Related papers: Assessing mixed quantum-classical molecular dynami…
A novel mixed quantum-classical approach to simulating nonadiabatic dynamics of molecules at metal surfaces is presented. The method combines the numerically exact hierarchical equations of motion approach for the quantum electronic degrees…
Nonadiabatic coupling between electrons and molecular motion at metal surfaces leads to energy dissipation and dynamical steering effects during chemical surface dynamics. We present a theoretical approach to the scattering of molecules…
Mixed-quantum-classical molecular dynamics simulation implies an effective measurement on the electronic states owing to continuously tracking the atomic forces.Based on this insight, we propose a quantum trajectory mean-field approach for…
Adequate simulation of non-adiabatic dynamics through conical intersection requires account for a non-trivial geometric phase (GP) emerging in electronic and nuclear wave-functions in the adiabatic representation. Popular mixed…
Accurate description of nonadiabatic dynamics of molecules at metal surfaces involving electron transfer has been a longstanding challenge for theory. Here, we tackle this problem by first constructing high-dimensional neural network…
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…
A novel quantum dynamical method to simulate vibronic reaction dynamics in molecules at metal surfaces is proposed. The method is based on the hierarchical quantum master equation approach and uses a discrete variable representation of the…
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…
We implement a rare-event sampling scheme for quantifying the rate of thermally-activated nonadiabatic transitions in the condensed phase. Our QM/MM methodology uses the recently developed INAQS package to interface between an elementary…
An accurate description of nonadiabatic dynamics of molecular species on metallic surfaces poses a serious computational challenge associated with a multitude of closely-spaced electronic states. We propose a mixed quantum-classical scheme…
Trajectory-based mixed quantum-classical approaches to coupled electron-nuclear dynamics suffer from well-studied problems such as the lack of (or incorrect account for) decoherence in the trajectory surface hopping method and the inability…
Collisions of atoms and molecules with metal surfaces create electronic excitations in the metal, leading to nonadiabatic energy dissipation, inelastic scattering, and sticking. Mixed quantum-classical molecular dynamics simulation methods,…
Within a 2-D scattering model, we investigate the vibrational relaxation of an idealized molecule colliding with a metal surface. Two perturbative nonadiabatic dynamics schemes are compared: $(i)$ electronic friction (EF) and $(ii)$…
We perform on-the-fly non-adiabatic molecular dynamics simulations using the symmetrical quasi-classical (SQC) approach with the recently suggested molecular Tully models: ethylene and fulvene. We attempt to provide benchmarks of the SQC…
Dissociative chemisorption is a key process in hydrogen-metal surface chemistry, where nonadiabatic effects due to low-lying electron-hole-pair excitations may affect reaction outcomes. Molecular dynamics with electronic friction…
Energy transfer during molecular collisions on metal surfaces plays a pivotal role in a host of critical interfacial processes. Despite significant efforts, our understanding of relevant energy transfer mechanisms, even in an…
We present an approach for carrying out non-adiabatic molecular dynamics simulations of systems in which non-adiabatic transitions arise from the coupling between the classical atomic motions and a quasi-continuum of electronic quantum…
Electronic friction and Langevin dynamics is a popular mixed quantum-classical method for simulating the nonadiabatic dynamics of molecules interacting with metal surfaces, as it can be computationally more efficient than fully quantum…
Accelerating quantum dynamical simulations with quantum computing has received considerable attention but remains a significant challenge. In variational quantum algorithms for quantum dynamics, designing an expressive and shallow-depth…
The dynamics of an electronic two-level system coupled to an electromagnetic field are simulated explicitly for one and three dimensional systems through semiclassical propagation of the Maxwell-Liouville equations. We consider three…