Gaussian process regression for geometry optimization

We implemented a geometry optimizer based on Gaussian process regression (GPR) to find minimum structures on potential energy surfaces. We tested both a two times differentiable form of the Matern kernel and the squared exponential kernel. The Matern kernel performs much better. We give a detailed description of the optimization procedures. These include overshooting the step resulting from GPR in order to obtain a higher degree of interpolation vs. extrapolation. In a benchmark against the Limited-memory Broyden-Fletcher-Goldfarb-Shanno optimizer of the DL-FIND library on 26 test systems, we found the new optimizer to generally reduce the number of required optimization steps. Published by AIP Publishing.