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Title: New Angles on Standard Force Fields: Toward a General Approach for Treating Atomic-Level Anisotropy

Nearly all standard force fields employ the “sum-of-spheres” approximation, which models intermolecular interactions purely in terms of interatomic distances. Nonetheless, atoms in molecules can have significantly nonspherical shapes, leading to interatomic interaction energies with strong orientation dependencies. Neglecting this “atomic-level anisotropy” can lead to significant errors in predicting interaction energies. Herein, we propose a simple, transferable, and computationally efficient model (MASTIFF) whereby atomic-level orientation dependence can be incorporated into ab initio intermolecular force fields. MASTIFF includes anisotropic exchange-repulsion, charge penetration, and dispersion effects, in conjunction with a standard treatment of anisotropic long-range (multipolar) electrostatics. To validate our approach, we benchmark MASTIFF against various sum-of-spheres models over a large library of intermolecular interactions between small organic molecules. MASTIFF achieves quantitative accuracy, with respect to both high-level electronic structure theory and experiment, thus showing promise as a basis for “next-generation” force field development.
Authors:
 [1] ;  [2] ; ORCiD logo [1]
  1. Univ. of Wisconsin, Madison, WI (United States). Theoretical Chemistry Inst. Dept. of Chemistry
  2. Queen Mary Univ. of London (United Kingdom). Dept. of Physics and Astronomy
Publication Date:
Grant/Contract Number:
SC0014059; DGE-1256259; CHE-0840494; TG-CHE120088; TG-CHE170079
Type:
Published Article
Journal Name:
Journal of Chemical Theory and Computation
Additional Journal Information:
Journal Volume: 14; Journal Issue: 2; Journal ID: ISSN 1549-9618
Publisher:
American Chemical Society
Research Org:
Univ. of Wisconsin, Madison, WI (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 97 MATHEMATICS AND COMPUTING
OSTI Identifier:
1417681
Alternate Identifier(s):
OSTI ID: 1433884

Van Vleet, Mary J., Misquitta, Alston J., and Schmidt, J. R.. New Angles on Standard Force Fields: Toward a General Approach for Treating Atomic-Level Anisotropy. United States: N. p., Web. doi:10.1021/acs.jctc.7b00851.
Van Vleet, Mary J., Misquitta, Alston J., & Schmidt, J. R.. New Angles on Standard Force Fields: Toward a General Approach for Treating Atomic-Level Anisotropy. United States. doi:10.1021/acs.jctc.7b00851.
Van Vleet, Mary J., Misquitta, Alston J., and Schmidt, J. R.. 2017. "New Angles on Standard Force Fields: Toward a General Approach for Treating Atomic-Level Anisotropy". United States. doi:10.1021/acs.jctc.7b00851.
@article{osti_1417681,
title = {New Angles on Standard Force Fields: Toward a General Approach for Treating Atomic-Level Anisotropy},
author = {Van Vleet, Mary J. and Misquitta, Alston J. and Schmidt, J. R.},
abstractNote = {Nearly all standard force fields employ the “sum-of-spheres” approximation, which models intermolecular interactions purely in terms of interatomic distances. Nonetheless, atoms in molecules can have significantly nonspherical shapes, leading to interatomic interaction energies with strong orientation dependencies. Neglecting this “atomic-level anisotropy” can lead to significant errors in predicting interaction energies. Herein, we propose a simple, transferable, and computationally efficient model (MASTIFF) whereby atomic-level orientation dependence can be incorporated into ab initio intermolecular force fields. MASTIFF includes anisotropic exchange-repulsion, charge penetration, and dispersion effects, in conjunction with a standard treatment of anisotropic long-range (multipolar) electrostatics. To validate our approach, we benchmark MASTIFF against various sum-of-spheres models over a large library of intermolecular interactions between small organic molecules. MASTIFF achieves quantitative accuracy, with respect to both high-level electronic structure theory and experiment, thus showing promise as a basis for “next-generation” force field development.},
doi = {10.1021/acs.jctc.7b00851},
journal = {Journal of Chemical Theory and Computation},
number = 2,
volume = 14,
place = {United States},
year = {2017},
month = {12}
}