Reaction energetics of Hydrogen on the Si(100) surface: A periodic many-electron theory study

TL;DR

This study uses advanced many-electron wavefunction methods with periodic boundary conditions to accurately predict hydrogen dissociation energetics on Si(100), providing insights and benchmarks for computational surface chemistry.

Contribution

It demonstrates that wavefunction-based periodic methods can achieve chemically accurate reaction energetics, improving understanding and benchmarking of surface reactions.

Findings

Accurate activation barrier and chemisorption energy predictions.

Agreement with experimental data.

Benchmarking of density functional theory methods.

Abstract

We report on a many-electron wavefunction theory study for the reaction energetics of hydrogen dissociation on the Si(100) surface. We demonstrate that quantum chemical wavefunction based methods using periodic boundary conditions can predict chemically accurate results for the activation barrier and the chemisorption energy in agreement with experimental findings. These highly accurate results for the reaction energetics enable a deeper understanding of the underlying physical mechanism and make it possible to benchmark widely used density functional theory methods.