相关论文: Determining the effect of hot electron dissipation…
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…
In the dynamics of atoms and molecules at metal surfaces, electron-hole pair excitations can play a crucial role. In the case of hyperthermal hydrogen atom scattering, they lead to nonadiabatic energy loss and highly inelastic scattering.…
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…
Electronic friction and the ensuing nonadiabatic energy loss play an important role in chemical reaction dynamics at metal surfaces. Using molecular dynamics with electronic friction evaluated on-the-fly from Density Functional Theory, we…
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,…
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…
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…
Experimental observations of multi-quantum relaxation of highly vibrationally excited NO scattering from Au(111) are a benchmark for the breakdown of Born-Oppenheimer approximation in molecule-surface systems. This remarkable vibrational…
We present a perturbation approach rooted in time-dependent density-functional theory to calculate electron hole (eh)-pair excitation spectra during the non-adiabatic vibrational damping of adsorbates on metal surfaces. Our analysis for the…
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…
Molecular adsorbates on metal surfaces exchange energy with substrate phonons and low-lying electron-hole pair excitations. In the limit of weak coupling, electron-hole pair excitations can be seen as exerting frictional forces on…
Nonadiabatic effects in chemical reaction at metal surfaces, due to excitation of electron-hole pairs, stand at the frontier of the studies of gas-surface reaction dynamics. However, the first principles description of electronic excitation…
An accurate description of nonadiabatic energy relaxation is crucial for modeling atomistic dynamics at metal surfaces. Interfacial energy transfer due to electron-hole pair excitations coupled to motion of molecular adsorbates is often…
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 $(ii)$…
NO scattering from metallic and insulating surfaces represent contrasting benchmark systems for understanding energy transfer at gas-surface interface. Strikingly different behaviors of highly vibrationally excited NO scattered from Au(111)…
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…
A theory of electronic friction is developed using the exact factorization of the electron-nuclear wavefunction. No assumption is made regarding the electronic bath, which can be made of independent or interacting electrons, and the nuclei…
We examine time-resolved X-ray diffraction from molecules in the gas phase which undergo nonadiabatic avoided-crossing dynamics involving strongly coupled electrons and nuclei. Several contributions to the signal are identified,…
The interaction between electronic and vibrational degrees of freedom in single-molecule junctions may result from the dependence of the electronic energies or the electronic states of the molecular bridge on the nuclear displacement. The…
We derive an explicit form for the electronic friction as felt by a molecule near a metal surface for the general case that molecule-metal couplings depend on nuclear coordinates. Our work generalizes a previous study by von Oppen et al…