Finding chemical reaction paths with a multilevel preconditioning protocol

Seyit Kale, Olaseni Sode, Jonathan Weare, Aaron R. Dinner

Research output: Contribution to journalArticle

Abstract

Finding transition paths for chemical reactions can be computationally costly owing to the level of quantum-chemical theory needed for accuracy. Here, we show that a multilevel preconditioning scheme that was recently introduced (Tempkin et al. J. Chem. Phys. 2014, 140, 184114) can be used to accelerate quantum-chemical string calculations. We demonstrate the method by finding minimum-energy paths for two well-characterized reactions: tautomerization of malonaldehyde and Claissen rearrangement of chorismate to prephanate. For these reactions, we show that preconditioning density functional theory (DFT) with a semiempirical method reduces the computational cost for reaching a converged path that is an optimum under DFT by several fold. The approach also shows promise for free energy calculations when thermal noise can be controlled. (Chemical Presented).

Original languageEnglish (US)
Pages (from-to)5467-5475
Number of pages9
JournalJournal of Chemical Theory and Computation
Volume10
Issue number12
DOIs
StatePublished - Dec 9 2014

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preconditioning
Density functional theory
Chemical reactions
chemical reactions
Thermal noise
Malondialdehyde
density functional theory
Free energy
thermal noise
strings
free energy
costs
Costs
energy

ASJC Scopus subject areas

  • Computer Science Applications
  • Physical and Theoretical Chemistry

Cite this

Finding chemical reaction paths with a multilevel preconditioning protocol. / Kale, Seyit; Sode, Olaseni; Weare, Jonathan; Dinner, Aaron R.

In: Journal of Chemical Theory and Computation, Vol. 10, No. 12, 09.12.2014, p. 5467-5475.

Research output: Contribution to journalArticle

Kale, Seyit ; Sode, Olaseni ; Weare, Jonathan ; Dinner, Aaron R. / Finding chemical reaction paths with a multilevel preconditioning protocol. In: Journal of Chemical Theory and Computation. 2014 ; Vol. 10, No. 12. pp. 5467-5475.
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