molecular dynamics, including the electronic and vibrational properties of molecules. However, very little attention has been paid to the utility of cavity…

Materials Science · Physics 2024-06-12 Bin Liu , Vinod M. Menon , Matthew Y. Sfeir

Organic microcavities can be engineered to reach exotic quantum regimes of strong and ultrastrong light-matter coupling. However, the microscopic interpretation of their spectroscopic signals can be challenging due to the competition…

Quantum Physics · Physics 2017-06-07 Felipe Herrera , Frank C. Spano

Optical nonlinearities - how light-matter interactions are influenced by previous interactions with photons, are key resources in the contemporary photonics toolbox, relevant to quantum gate operations and all-optical switches. Optical…

We consider an ensemble of homonuclear diatomic molecules coupled to the two polarization directions of a Fabry-P\'erot cavity via fully quantum simulations. Accompanied by analytical results, we identify a coupling mechanism mediated…

Chemical Physics · Physics 2024-01-22 Niclas Krupp , Oriol Vendrell

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

Molecular polaritons arise from electronic or vibrational strong coupling (ESC and VSC) with confined electromagnetic fields. While these have been widely studied, the influence of electron-nuclear dynamics in driven cavities remains…

Recent experiments in polariton chemistry have demonstrated that reaction rates can be modified by vibrational strong coupling to an optical cavity mode. Importantly, this modification only occurs when the frequency of the cavity mode is…

Chemical Physics · Physics 2023-05-15 Marit R. Fiechter , Johan E. Runeson , Joseph E. Lawrence , Jeremy O. Richardson

Conventional approaches to probing ultrafast molecular dynamics rely on the use of synchronized laser pulses with a well-defined time delay. Typically, a pump pulse excites a wavepacket in the molecule. A subsequent probe pulse can then…

Mesoscale and Nanoscale Physics · Physics 2020-03-27 R. E. F. Silva , Javier del Pino , Francisco J. García-Vidal , Johannes Feist