Many-Body Effects in Aqueous Systems: Synergies Between Interaction Analysis Techniques and Force Field Development

Interaction analysis techniques, including the many-body expansion (MBE), symmetry-adapted perturbation theory, and energy decomposition analysis, allow for an intuitive understanding of complex molecular interactions. We review these methods by first providing a historical context for the study of...

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Bibliographic Details
Published in:Annual review of physical chemistry 2023-04, Vol.74 (1), p.337-360
Main Authors: Heindel, Joseph P, Herman, Kristina M, Xantheas, Sotiris S
Format: Article
Language:English
Subjects:
Electronic structure
Granulation
INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
intermolecular interactions
Many body problem
many-body expansion
Molecular dynamics
Molecular interactions
Multipoles
Neural networks
Parameterization
Perturbation theory
polarizable force fields
Potential energy
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Summary:Interaction analysis techniques, including the many-body expansion (MBE), symmetry-adapted perturbation theory, and energy decomposition analysis, allow for an intuitive understanding of complex molecular interactions. We review these methods by first providing a historical context for the study of many-body interactions and discussing how nonadditivities emerge from Hamiltonians containing strictly pairwise-additive interactions. We then elaborate on the synergy between these interaction analysis techniques and the development of advanced force fields aimed at accurately reproducing the Born-Oppenheimer potential energy surface. In particular, we focus on ab initio-based force fields that aim to explicitly reproduce many-body terms and are fitted to high-level electronic structure results. These force fields generally incorporate many-body effects through ( a ) parameterization of distributed multipoles, ( b ) explicit fitting of the MBE, ( c ) inclusion of many-atom features in a neural network, and ( d ) coarse-graining of many-body terms into an effective two-body term. We also discuss the emerging use of the MBE to improve the accuracy and speed of ab initio molecular dynamics.
ISSN:0066-426X
1545-1593
DOI:10.1146/annurev-physchem-062422-023532