Gaussian Process Regression for Transition State Search

J Chem Theory Comput. 2018 Nov 13;14(11):5777-5786. doi: 10.1021/acs.jctc.8b00708. Epub 2018 Nov 1.


We implemented a gradient-based algorithm for transition state search which uses Gaussian process regression. Besides a description of the algorithm, we provide a method to find the starting point for the optimization if only the reactant and product minima are known. We perform benchmarks on 27 test systems against the dimer method and partitioned rational function optimization as implemented in the DL-FIND library. We found the new optimizer to significantly decrease the number of required energy and gradient evaluations.