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On the many-body nature of intramolecular forces in FFLUX and its implications.

Authors
  • Konovalov, Anton1, 2
  • Symons, Benjamin C B1, 2
  • Popelier, Paul L A1, 2
  • 1 Manchester Institute of Biotechnology (MIB), Manchester, United Kingdom. , (United Kingdom)
  • 2 Department of Chemistry, University of Manchester, Manchester, United Kingdom. , (United Kingdom)
Type
Published Article
Journal
Journal of Computational Chemistry
Publisher
Wiley (John Wiley & Sons)
Publication Date
Jan 15, 2021
Volume
42
Issue
2
Pages
107–116
Identifiers
DOI: 10.1002/jcc.26438
PMID: 33107993
Source
Medline
Keywords
Language
English
License
Unknown

Abstract

FFLUX is a biomolecular force field under construction, based on Quantum Chemical Topology (QCT) and machine learning (kriging), with a minimalistic and physically motivated design. A detailed analysis of the forces within the kriging models as treated in FFLUX is presented, taking as a test example a liquid water model. The energies of topological atoms are modeled as 3Natoms -6 dimensional potential energy surfaces, using atomic local frames to represent the internal degrees of freedom. As a result, the forces within the kriging models in FFLUX are inherently N-body in nature where N refers to Natoms . This provides a fuller picture that is closer to a true quantum mechanical representation of interactions between atoms. The presented computational example quantitatively showcases the non-negligible (as much as 9%) three-body nature of bonded forces and angular forces in a water molecule. We discuss the practical impact on the pressure calculation with N-body forces and periodic boundary conditions (PBC) in molecular dynamics, as opposed to classical force fields with two-body forces. The equivalence between the PBC-related correction terms in the general virial equation is shown mathematically. © 2020 The Authors. Journal of Computational Chemistry published by Wiley Periodicals LLC.

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