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Title: Beyond Born-Mayer: Improved models for short-range repulsion in ab initio force fields

Abstract

Short-range repulsion within inter-molecular force fields is conventionally described by either Lennard-Jones or Born-Mayer forms. Despite their widespread use, these simple functional forms are often unable to describe the interaction energy accurately over a broad range of inter-molecular distances, thus creating challenges in the development of ab initio force fields and potentially leading to decreased accuracy and transferability. Herein, we derive a novel short-range functional form based on a simple Slater-like model of overlapping atomic densities and an iterated stockholder atom (ISA) partitioning of the molecular electron density. We demonstrate that this Slater-ISA methodology yields a more accurate, transferable, and robust description of the short-range interactions at minimal additional computational cost compared to standard Lennard-Jones or Born-Mayer approaches. Lastly, we show how this methodology can be adapted to yield the standard Born-Mayer functional form while still retaining many of the advantages of the Slater-ISA approach.

Authors:
 [1];  [2];  [3];  [1]
  1. Univ. of Wisconsin-Madison, Madison, WI (United States)
  2. Queen Mary Univ. of London, London (United Kingdom)
  3. Univ. of Cambridge, Cambridge (United Kingdom)
Publication Date:
Research Org.:
Univ. of Wisconsin-Madison, Madison, WI (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1299438
Alternate Identifier(s):
OSTI ID: 1259280; OSTI ID: 1433883
Grant/Contract Number:
SC0014059
Resource Type:
Journal Article: Published Article
Journal Name:
Journal of Chemical Theory and Computation
Additional Journal Information:
Journal Volume: 12; Journal Issue: 8; Journal ID: ISSN 1549-9618
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS

Citation Formats

Van Vleet, Mary J., Misquitta, Alston J., Stone, Anthony J., and Schmidt, Jordan R.. Beyond Born-Mayer: Improved models for short-range repulsion in ab initio force fields. United States: N. p., 2016. Web. doi:10.1021/acs.jctc.6b00209.
Van Vleet, Mary J., Misquitta, Alston J., Stone, Anthony J., & Schmidt, Jordan R.. Beyond Born-Mayer: Improved models for short-range repulsion in ab initio force fields. United States. doi:10.1021/acs.jctc.6b00209.
Van Vleet, Mary J., Misquitta, Alston J., Stone, Anthony J., and Schmidt, Jordan R.. Thu . "Beyond Born-Mayer: Improved models for short-range repulsion in ab initio force fields". United States. doi:10.1021/acs.jctc.6b00209.
@article{osti_1299438,
title = {Beyond Born-Mayer: Improved models for short-range repulsion in ab initio force fields},
author = {Van Vleet, Mary J. and Misquitta, Alston J. and Stone, Anthony J. and Schmidt, Jordan R.},
abstractNote = {Short-range repulsion within inter-molecular force fields is conventionally described by either Lennard-Jones or Born-Mayer forms. Despite their widespread use, these simple functional forms are often unable to describe the interaction energy accurately over a broad range of inter-molecular distances, thus creating challenges in the development of ab initio force fields and potentially leading to decreased accuracy and transferability. Herein, we derive a novel short-range functional form based on a simple Slater-like model of overlapping atomic densities and an iterated stockholder atom (ISA) partitioning of the molecular electron density. We demonstrate that this Slater-ISA methodology yields a more accurate, transferable, and robust description of the short-range interactions at minimal additional computational cost compared to standard Lennard-Jones or Born-Mayer approaches. Lastly, we show how this methodology can be adapted to yield the standard Born-Mayer functional form while still retaining many of the advantages of the Slater-ISA approach.},
doi = {10.1021/acs.jctc.6b00209},
journal = {Journal of Chemical Theory and Computation},
number = 8,
volume = 12,
place = {United States},
year = {Thu Jun 23 00:00:00 EDT 2016},
month = {Thu Jun 23 00:00:00 EDT 2016}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1021/acs.jctc.6b00209

Citation Metrics:
Cited by: 7works
Citation information provided by
Web of Science

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