Ab initio molecular dynamics with enhanced sampling in heterogeneous catalysis

Giovannimaria Piccini, Mal Soon Lee, Simuck F. Yuk, Difan Zhang, Greg Collinge, Loukas Kollias, Manh Thuong Nguyen, Vassiliki Alexandra Glezakou, Roger Rousseau

Research output: Contribution to journalReview articlepeer-review

51 Scopus citations

Abstract

Ab initio molecular dynamics simulations combined with enhanced sampling techniques are becoming widespread methods to investigate chemical phenomena in catalytic systems. These techniques automatically include finite temperature effects, anharmonicity, and collective dynamics in their robust description of enthalpic and entropic contributions, which can have significant impact on reaction free energy landscapes. This contrasts with standard ab initio static approaches that are based on assessing reaction free energies from various coarse-grained descriptions of the reaction potential energy surface. Enhanced sampling ab initio molecular dynamics opens the way to first principles simulations of systems of increasing complexity like solid/liquid catalytic interfaces. In this work, we aim at guiding the reader through the basis of these techniques, summarizing their fundamental theoretical and practical aspects, and reviewing the relevant literature in the field. After a brief introduction to the problem, we will illustrate the advantage of using molecular simulations to include finite temperature effects, examine the most common ab initio techniques currently in use, describe their application to solid state heterogeneous catalysts, and finally critically review the most popular enhanced sampling techniques used in computational catalysis.

Original languageEnglish
Pages (from-to)12-37
Number of pages26
JournalCatalysis Science and Technology
Volume12
Issue number1
DOIs
StatePublished - Jan 7 2022
Externally publishedYes

Funding

GMP, MSL, MTN, LK, and VAG acknowledge support from the US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences. SFY, DZ, GC, and RR were supported by funding from US-DOE, Office of Energy Efficiency and Renewable Energy, Biotechnology Office's Consortium for Computationally Physics and Chemistry. Pacific Northwest National Laboratory is operated by Battelle for DOE under contract DE-AC05-76RL01830.

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