Related papers: Mechanistic Insights into Non-Adiabatic Interband …
Atomic and molecular scattering at semiconductor interfaces plays a central role in surface chemistry and catalysis, yet predictive simulations remain challenging due to strong nonadiabatic effects causing the breakdown of the…
A first-principles coupled electron-nuclear dynamics simulation based on real-time, time-dependent density functional theory and Ehrenfest dynamics quantitatively repro-duces bimodal translational energy loss and angular distributions…
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,…
Motivated by experiments with current biased superconducting atomic point contacts the general problem of nonadiabatic transitions between adiabatic surfaces in presence of strong dissipation is studied. For a single channel device the…
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…
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…
Electron transfer is an important and fundamental process in chemistry, biology and physics, and has received significant attention in recent years. Perhaps one of the most intriguing questions concerns with the realization of the…
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…
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…
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…
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…
Exceptional points, the spectral degeneracy points in the complex parameter space, are fundamental to non-Hermitian quantum systems. The dynamics of non-Hermitian systems in the presence of exceptional points differ significantly from those…
In the paper we derive a semiclassical model for surface hopping allowing quantum dynamical non-adiabatic transition between different potential energy surfaces in which cases the classical Born-Oppenheimer approximation breaks down. The…
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…
Density-functional theory calculations are performed to investigate hydrogen transport in the proton conductor BaSnO$_3$. Structural optimizations in the stable and saddle point configurations for transfer and reorientation allow…
We propose that the indirect adatom-adatom interaction mediated by the conduction electrons of a metallic surface is responsible for the $\sqrt{3}\times \sqrt{3}\Leftrightarrow 3\times 3$ structural phase transitions observed in Sn/Ge (111)…
The vibrational relaxation of NO molecules scattering from an Au(111) surface has served as the focus of efforts to understand nonadiabatic energy transfer at metal-molecule interfaces. Experimental measurements and previous theoretical…
We investigate the transition of a quantum wave-packet through a one-dimensional avoided crossing of molecular energy levels when the energy levels at the crossing point are tilted. Using superadiabatic representations, and an approximation…
Akin to the traditional quasi-classical trajectory method for investigating the dynamics on a single adiabatic potential energy surface for an elementary chemical reaction, we carry out the dynamics on a 2-state ab initio potential energy…
An extension of the CCS-method [Chem. Phys. 2004, 304, p. 103-120] for simulating non-adiabatic dynamics with quantum effects of the nuclei is put forward. The time-dependent Schr\"{o}dinger equation for the motion of the nuclei is solved…