Quantum Monte Carlo Calculations on a Benchmark Molecule-Metal Surface Reaction: H₂ + Cu(111).

ABSTRACT: Accurate modeling of heterogeneous catalysis requires the availability of highly accurate potential energy surfaces. Within density functional theory, these can-unfortunately-depend heavily on the exchange-correlation functional. High-level ab initio calculations, on the other hand, are challenging due to the system size and the metallic character of the metal slab. Here, we present a quantum Monte Carlo (QMC) study for the benchmark system H₂ + Cu(111), focusing on the dissociative chemisorption barrier height. These computationally extremely challenging ab initio calculations agree to within 1.6 ± 1.0 kcal/mol with a chemically accurate semiempirical value. Remaining errors, such as time-step errors and locality errors, are analyzed in detail in order to assess the reliability

SUBMITTER: Doblhoff-Dier K 

PROVIDER: S-EPMC5508338 | biostudies-literature | 2017 Jul

REPOSITORIES: biostudies-literature