Adaptive regularized Gaussian process regression for application in the context of hydrogen adsorption on graphene sheets.

We present a Gaussian process regression (GPR) scheme with an adaptive regularization scheme applied to the QM7 and QM9 test set, several protonated water clusters and specifically to the problem of atomic hydrogen adsorption on graphene sheets. For the last system our goal is to achieve good predictive accuracy with only a few training points. Therefore, we assess for these systems a self-correcting multilayer GPR model, in which the prediction is corrected by a chain of additional GPR models. In our adaptive regularization scheme, we impose no noise on the training data, but use an approach based on the data itself to account for its impurity. The strength of this strategy is that the data points are treated differently based on their importance and that the regularization can still be controlled by a single parameter. We assess how the accuracy of the prediction depends on this parameter. We can show that the new regularization scheme as well as the multilayer approach results in more robust predictors. Furthermore, we demonstrate that the predictor can be in good agreement with the density-functional theory results.