Energy dissipation at metal surfaces

Abstract

Conversion of energy at the gas-solid interface lies at the heart of many industrial applications such as heterogeneous catalysis. Dissipation of parts of this energy into the substrate bulk drives the thermalization of surface species, but also constitutes a potentially unwanted loss channel. At present, little is known about the underlying microscopic dissipation mechanisms and their (relative) efficiency. At metal surfaces, prominent such mechanisms are the generation of substrate phonons and the electronically non-adiabatic excitation of electron-hole pairs. In recent years, dedicated surface science experiments at defined single-crystal surfaces and predictive-quality firstprinciples simulations have increasingly been used to analyze these dissipation mechanisms in prototypical surface dynamical processes such as gas-phase scattering and adsorption, diffusion, vibration, and surface reactions. In this topical review we provide an overview of modeling approaches to incorporate dissipation into corresponding dynamical simulations starting from coarsegrained effective theories to increasingly sophisticated methods. We illustrate these at the level of individual elementary processes through applications found in the literature, while specifically highlighting the persisting difficulty of gauging their performance based on experimentally accessible observables.

Material properties particularly suited to be measured with helium scattering: selected examples from 2D materials, van der Waals heterostructures, glassy materials, catalytic substrates, topological insulators and superconducting radio frequency materials

“…Through surface correlation measurements, HeSE offers a unique way to measure rates of energy transfer, and thus the strength of energetic coupling. 113,122,123 The method has been used to measure atomic scale frictional coupling constants, 124 explain the absolute rate of motion in complex systems, 125 and to test quantum rate theories. 119 3.6.4 Ultra low energy vibrational properties.…”

Determining the Effect of Hot Electron Dissipation on Molecular Scattering Experiments at Metal Surfaces

“… 2 As a result, the gaseous species in the vicinity of a metal surface can easily dissipate their energy not only by exciting lattice vibrations but also through electron–hole pair excitations (EHPs). 3 Indeed, there has been growing experimental evidence of such nonadiabatic effects in surface chemistry 4 from quantum-state-resolved molecular beam scattering experiments, 5 chemicurrent measurements, 6 , 7 and ultrafast spectroscopy, 8 providing valuable benchmark data for testing first-principles theories of nonadiabatic gas-surface interactions. 9 However, a predictive quantitation of how nonadiabatic effects contribute to measurable dynamic properties remains elusive.…”

Hot-electron effects during reactive scattering of H2 from Ag(111): the interplay between mode-specific electronic friction and the potential energy landscape

“…Energy exchange between adsorbate and substrate degrees of freedom (DOFs) has a potentially significant impact on chemical reaction dynamics at solid surfaces 1. At metal surfaces, in particular, energy carried by the adsorbate could dissipate to either surface phonons or electrons 2. Due to the continuous distribution of metallic electronic states across the Fermi level, the excitation of electron–hole pairs (EHPs) can be induced by the interaction between the adsorbate and metal atoms with the electrons in the metal surface 3,4.…”