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The vacuum Rabi splitting (VRS) in molecular polaritons stands as a fundamental measure of collective light-matter coupling. Despite its significance, the impact of molecular disorder on VRS is not fully understood yet. This study delves…

Chemical Physics · Physics 2024-04-18 Kai Schwennicke , Noel C. Giebink , Joel Yuen-Zhou

Strong light-matter interactions between molecules and quantized electromagnetic fields inside an optical cavity open up novel possibilities, though inevitably influenced by disorder, an inherent attribute of realistic molecular systems.…

Chemical Physics · Physics 2025-05-29 Robert F. Catuto , Hsing-Ta Chen

We consider molecules confined to a microcavity whose dimensions are such that an excitation of the molecule is nearly resonant with a cavity mode. We investigate the situation where the excitation energies of the molecules are randomly…

Quantum Physics · Physics 2022-06-01 Tarun Gera , K. L. Sebastian

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.…

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

Vacuum Rabi splitting relies on symmetrical splitting of the common resonance frequency of atoms and the cavity in which the atoms reside. In this work, we argue that vacuum Rabi splitting is a manifestation of virtual light-matter two-mode…

Quantum Physics · Physics 2024-03-20 Karol Gietka

Vibronic coupling effects usually manifest themselves in molecules and crystals rather than in an unbound atoms. We theoretically demonstrate the existence of vibronic states in a moving two-level atom exposed to a strong electromagnetic…

Quantum Physics · Physics 2020-10-28 Andrei Ivanov , Evgeniy Perlin

The notion of strong light-matter coupling is typically associated with the observation of Rabi splitting, corresponding to the formation of the hybrid light-matter states known as polaritons. However, this relationship is derived based on…

Chemical Physics · Physics 2025-12-03 Wei-Kuo Li , Hsing-Ta Chen

The interplay between collective optical response and molecular static and dynamic disorder is studied using simple effective Hamiltonians for an ensemble of two-level emitters inside and outside a single-mode cavity. We model environmental…

Chemical Physics · Physics 2022-11-30 Zeyu Zhou , Hsing-Ta Chen , Joseph E. Subotnik , Abraham Nitzan

We have developed a femtosecond ultra-voilet (UV) stimulated Raman spectroscopy (UV-FSRS) for $N$ molecules in optical cavities. The scheme enables a real-time monitoring of collective dynamics of molecular polaritons and their coupling to…

Quantum Physics · Physics 2023-09-19 Jianhua Ren , Zhedong Zhang

The effect of disorder in the intensity of the driving laser on a coupled array of cavities described by a Bose-Hubbard Hamiltonian for dark-state polaritons is investigated. A canonically-transformed Gutzwiller wave function is used to…

Other Condensed Matter · Physics 2020-05-15 Abuenameh Aiyejina , Roger Andrews

Collective strong coupling between a disordered ensemble of $N$ localized molecular vibrations and a resonant optical cavity mode gives rise to 2 polariton and $N-1\gg2$ dark modes. Thus, experimental changes in thermally-activated reaction…

Quantum Physics · Physics 2022-03-14 Matthew Du , Joel Yuen-Zhou

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…

While the emerging field of vibrational polariton chemistry has the potential to overcome traditional limitations of synthetic chemistry, the underlying mechanism is not yet well understood. Here, we explore how the dynamics of unimolecular…

Chemical Physics · Physics 2021-11-16 Derek S Wang , Tomáš Neuman , Susanne F Yelin , Johannes Flick

Vibrational polaritons form in a planar Fabry-Perot microcavity when a vibrational mode of a layer of molecules is near resonant with an infrared cavity mode. Herein, dispersion relations of vibrational polaritons are studied when the…

Chemical Physics · Physics 2024-06-18 Tao E. Li

We report experimental measurements of the transmission spectrum of an optical cavity coupled with cold Rb atoms. We observe the multi-atom vacuum Rabi splitting of a composite cavity and atom system. When a coupling field is applied to the…

Optics · Physics 2009-11-13 Gessler Hernandez , Jiepeng Zhang , Yifu Zhu

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

Equation of state for systems with particles self-assembling into aggregates is derived within a mesoscopic theory combining density functional and field-theoretic approaches. We focus on the effect of mesoscopic fluctuations in the…

Statistical Mechanics · Physics 2012-07-13 Alina Ciach , Oksana Patsahan

The aim of this review is to show how ``ferromagnetic'' states, that is, states having a fully polarization, can produce intrinsic decoherence by unitary evolution. This effect can give an understanding of recent experiments on mesoscopic…

Mesoscale and Nanoscale Physics · Physics 2007-05-23 Marco Frasca

We study theoretically the quantum dynamics and spectroscopy of rovibrational polaritons formed in a model system composed of a single rovibrating diatomic molecule, which interacts with two degenerate, orthogonally polarized modes of an…

Chemical Physics · Physics 2023-01-11 Eric W. Fischer , Peter Saalfrank
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