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How Accurate Can a Force Field Become? A Polarizable Multipole Model Combined with Fragment-wise Quantum-Mechanical Calculations

Söderhjelm, Pär LU and Ryde, Ulf LU (2009) In Journal of physical chemistry. A 113(3). p.617-627
Abstract
A new method to accurately estimate the interaction energy between a large molecule and a smaller ligand

is presented. The method approximates the electrostatic and induction contributions classically by multipole

and polarizability expansions, but uses explicit quantum-mechanical fragment calculations for the remaining

(nonclassical) contributions, mainly dispersion and exchange repulsion. Thus, it represents a limit of how

accurate a force field can ever become for interaction energies if pairwise additivity of the nonclassical term

is assumed (e.g., all general-purpose force fields). The accuracy is tested by considering protein-ligand model

systems for which the true... (More)
A new method to accurately estimate the interaction energy between a large molecule and a smaller ligand

is presented. The method approximates the electrostatic and induction contributions classically by multipole

and polarizability expansions, but uses explicit quantum-mechanical fragment calculations for the remaining

(nonclassical) contributions, mainly dispersion and exchange repulsion. Thus, it represents a limit of how

accurate a force field can ever become for interaction energies if pairwise additivity of the nonclassical term

is assumed (e.g., all general-purpose force fields). The accuracy is tested by considering protein-ligand model

systems for which the true MP2/6-31G* interaction energies can be computed. The method is shown to be

more accurate than related fragmentation approaches. The remaining error (2-5 and ∼10 kJ/mol for neutral and charged ligands, respectively) can be decreased by including the polarizing effect from surrounding fragments in the quantum-mechanical calculations. (Less)
Please use this url to cite or link to this publication:
author
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Journal of physical chemistry. A
volume
113
issue
3
pages
617 - 627
publisher
The American Chemical Society
external identifiers
  • wos:000262522300012
  • scopus:60549094599
ISSN
1520-5215
DOI
10.1021/jp8073514
language
English
LU publication?
yes
id
c68f67fe-1386-4f9f-886e-87931e12cd76 (old id 1277140)
date added to LUP
2009-01-16 08:43:07
date last changed
2017-10-29 04:01:02
@article{c68f67fe-1386-4f9f-886e-87931e12cd76,
  abstract     = {A new method to accurately estimate the interaction energy between a large molecule and a smaller ligand <br/><br>
is presented. The method approximates the electrostatic and induction contributions classically by multipole <br/><br>
and polarizability expansions, but uses explicit quantum-mechanical fragment calculations for the remaining <br/><br>
(nonclassical) contributions, mainly dispersion and exchange repulsion. Thus, it represents a limit of how <br/><br>
accurate a force field can ever become for interaction energies if pairwise additivity of the nonclassical term <br/><br>
is assumed (e.g., all general-purpose force fields). The accuracy is tested by considering protein-ligand model <br/><br>
systems for which the true MP2/6-31G* interaction energies can be computed. The method is shown to be <br/><br>
more accurate than related fragmentation approaches. The remaining error (2-5 and ∼10 kJ/mol for neutral and charged ligands, respectively) can be decreased by including the polarizing effect from surrounding fragments in the quantum-mechanical calculations.},
  author       = {Söderhjelm, Pär and Ryde, Ulf},
  issn         = {1520-5215},
  language     = {eng},
  number       = {3},
  pages        = {617--627},
  publisher    = {The American Chemical Society},
  series       = {Journal of physical chemistry. A},
  title        = {How Accurate Can a Force Field Become? A Polarizable Multipole Model Combined with Fragment-wise Quantum-Mechanical Calculations},
  url          = {http://dx.doi.org/10.1021/jp8073514},
  volume       = {113},
  year         = {2009},
}