Related papers: Towards Accurate Mixed Quantum Classical Simulatio…
We employ an exact quantum mechanical simulation technique to investigate a model of cavity-modified chemical reactions in the condensed phase. The model contains the coupling of the reaction coordinate to a generic solvent, cavity coupling…
The prospect of controlling chemical reactivity using frequency-tunable optical microcavities has materialized over the past decade, evolving into a fascinating yet challenging new field of polaritonic chemistry, a multidisciplinary domain…
Vibrational strong coupling (VSC) provides a novel means to modify chemical reactions and energy transfer pathways. To efficiently model chemical dynamics under VSC in the collective regime, herein a hybrid quantum mechanical/molecular…
Recently, the mapping approach to surface hopping (MASH) was proposed as a method to simulate the non-adiabatic dynamics of two-level systems. It was shown that the method possesses many desirable qualities, both theoretically and through…
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…
Mixed-quantum classical (MQC) methods for simulating the dynamics of molecules at metal surfaces have the potential to accurately and efficiently provide mechanistic insight into reactive processes. Here, we introduce simple two-dimensional…
We develop a multi-state generalisation of the recently proposed mapping approach to surface hopping (MASH) for the simulation of electronically nonadiabatic dynamics. This new approach extends the original MASH method to be able to treat…
In the field of polaritonic chemistry, strong light-matter interactions are used to alter a chemical reaction inside an optical cavity. To explain and understand these processes, the development of reliable theoretical models is essential.…
In this paper, we aim to broaden the spectrum of possible applications of quantum computers and use their capabilities to investigate effects in cavity quantum electrodynamics ("cavity QED"). Interesting application examples are material…
Recent advances in polaritonic chemistry suggest that chemical reactions can be controlled via collective vibrational strong coupling (VSC) in a cavity. In this fully analytical work, we demonstrate that the collective vibrations of a…
Experiments indicate that collective coupling of molecular ensembles to confined optical modes can modify excited-state dynamics and photochemical reactivity. To describe such cavity-induced effects at atomic resolution, semi-classical…
We developed a general theoretical approach and a user-ready computer code that permit to study the dynamics of collisional energy transfer and ro-vibrational energy exchange in complex molecule-molecule collisions. The method is a mixture…
The violation of detailed balance poses a serious problem for the majority of current quasiclassical methods for simulating nonadiabatic dynamics. In order to analyze the severity of the problem, we predict the long-time limits of the…
We present a nonadiabatic classical-trajectory approach that offers the best of both worlds between fewest-switches surface hopping (FSSH) and quasiclassical mapping dynamics. This mapping approach to surface hopping (MASH) propagates the…
We propose a method which combines the quantum-classical mapping approach to surface hopping (MASH) with the dissipative quantum dynamics of the Lindblad master equation. Like conventional surface-hopping methods, our approach is based on…
Recent experiments in polariton chemistry have demonstrated that reaction rates can be modified by vibrational strong coupling to an optical cavity mode. Importantly, this modification only occurs when the frequency of the cavity mode is…
Quantum algorithms for simulating large and complex molecular systems are still in their infancy, and surpassing state-of-the-art classical techniques remains an ever-receding goal post. A promising avenue of inquiry in the meanwhile is to…
Nonadiabatic dynamics methods are an essential tool for investigating photochemical processes. In the context of employing first principles electronic structure techniques, such simulations can be carried out in a practical manner using…
The powerful molecular dynamics (MD) simulation is basically based on a picture that the atoms experience classical-like trajectories under the exertion of classical force field determined by the quantum mechanically solved electronic…
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…