Improving the convergence of closed and open path integral molecular dynamics via higher order Trotter factorization schemes

Alejandro Pérez, Mark Tuckerman

Research output: Contribution to journalArticle

Abstract

Higher order factorization schemes are developed for path integral molecular dynamics in order to improve the convergence of estimators for physical observables as a function of the Trotter number. The methods are based on the Takahashi-Imada and Susuki decompositions of the Boltzmann operator. The methods introduced improve the averages of the estimators by using the classical forces needed to carry out the dynamics to construct a posteriori weighting factors for standard path integral molecular dynamics. The new approaches are straightforward to implement in existing path integral codes and carry no significant overhead. The Suzuki higher order factorization was also used to improve the end-to-end distance estimator in open path integral molecular dynamics. The new schemes are tested in various model systems, including an ab initio path integral molecular dynamics calculation on the hydrogen molecule and a quantum water model. The proposed algorithms have potential utility for reducing the cost of path integral molecular dynamics calculations of bulk systems.

Original languageEnglish (US)
Article number064104
JournalJournal of Chemical Physics
Volume135
Issue number6
DOIs
StatePublished - Aug 14 2011

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Factorization
factorization
Molecular dynamics
molecular dynamics
estimators
Hydrogen
Decomposition
Molecules
Water
costs
decomposition
operators
hydrogen
Costs
water
molecules

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Cite this

Improving the convergence of closed and open path integral molecular dynamics via higher order Trotter factorization schemes. / Pérez, Alejandro; Tuckerman, Mark.

In: Journal of Chemical Physics, Vol. 135, No. 6, 064104, 14.08.2011.

Research output: Contribution to journalArticle

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