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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

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

This study investigates the dynamic behavior of polaritons in an optical cavity containing one million molecules, emphasizing the influence of molecular rotation and level disorder on the coupling between molecules and photons. Through…

Optics · Physics 2024-02-22 Wei Liu , Jingqi Chen , Wenjie Dou

Molecules constitute compact hybrid quantum optical systems that can interface photons, electronic degrees of freedom, localized mechanical vibrations and phonons. In particular, the strong vibronic interaction between electrons and nuclear…

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…

We present an approximate analytic expression for the photoluminescence spectral function of a model polariton system, which describes a quantum dot, with a finite number of fermionic levels, strongly interacting with the lowest photon mode…

Mesoscale and Nanoscale Physics · Physics 2013-05-29 Carlos Andres Vera , Herbert Vinck-Posada , Augusto Gonzalez

The paradigm of $N$ quantum emitters coupled to a single cavity mode appears in many situations ranging from quantum technologies to polaritonic chemistry. The ideal case of identical emitters is elegantly modeled in terms of symmetric…

Photons strongly coupled to material systems constitute a novel system for studying the dynamics of non-equilibrium quantum many-body systems. We give a fully analytical description of the dynamics of photons coupled to a one-dimensional…

Quantum Physics · Physics 2023-01-04 Björn Schrinski , Anders S. Sørensen

Two-dimensional infrared (2DIR) spectroscopy is widely used to study molecular dynamics but it is typically restricted to solid and liquid phase samples and modest spectral resolution. Only recently, its potential to study gas-phase…

Optics · Physics 2022-11-01 Grzegorz Kowzan , Thomas K. Allison

An ensemble of identical, intrinsically non-interacting molecules exposed to quantum light is discussed. Their interaction with the quantum light induces interactions between the molecules. The resulting hybrid light-matter states exhibit…

Chemical Physics · Physics 2024-06-19 Lorenz S. Cederbaum

Strong coupling of molecular vibrations to an infrared cavity mode affects their nature by creating dressed polariton states. We show how the single and double vibrational polariton manifolds may be controlled by varying the cavity coupling…

Quantum Physics · Physics 2016-05-10 Prasoon Saurabh , Shaul Mukamel

Quantum beats in nonlinear spectroscopy of molecular aggregates are often attributed to electronic phenomena of excitonic systems, while nuclear degrees of freedom are commonly included into models as overdamped oscillations of bath…

Chemical Physics · Physics 2012-11-27 Vytautas Butkus , Leonas Valkunas , Darius Abramavicius

Molecular polaritons are the optical excitations which emerge when molecular transitions interact strongly with confined electromagnetic fields. Increasing interest in the hybrid molecular-photonic materials that host these excitations…

Mesoscale and Nanoscale Physics · Physics 2018-02-26 Raphael F. Ribeiro , Luis A. Martínez-Martínez , Matthew Du , Jorge Campos-Gonzalez-Angulo , Joel Yuen-Zhou

Two-dimensional electronic spectroscopy provides information on coupling and energy transfer between excited states on ultrafast timescales. Only recently, incoherent fluorescence detection has made it possible to combine this method with…

Optics · Physics 2025-05-14 Sanchayeeta Jana , Simon Durst , Lucas Ludwig , Markus Lippitz

The large number of degrees of freedom involved in polaritonic chemistry processes considerably restricts the systems that can be described by any ab initio approach, due to the resulting high computational cost. Semiclassical methods that…

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…

Chemical Physics · Physics 2022-04-07 Tao E. Li , Abraham Nitzan , Joseph E. Subotnik

We studied the interaction of a two-level atom with a frequency modulated cavity mode in an ideal optical cavity. The system, described by a Jaynes-Cumming Hamiltonian, gave rise to a set of stiff nonlinear first order equations solved…

Quantum Physics · Physics 2013-01-22 U. Pishipati , I. Almakremi , Amitabh Joshi , Juan D. Serna

Femtosecond coherent multidimensional spectroscopy is demonstrated for an ultracold gas. For this, a setup for phase modulation spectroscopy is used to probe the $3^2\mathrm{S}_{1/2} - 2^2\mathrm{P}_{1/2, 3/2}$ transition in an 800…

Atomic Physics · Physics 2023-01-16 Friedemann Landmesser , Tobias Sixt , Katrin Dulitz , Lukas Bruder , Frank Stienkemeier

A general theory of electronic excitations in aggregates of molecules coupled to intramolecular vibrations and the harmonic environment is developed for simulation of the third-order nonlinear spectroscopy signals. The model is applied in…

Chemical Physics · Physics 2014-01-17 Vytautas Butkus , Leonas Valkunas , Darius Abramavicius

Polariton chemistry has been hailed as a potential new route to direct molecular processes with electromagnetic fields. To make further strides, it is essential for the community to clarify which unusual polaritonic phenomena are true…

Chemical Physics · Physics 2025-11-19 Alexander M. McKillop , Marissa L. Weichman