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

Journal of Chemical Theory and Computation
Katharina Doblhoff-DierGeert-Jan Kroes

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 of the results. The benchmark studies presented here are at the cutting edge of what is computationally feasible at the present time. Illustrating not only the achievable accuracy but also the challenges arising within QMC in such a calculation, our study presents a clear picture of where we stand at the moment and which approaches might allow for even more accurate results in the future.

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Citations

Dec 7, 2018·The Journal of Chemical Physics·Christopher R Bernard Rodríguez, Juan A Santana
Aug 25, 2018·Physical Chemistry Chemical Physics : PCCP·Kun CaoLudo B F Juurlink
Apr 1, 2021·The Journal of Physical Chemistry. a·Olga V LushchikovaJoost M Bakker
Apr 23, 2021·Physical Chemistry Chemical Physics : PCCP·Geert-Jan Kroes
Sep 21, 2019·The Journal of Physical Chemistry Letters·Rongrong YinBin Jiang
Aug 18, 2017·The Journal of Physical Chemistry Letters·Davide MiglioriniGeert-Jan Kroes
Feb 12, 2019·The Journal of Physical Chemistry. C, Nanomaterials and Interfaces·Gernot FüchselGeert-Jan Kroes

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Software Mentioned

CASINO
SRP
pwscf espresso
VASP
DMC
DFT

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