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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…

The optical hybridization of the electronic states in strongly coupled molecule-cavity systems have revealed unique properties such as lasing, room temperature polariton condensation, and the modification of excited electronic landscapes…

Plasmon resonances at the surface of plasmonic antennas allow for extremely strong enhancement of Raman scattering. Intrinsic to plasmonics, however, is that extreme field confinement lacks precise spectral control, which would hold great…

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 consider the process of four-wave mixing in an array of gold nanowires strongly coupled to a gold film. Using full-wave simulations, we perform a quantitative comparison of the four-wave mixing efficiency associated with the thin film…

The interaction of organic molecules and molecular aggregates with electromagnetic fields that are strongly confined inside optical cavities within nanoscale volumes, has allowed the observation of exotic quantum regimes of light-matter…

Quantum Physics · Physics 2018-01-30 Felipe Herrera , Frank C. Spano

As pioneering experiments have shown, strong vibrational coupling between molecular vibrations and light modes in an optical cavity can significantly alter molecular properties and even affect chemical reactivity. However, the current…

Chemical Physics · Physics 2024-07-26 Thomas Schnappinger , Markus Kowalewski

Strongly coupled plasmon-exciton systems offer promising applications in nanooptics. The classification of the coupling regime is currently debated both from experimental and theoretical perspectives. We present a method to unambiguously…

Mesoscale and Nanoscale Physics · Physics 2023-07-19 Felix Stete , Wouter Koopman , Matias Bargheer

We derive the transition rates, dephasing rates, and Lamb shifts for a system consisting of many molecules collectively coupled to a resonant cavity mode. Using a variational polaron master equation, we show that strong vibrational…

Quantum Physics · Physics 2024-07-24 Dominic M Rouse , Erik M Gauger , Brendon W Lovett

Strong coupling between cavity photons and molecular vibrations can lead to the formation of vibron-polaritons. In a recent experiment with PVAc molecules in a metal-metal microcavity [A.Shalabney et al., Ang.Chem.Int.Ed. 54 7971 (2015)],…

Optics · Physics 2016-08-31 Artem Strashko , Jonathan Keeling

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 experiments have revealed the profound effect of strong light-matter interactions in optical cavities on the electronic ground state of molecular systems. This phenomenon, known as vibrational strong coupling (VSC), can modify…

Quantum Physics · Physics 2023-12-19 Thomas Schnappinger , Markus Kowalewski

We demonstrate that collective vibrational strong coupling of molecules in thermal equilibrium can give rise to significant local electronic polarizations in the thermodynamic limit. We do so by first showing that the full non-relativistic…

Molecular polaritons, hybrid light-matter states resulting from strong cavity coupling of optical transitions, may provide a new route to guide chemical reactions. However, demonstrations of cavity-modified reactivity in clean benchmark…

Chemical Physics · Physics 2024-08-20 Liying Chen , Ashley P. Fidler , Alexander M. McKillop , Marissa L. Weichman

Prospects of using metal hole arrays for the enhanced optical detection of molecular chirality in nanosize volumes are investigated. Light transmission through the holes filled with an optically active material is modeled and the activity…

Polaritons are compositional light-matter quasiparticles that arise as a result of strong coupling between a vacuum field of a resonant optical cavity and electronic excitations in quantum emitters. Reaching such a regime is often hard, as…

Recent experiments and theory demonstrate that the the ground state properties and chemical reactivity of molecules can be modified inside an optical cavity. The vibrational strong or ultrastrong coupling results in the formation of…

Chemical Physics · Physics 2022-12-01 Qi Yu

Polaritons are unique hybrid light-matter states that offer an alternative way to manipulate chemical processes and change material properties. In this work we theoretically demonstrate that singlet fission dynamics can be accelerated under…

Chemical Physics · Physics 2021-10-06 Clàudia Climent , David Casanova , Johannes Feist , Francisco J. García-Vidal

This review outlines several linear optical effects featured by molecular polaritons arising in the collective strong light-matter coupling regime. Under weak laser irradiation and when the single-molecule light-matter coupling can be…

By modifying the density of optical states at the location of an emitter, weak cavity-emitter coupling can enable a host of potential applications in quantum optics, from the development of low- threshold lasers to brighter single-photon…

Optics · Physics 2011-11-03 Kasey J. Russell , Tsung-Li Liu , Shanying Cui , Evelyn L. Hu