Finding Chemical Reaction Paths with a Multilevel Preconditioning Protocol
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. In conclusion, the approach also shows promise for free energy calculations when thermal noise can be controlled.
- Authors:
-
- Univ. of Chicago, IL (United States). Dept. of Chemistry; Univ. of Chicago, IL (United States). James Franck Inst.
- Univ. of Chicago, IL (United States). Dept. of Chemistry; Univ. of Chicago, IL (United States). James Franck Inst.; Univ. of Chicago, IL (United States). Inst. for Biophysical Dynamics; Univ. of Chicago, IL (United States). Computation Inst.; Argonne National Lab. (ANL), Argonne, IL (United States)
- Univ. of Chicago, IL (United States). James Franck Inst.; Univ. of Chicago, IL (United States). Computation Inst.; Univ. of Chicago, IL (United States). Dept. of Statistics
- Univ. of Chicago, IL (United States). Dept. of Chemistry; Univ. of Chicago, IL (United States). James Franck Inst.; Univ. of Chicago, IL (United States). Inst. for Biophysical Dynamics; Univ. of Chicago, IL (United States). Computation Inst.
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE; National Institutes of Health (NIH); National Science Foundation (NSF)
- OSTI Identifier:
- 1261135
- Grant/Contract Number:
- CHE-1136709; R01 GM109455-02; S10 RR029030-01; GM109455-02
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Theory and Computation
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 12; Journal ID: ISSN 1549-9618
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Kale, Seyit, Sode, Olaseni, Weare, Jonathan, and Dinner, Aaron R. Finding Chemical Reaction Paths with a Multilevel Preconditioning Protocol. United States: N. p., 2014.
Web. doi:10.1021/ct500852y.
Kale, Seyit, Sode, Olaseni, Weare, Jonathan, & Dinner, Aaron R. Finding Chemical Reaction Paths with a Multilevel Preconditioning Protocol. United States. https://doi.org/10.1021/ct500852y
Kale, Seyit, Sode, Olaseni, Weare, Jonathan, and Dinner, Aaron R. Fri .
"Finding Chemical Reaction Paths with a Multilevel Preconditioning Protocol". United States. https://doi.org/10.1021/ct500852y. https://www.osti.gov/servlets/purl/1261135.
@article{osti_1261135,
title = {Finding Chemical Reaction Paths with a Multilevel Preconditioning Protocol},
author = {Kale, Seyit and Sode, Olaseni and Weare, Jonathan and Dinner, Aaron R.},
abstractNote = {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. In conclusion, the approach also shows promise for free energy calculations when thermal noise can be controlled.},
doi = {10.1021/ct500852y},
journal = {Journal of Chemical Theory and Computation},
number = 12,
volume = 10,
place = {United States},
year = {Fri Nov 07 00:00:00 EST 2014},
month = {Fri Nov 07 00:00:00 EST 2014}
}
Web of Science
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