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Perspective: Ab initio force field methods derived from quantum mechanics

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/1.5009551· OSTI ID:1481785
 [1];  [2];  [3];  [1]
  1. Ames Lab., and Iowa State Univ., Ames, IA (United States)
  2. Univ. of Colorado, Denver, CO (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
+ Show Author Affiliations
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.
Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
Air Force Research Laboratory (AFRL) - Air Force Office of Scientific Research (AFOSR); National Science Foundation (NSF); USDOE Office of Science (SC)
Grant/Contract Number:
AC02-06CH11357; AC02-07CH11358
OSTI ID:
1481785
Alternate ID(s):
OSTI ID: 1423723
Journal Information:
Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 9 Vol. 148; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English

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Could Quantum Mechanical Properties Be Reflected on Classical Molecular Dynamics? The Case of Halogenated Organic Compounds of Biological Interest journal December 2019
Multiscale Approach to Fluid-Solid Interfaces: An overview of methodologies coupling fluid mechanics to molecular dynamics and quantum theory text January 2019

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Related Subjects

71 CLASSICAL AND QUANTUM MECHANICS
GENERAL PHYSICS
Ab-initio methods
Chemical elements
Classical force fields
Electrostatics
Intermolecular forces
Molecular dynamics
Molecular electronic properties
Perturbation theory
Polarizability
Polarization