Related papers: Coupled cluster cavity Born-Oppenheimer approximat…
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…
We present an ab initio method for computing vibro-polariton and phonon-polariton spectra of molecules and solids coupled to the photon modes of optical cavities. We demonstrate that if interactions of cavity photon modes with both nuclear…
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…
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…
In this work, we provide an overview of how well-established concepts in the fields of quantum chemistry and material sciences have to be adapted when the quantum nature of light becomes important in correlated matter-photon problems.…
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…
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…
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 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…
Intermolecular bonds are weak compared to covalent bonds, but they are strong enough to influence the properties of large molecular systems. In this work, we investigate how strong light-matter coupling inside an optical cavity can modify…
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…
Dissipation-free photon-photon interaction at the single photon level is studied in the context of cavity electromagnetically induced transparency (EIT). For a single multilevel atom exhibiting EIT in the strong cavity-coupling regime, the…
We develop coupled-cluster theory for systems of electrons strongly coupled to photons, providing a promising theoretical tool in polaritonic chemistry with a perspective of application to all types of fermion-boson coupled systems. We show…
In most theoretical descriptions of collective strong coupling of organic molecules to a cavity mode, the molecules are modeled as simple two-level systems. This picture fails to describe the rich structure provided by their internal…
Recent experimental progress in the field of cavity quantum electrodynamics allows to study the regime of strong interaction between quantized light and complex matter systems. Due to the coherent coupling between photons and matter-degrees…
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…
In this paper, we consider the time-dependent Born-Oppenheimer approximation (BOA) of a classical quantum molecule involving a possibly large number of nuclei and electrons, described by a Schr\"odinger equation. In the spirit of Born and…
Recent years have witnessed a surge of experimental and theoretical interest in controlling the properties of matter, such as its chemical reactivity, by confining it in optical cavities, where the enhancement of the light-matter coupling…
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…
We develop a mixed quantum-classical framework, dubbed the Moving Born-Oppenheimer Approximation (MBOA), to describe the dynamics of slow degrees of freedom (DOFs) coupled to fast ones. As in the Born-Oppenheimer Approximation (BOA), the…