Related papers: Vibrational strong coupling in liquid water from c…
In this work, we combine the density functional tight-binding (DFTB) approach with a light-matter Hamiltonian beyond the long-wavelength approximation to propagate the dynamics of vibrational polaritons formed by coupling molecular…
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…
In this article, we show that the collective light-matter strong coupling regime, where $N$ molecular emitters couple to the photon mode of an optical cavity, can be mapped to a quantum impurity model where the photon is the impurity that…
We theoretically demonstrate that chemical reaction rate constant can be significantly suppressed by coupling molecular vibrations with an optical cavity, exhibiting both the collective coupling effect and the cavity-frequency modification…
In this thesis, we use classical, semi-classical and quantum-mechanical methods to simulate chemical reaction dynamics inside of an optical cavity. Within such a cavity, by selectively coupling vibrational modes of the reactants to the…
Strong coupling between molecular excitations and quantized electromagnetic fields in optical cavities provides a powerful means to control the physical and chemical properties of molecular systems. Here, we study electron transfer (ET)…
For a small fraction of hot CO2 molecules immersed in a liquid-phase CO2 thermal bath, classical cavity molecular dynamics simulations show that forming collective vibrational strong coupling (VSC) between the C=O asymmetric stretch of CO2…
In this work we investigate anharmonic vibrational polaritons formed due to strong light-matter interactions in an optical cavity between radiation modes and anharmonic vibrations beyond the long-wavelength limit. We introduce a…
Resonant coupling of a vibration to a cavity mode has been reported to dramatically modify spontaneous Raman scattering, but subsequent studies have produced conflicting results. In this Letter, we develop a microscopic quantum framework…
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…
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…
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…
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…
Developing theoretical frameworks for vibrational strong coupling (VSC) beyond the single-mode approximation is crucial for a comprehensive understanding of experiments with planar Fabry-P\'erot cavities. Herein, a generalized cavity…
The strong coupling of an IR-active molecular transition with an optical mode of the cavity results in vibrational polaritons, which opens a new way to control chemical reactivity via confined electromagnetic fields of the cavity. In this…
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…
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…
In this paper we develop quantum dynamical methods capable of treating the dynamics of chemically reacting systems in an optical cavity in the vibrationally strong-coupling (VSC) limit at finite temperatures and in the presence of a…
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…
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…