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Title: Perspective: Ab initio force field methods derived from quantum mechanics

Abstract

It is often desirable to accurately and efficiently model the behavior of large molecular systems in the condensed phase (thousands to tens of thousands of atoms) over long time scales (from nanoseconds to milliseconds). In these cases, ab initio methods are difficult due to the increasing computational cost with the number of electrons. A more computationally attractive alternative is to perform the simulations at the atomic level using a parameterized function to model the electronic energy. Many empirical force fields have been developed for this purpose. However, the functions that are used to model interatomic and intermolecular interactions contain many fitted parameters obtained from selected model systems, and such classical force fields cannot properly simulate important electronic effects. Furthermore, while such force fields are computationally affordable, they are not reliable when applied to systems that differ significantly from those used in their parameterization. They also cannot provide the information necessary to analyze the interactions that occur in the system, making the systematic improvement of the functional forms that are used difficult. Ab initio force field methods aim to combine the merits of both types of methods. The ideal ab initio force fields are built on first principles and require nomore » fitted parameters. Ab initio force field methods surveyed in this perspective are based on fragmentation approaches and intermolecular perturbation theory. This perspective summarizes their theoretical foundation, key components in their formulation, and discusses key aspects of these methods such as accuracy and formal computational cost. The ab initio force fields considered here were developed for different targets, and this perspective also aims to provide a balanced presentation of their strengths and shortcomings. Finally, this perspective suggests some future directions for this actively developing area.« less

Authors:
 [1]; ORCiD logo [2];  [3];  [1]
  1. Department of Chemistry and Ames Laboratory, Iowa State University, Ames, Iowa 50011, USA
  2. Department of Chemistry, University of Colorado Denver, Denver, Colorado 80217, USA
  3. Argonne Leadership Computing Facility, Argonne, Illinois 60439, USA
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
National Science Foundation (NSF); Air Force Research Laboratory (AFRL) - Air Force Office of Scientific Research (AFOSR)
OSTI Identifier:
1481785
DOE Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 148; Journal Issue: 9; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English

Citation Formats

Xu, Peng, Guidez, Emilie B., Bertoni, Colleen, and Gordon, Mark S. Perspective: Ab initio force field methods derived from quantum mechanics. United States: N. p., 2018. Web. doi:10.1063/1.5009551.
Xu, Peng, Guidez, Emilie B., Bertoni, Colleen, & Gordon, Mark S. Perspective: Ab initio force field methods derived from quantum mechanics. United States. doi:10.1063/1.5009551.
Xu, Peng, Guidez, Emilie B., Bertoni, Colleen, and Gordon, Mark S. Wed . "Perspective: Ab initio force field methods derived from quantum mechanics". United States. doi:10.1063/1.5009551.
@article{osti_1481785,
title = {Perspective: Ab initio force field methods derived from quantum mechanics},
author = {Xu, Peng and Guidez, Emilie B. and Bertoni, Colleen and Gordon, Mark S.},
abstractNote = {It is often desirable to accurately and efficiently model the behavior of large molecular systems in the condensed phase (thousands to tens of thousands of atoms) over long time scales (from nanoseconds to milliseconds). In these cases, ab initio methods are difficult due to the increasing computational cost with the number of electrons. A more computationally attractive alternative is to perform the simulations at the atomic level using a parameterized function to model the electronic energy. Many empirical force fields have been developed for this purpose. However, the functions that are used to model interatomic and intermolecular interactions contain many fitted parameters obtained from selected model systems, and such classical force fields cannot properly simulate important electronic effects. Furthermore, while such force fields are computationally affordable, they are not reliable when applied to systems that differ significantly from those used in their parameterization. They also cannot provide the information necessary to analyze the interactions that occur in the system, making the systematic improvement of the functional forms that are used difficult. Ab initio force field methods aim to combine the merits of both types of methods. The ideal ab initio force fields are built on first principles and require no fitted parameters. Ab initio force field methods surveyed in this perspective are based on fragmentation approaches and intermolecular perturbation theory. This perspective summarizes their theoretical foundation, key components in their formulation, and discusses key aspects of these methods such as accuracy and formal computational cost. The ab initio force fields considered here were developed for different targets, and this perspective also aims to provide a balanced presentation of their strengths and shortcomings. Finally, this perspective suggests some future directions for this actively developing area.},
doi = {10.1063/1.5009551},
journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 9,
volume = 148,
place = {United States},
year = {2018},
month = {3}
}