Related papers: Vibrational strong coupling in liquid water from c…
Molecular polaritons are hybrid light-matter states that enable the exploration of potential cavity-modified chemistry. The development of dynamical, first-principles approaches for simulating molecular polaritons is important for…
Based on quantum-mechanical path-integral molecular dynamics simulations the impact of nuclear quantum effects on the vibrational and hydrogen bond dynamics in liquid water is investigated. The instantaneous fluctuations in the frequencies…
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…
The first exact quantum simulation of a real molecular system (HD$^+$) under strong ro-vibrational coupling to a quantized optical cavity mode in thermal equilibrium is presented. Theoretical challenges in describing strongly coupled…
A model designed to mimic the implications of the collective optical response of molecular ensembles in optical cavities on molecular vibronic dynamics is investigated. Strong molecule-radiation field coupling is often reached when a large…
Dielectric spectra are typically obtained in molecular dynamics (MD) simulations by analyzing the fluctuations, in the absence of an applied electric field, of the total dipole moment of the simulation box. We compare this standard method…
Recent experiments have demonstrated that vibrational strong coupling (VSC) between molecular vibrations and the optical cavity field can modify vibrational energy transfer (VET) processes in molecular systems. However, the underlying…
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.…
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)],…
Polaritons have gained significant attention for the tantalizing possibility of modifying chemical properties and dynamics by coupling molecules to resonant cavity modes to create hybrid light-matter quantum states. Herein, we implement the…
Polaritonic states arise when a bright optical transition of a molecular ensemble is resonantly matched to an optical cavity mode frequency. Here, we lay the groundwork to study the behavior of polaritons in clean, isolated systems by…
Phonon interactions are inevitable in cavity quantum electrodynamical systems based on solid-state emitters or fluorescent molecules, where vibrations of the lattice or chemical bonds couple to the electronic degrees of freedom. Due to the…
Vibrational spectroscopy is key for probing the interplay between the structure and dynamics of aqueous systems. In order to map different regions of experimental spectra to the microscopic structure of a system, it is important to combine…
We introduce a theory of chemical equilibrium in optical microcavities, which allows us to relate equilibrium reaction quotients in different electromagnetic environments. Our theory shows that in planar microcavities under strong coupling…
A theoretical approach aimed at the quantum statistical mechanics of a molecular ensemble coupled to a lossless cavity mode is presented. A canonical ensemble is considered and an approximate formula is devised for the Helmholtz free energy…
In this work, we present the analytical derivation and implementation of the quantum electrodynamics Hartree-Fock Hessian. We investigate how electronic strong coupling influences molecular vibrational properties, applying this framework to…
There is growing interest in using strongly coupled organic microcavities to tune molecular dynamics, including the electronic and vibrational properties of molecules. However, very little attention has been paid to the utility of cavity…
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…
Strong coupling between light and matter is possible with a variety of organic materials. In contrast to the simpler inorganic case, organic materials often have a complicated spectrum, with vibrationally dressed electronic transitions.…
When the interaction between a molecular system and confined light modes in an optical or plasmonic cavity is strong enough to overcome the dissipative process, hybrid light-matter states (polaritons) become the fundamental excitations in…