TY - JOUR
T1 - Nudged Elastic Band Calculations Accelerated with Gaussian Process Regression Based on Inverse Interatomic Distances
AU - Koistinen, Olli Pekka
AU - Ásgeirsson, Vilhjálmur
AU - Vehtari, Aki
AU - Jónsson, Hannes
N1 - Funding Information: This work was financially supported by the Academy of Finland (Grant 278260; Flagship program: Finnish Center for Artificial Intelligence, FCAI, Grants 320181, 320182, 320183). O.-P.K. was supported by the Finnish Cultural Foundation (Grant 180536) and V.A by a doctoral fellowship from the University of Iceland Research Fund. Funding Information: The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.jctc.9b00692 . Extensions of Figures 1 – 4 and 7 including GP approximations obtained with stationary Matérn covariance functions and GP-NEB results obtained by feeding the inverse-distance difference measure to Matérn covariance functions ( PDF ) This work was financially supported by the Academy of Finland (Grant 278260; Flagship program: Finnish Center for Artificial Intelligence, FCAI, Grants 320181, 320182, 320183). O.-P.K. was supported by the Finnish Cultural Foundation (Grant 180536) and V.Á by a doctoral fellowship from the University of Iceland Research Fund. The authors declare no competing financial interest. Publisher Copyright: Copyright © 2019 American Chemical Society.
PY - 2019/12/10
Y1 - 2019/12/10
N2 - Calculations of minimum energy paths for atomic rearrangements using the nudged elastic band method can be accelerated with Gaussian process regression to reduce the number of energy and atomic force evaluations needed for convergence. Problems can arise, however, when configurations with large forces due to short distance between atoms are included in the data set. Here, a significant improvement to the Gaussian process regression approach is obtained by basing the difference measure between two atomic configurations in the covariance function on the inverted interatomic distances and by adding a new early stopping criterion for the path relaxation phase. This greatly improves the performance of the method in two applications where the original formulation does not work well: a dissociative adsorption of an H2 molecule on a Cu(110) surface and a diffusion hop of an H2O molecule on an ice Ih(0001) surface. Also, the revised method works better in the previously analyzed benchmark application to rearrangement transitions of a heptamer island on a surface, requiring fewer energy and force evaluations for convergence to the minimum energy path.
AB - Calculations of minimum energy paths for atomic rearrangements using the nudged elastic band method can be accelerated with Gaussian process regression to reduce the number of energy and atomic force evaluations needed for convergence. Problems can arise, however, when configurations with large forces due to short distance between atoms are included in the data set. Here, a significant improvement to the Gaussian process regression approach is obtained by basing the difference measure between two atomic configurations in the covariance function on the inverted interatomic distances and by adding a new early stopping criterion for the path relaxation phase. This greatly improves the performance of the method in two applications where the original formulation does not work well: a dissociative adsorption of an H2 molecule on a Cu(110) surface and a diffusion hop of an H2O molecule on an ice Ih(0001) surface. Also, the revised method works better in the previously analyzed benchmark application to rearrangement transitions of a heptamer island on a surface, requiring fewer energy and force evaluations for convergence to the minimum energy path.
UR - https://www.scopus.com/pages/publications/85075151213
U2 - 10.1021/acs.jctc.9b00692
DO - 10.1021/acs.jctc.9b00692
M3 - Article
C2 - 31638795
SN - 1549-9618
VL - 15
SP - 6738
EP - 6751
JO - Journal of Chemical Theory and Computation
JF - Journal of Chemical Theory and Computation
IS - 12
ER -