Towards a first-principles theory of surface thermodynamics and kinetics

TL;DR

This paper develops a first-principles theoretical framework that combines microscopic and macroscopic models to predict surface thermodynamics and kinetics, validated by application to the O/Ru(0001) system.

Contribution

It introduces a unified approach linking microscopic and macroscopic theories for surface processes, enabling predictive simulations.

Findings

Accurate prediction of thermal desorption spectra.

Calculation of heat of adsorption matching experimental data.

Surface phase diagram consistent with observations.

Abstract

Understanding of the complex behavior of particles at surfaces requires detailed knowledge of both macroscopic and microscopic processes that take place; also certain processes depend critically on temperature and gas pressure. To link these processes we combine state-of-the-art microscopic, and macroscopic phenomenological, theories. We apply our theory to the O/Ru(0001) system and calculate thermal desorption spectra, heat of adsorption, and the surface phase diagram. The agreement with experiment provides validity for our approach which thus identifies the way for a predictive simulation of surface thermodynamics and kinetics.