Adaptive pruning for increased robustness and reduced computational overhead in Gaussian process accelerated saddle point searches

DOI

<p>Gaussian process (GP) regression provides a strategy for accelerating saddle point searches on high-dimensional energy surfaces by reducing the number of times the energy and its derivatives with respect to atomic coordinates need to be evaluated. The computational overhead in the hyperparameter optimization can, however, be large and make the approach inefficient. Failures can also occur if the search ventures too far into regions that are not represented well enough by the GP model. Here, these challenges are resolved by using geometry-aware optimal transport measures and an active pruning strategy using a summation over Wasserstein-1 distances for each atom-type in farthest-point sampling, selecting a fixed-size subset of geometrically diverse configurations to avoid rapidly increasing cost of GP updates as more observations are made. Stability is enhanced by permutation-invariant metric that provides a reliable trust radius for early-stopping and a logarithmic barrier penalty for the growth of the signal variance. These physically motivated algorithmic changes prove their efficacy by reducing to less than a half the mean computational time on a set of 238 challenging configurations from a previously published data set of chemical reactions. With these improvements, the GP approach is established as a robust and scalable algorithm for accelerating saddle point searches when the evaluation of the energy and atomic forces requires significant computational effort.</p> <p> </p> <p>This record contains the complete traces of dimer saddle search runs with the OT-GP (optimal transport GP) framework. This includes STDOUT and HDF5 trajectories. The record is a companion to the code in the associated GitHub repository and can be used to regenerate the figures and validate the analysis in the accompanying manuscript.</p>

Identifier
DOI https://doi.org/10.24435/materialscloud:3c-2f
Related Identifier https://github.com/theochemUI/otgpd_repro
Related Identifier https://doi.org/10.48550/arXiv.2510.06030
Related Identifier https://archive.materialscloud.org/communities/mcarchive
Related Identifier https://doi.org/10.24435/materialscloud:7t-f1
Metadata Access https://archive.materialscloud.org/oai2d?verb=GetRecord&metadataPrefix=oai_dc&identifier=oai:materialscloud.org:nfg5s-35666
Provenance
Creator Goswami, Rohit; Jónsson, Hannes
Publisher Materials Cloud
Contributor Goswami, Rohit
Publication Year 2025
Rights info:eu-repo/semantics/openAccess; Materials Cloud non-exclusive license to distribute v1.0; https://www.materialscloud.org/licenses/nonexclusive-distrib/1.0
OpenAccess true
Contact archive(at)materialscloud.org
Representation
Language English
Resource Type info:eu-repo/semantics/other
Format application/x-xz; text/markdown
Discipline Materials Science and Engineering