相关论文: Cavity-Born Oppenheimer Approximation for Molecule…
Recent years have seen significant developments in the study of strong light-matter coupling including the control of chemical reactions by altering the vibrational normal modes of molecules. In the vibrational strong coupling regime the…
Chemical and photochemical reactivity, as well as supramolecular organization and several other molecular properties, can be modified by strong interactions between light and matter. Theoretical studies of these phenomena require the…
Experiments have demonstrated that vibrational strong coupling between molecular vibrations and light modes can significantly change molecular properties, such as ground-state reactivity. Theoretical studies towards the origin of this…
In this work, we illustrate the recently introduced concept of the cavity Born-Oppenheimer approximation for correlated electron-nuclear-photon problems in detail. We demonstrate how an expansion in terms of conditional electronic and…
In the vibrational strong coupling (VSC) regime, molecular vibrations and resonant low-frequency cavity modes form light-matter hybrid states, named vibrational polaritons, with characteristic IR spectroscopic signatures. Here, we introduce…
The coupling of a molecule and a cavity induces non-adiabaticity in the molecule which makes the description of its dynamics complicated. For polyatomic molecules, reduced-dimensional models and the use of the Born-Oppenheimer approximation…
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…
Resonant vibrational strong coupling (VSC) between molecular vibrations and quantized field modes of low-frequency optical cavities constitutes the conceptual cornerstone of vibro-polaritonic chemistry. In this work, we theoretically…
Vibrational polaritons are formed by strong coupling of molecular vibrations and photon modes in an optical cavity. Experiments have demonstrated that vibrational strong coupling can change molecular properties and even affect chemical…
We introduce a theoretical framework that allows for the systematic and efficient description of the ultrafast nonlinear response of molecular polaritons, i.e., hybrid light-matter states, in the collective regime of large numbers of…
We introduce a simple scheme to efficiently compute photon exchange-correlation contributions due to the coupling to transversal photons as formulated in the newly developed quantum-electrodynamical density functional theory (QEDFT). Our…
We present a detailed derivation and discussion of cavity Born-Oppenheimer coupled cluster (CBO-CC) theory and address cavity-modified electron correlation in the vibrational strong coupling regime. Methodologically, we combine the recently…
The emerging field of vibro-polaritonic chemistry studies the impact of light-matter hybrid states known as vibrational polaritons on chemical reactivity and molecular properties. Here, we discuss vibro-polaritonic chemistry from a quantum…
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…
We consider the modes of the electric field of a cavity where there is an embedded polarized dielectric film. The model consists in the Maxwell equations coupled to a Duffing oscillator for the film which we assume infinitely thin. We…
Experimental studies indicate that optical cavities can affect chemical reactions, through either vibrational or electronic strong coupling and the quantized cavity modes. However, the current understanding of the interplay between…
The Born--Oppenheimer approximation is the standard tool for the study of molecular systems. It is founded on the observation that the energy scale of the electron dynamics in a molecule is larger than that of the nuclei. A very similar…
We report the experimental study of a hybrid quantum solid state system comprising two-level artificial atoms coupled to cavity confined optical and vibrational modes. In this system combining cavity quantum electrodynamics and cavity…
Polariton chemistry exploits the strong interaction between quantized excitations in molecules and quantized photon states in optical cavities to affect chemical reactivity. Molecular polaritons have been experimentally realized by the…
The standard description of cavity-modified molecular reactions typically involves a single (resonant) mode, while in reality the quantum cavity supports a range of photon modes. Here we demonstrate that as more photon modes are accounted…