Automated calculation of thermal rate coefficients using ring polymer molecular dynamics and machine-learning interatomic potentials with active learning
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c8cp06037a.pdf
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81040798e5d22eb71f1644b2e15b826f
Author(s)
Novikov, I. S.
Shapeev, A. V.
Suleimanov, Yuri V.
Date Issued
November 2018
Journal
Physical Chemistry Chemical Physics
Publisher
Royal Society of Chemistry
Citation
Novikov, I. S., Y. V. Suleimanov, and A. V. Shapeev. “Automated Calculation of Thermal Rate Coefficients Using Ring Polymer Molecular Dynamics and Machine-Learning Interatomic Potentials with Active Learning.” Physical Chemistry Chemical Physics 20, no. 46 (2018): 29503–29512.
Version
Final published version
Abstract
We propose a methodology for the fully automated calculation of thermal rate coefficients of gas phase chemical reactions, which is based on combining ring polymer molecular dynamics (RPMD) and machine-learning interatomic potentials actively learning on-the-fly. Based on the original computational procedure implemented in the RPMDrate code, our methodology gradually and automatically constructs the potential energy surfaces (PESs) from scratch with the data set points being selected and accumulated during the RPMDrate simulation. Such an approach ensures that our final machine-learning model provides a reliable description of the PES that avoids artifacts during exploration of the phase space by RPMD trajectories. We tested our methodology on two representative thermally activated chemical reactions studied recently by RPMDrate at temperatures within the interval of 300–1000 K. The corresponding PESs were generated by fitting to only a few thousand automatically generated structures (less than 5000) while the RPMD rate coefficients showed deviation from the reference values within the typical convergence error of RPMDrate. In future, we plan to apply our methodology to chemical reactions that proceed via complex-formation thus providing a completely general tool for calculating RPMD thermal rate coefficients for any polyatomic gas phase chemical reaction.
MIT Department
Massachusetts Institute of Technology. Department of Chemical Engineering
Terms of Use
Creative Commons Attribution Noncommercial 3.0 unported license
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DOI of Published Version
https://doi.org/10.1039/C8CP06037A
