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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…

量子物理 · 物理学 2023-03-29 Zhedong Zhang , Xiaoyu Nie , Dangyuan Lei , Shaul Mukame

Molecular polaritons are hybrid states of photonic and molecular character that form when molecules strongly interact with light. Strong coupling tunes energy levels and importantly, can modify molecular properties (e.g. photoreaction…

化学物理 · 物理学 2023-02-14 Francesca Fassioli , Kyu Hyung Park , Sarah E. Bard , Gregory D. Scholes

Hybrid lattice-light modes, known as phonon-polaritons, represent the backbone of advanced protocols based on THz pumping of infrared modes. Here we provide a theoretical framework able to capture the different roles played by…

材料科学 · 物理学 2025-05-02 Niccolò Sellati , Jacopo Fiore , Stefano Paolo Villani , Lara Benfatto , Mattia Udina

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…

介观与纳米尺度物理 · 物理学 2018-02-26 Raphael F. Ribeiro , Luis A. Martínez-Martínez , Matthew Du , Jorge Campos-Gonzalez-Angulo , Joel Yuen-Zhou

We have developed a non-Markovian theory of the polariton luminescence taking the molecular vibrations into account. The calculations were made in the polariton basis. We have shown that the frequency shift and the polariton spectral lines…

介观与纳米尺度物理 · 物理学 2022-04-19 B. D. Fainberg , V. Al. Osipov

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…

Forming new hybrid quasiparticles by strong light-matter coupling is a promising tool for tailoring photophysics and photochemistry of molecules. Thus, the ultrafast dynamics of polaritons formed upon strong light-matter coupling has been…

化学物理 · 物理学 2025-05-23 Luca Nils Philipp , Eva Münzel , Julian Lüttig , Roland Mitrić

We show how to simulate a model of many molecules with both strong coupling to many vibrational modes and collective coupling to a single photon mode. We do this by combining process tensor matrix product operator methods with a mean-field…

量子气体 · 物理学 2022-10-24 Piper Fowler-Wright , Brendon W. Lovett , Jonathan Keeling

We construct a model describing the response of a hybrid system where the electromagnetic field - in particular, surface plasmon polaritons - couples strongly with electronic excitations of atoms or molecules. Our approach is based on the…

量子物理 · 物理学 2020-01-01 K. S. U. Kansanen , A. Asikainen , J. J. Toppari , G. Groenhof , T. T. Heikkilä

This is a tutorial-style introduction to the field of molecular polaritons. We describe the basic physical principles and consequences of strong light-matter coupling common to molecular ensembles embedded in UV-visible or infrared…

化学物理 · 物理学 2020-03-18 Felipe Herrera , Jeffrey Owrutsky

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 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…

量子物理 · 物理学 2024-02-28 Q. Zhang , M. Asjad , M. Reitz , C. Sommer , B. Gurlek , C. Genes

Nonlinear spectroscopy is widely used to study the transient dynamics of molecules under strong light-matter coupling, though it remains unclear to what extent uncoupled intracavity molecules obscure signals from the strongly-coupled…

化学物理 · 物理学 2026-04-08 Alexander M. McKillop , Marissa L. Weichman

The influence of coherent optical nonlinearities on polariton propagation effects is studied within a theory-experiment comparison. A novel approach that combines a microscopic treatment of the boundary problem in a sample of finite…

其他凝聚态物理 · 物理学 2009-11-11 S. Schumacher , G. Czycholl , F. Jahnke , I. Kudyk , L. Wischmeier , I. Rückmann , T. Voss , J. Gutowski , A. Gust , D. Hommel

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…

化学物理 · 物理学 2025-11-19 Alexander M. McKillop , Marissa L. Weichman

Vibrational polaritons, hybrid light-matter states formed between molecular vibrations and infrared (IR) cavity modes, provide a novel approach for modifying chemical reaction pathways and energy transfer processes. For vibrational…

化学物理 · 物理学 2025-05-16 Xinwei Ji , Tao E. Li

Intramolecular energy transfer driven by near-field effects plays an important role in applications ranging from biophysics and chemistry to nano-optics and quantum communications. Advances in strong light-matter coupling in molecular…

介观与纳米尺度物理 · 物理学 2025-07-14 Kristin B. Arnardottir , Piper Fowler-Wright , Christos Tserkezis , Brendon W. Lovett , Jonathan Keeling

Nonlinear spectroscopy employs a series of laser pulses to interrogate dynamics in large interacting many-body systems, and has become a highly successful method for experiments in chemical physics. Current quantum optical experiments…

量子物理 · 物理学 2016-10-19 Frank Schlawin , Manuel Gessner , Shaul Mukamel , Andreas Buchleitner

We investigate the many-body states of exciton-polaritons that can be observed by pump-probe spectroscopy. Here, a weak-probe `spin-down' polariton is introduced into a coherent state of `spin-up' polaritons created by a strong pump. We…

量子气体 · 物理学 2020-01-01 Jesper Levinsen , Francesca Maria Marchetti , Jonathan Keeling , Meera M. Parish

We present a formalism to study molecular polaritons based on the bosonization of molecular vibronic states. This formalism accommodates an arbitrary number of molecules $N$, excitations and internal vibronic structures, making it ideal for…

量子物理 · 物理学 2025-03-18 Juan B. Pérez-Sánchez , Joel Yuen-Zhou
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