Accessing the usefulness of atomic adsorption configurations in predicting the adsorption properties of molecules with machine learning.

Abstract

We present a systematic study into the effect of adding atomic adsorption configurations into the training and validation dataset for a neural network's predictions of the adsorption energies of small molecules on single metal and bimetallic, single crystal surfaces. Specifically, we examine the efficacy of models trained with and without H and X atomic adsorption configurations, where X is C, N, or O, to predict XHn adsorption energies. In addition, we compare our machine learning models to traditional simple scaling relationships. We find that models trained with the atomic adsorption configurations outperform models trained with only molecular adsorption configurations, with as much as a 0.37 eV decrease in the MAE. We find that models trained with the atomic adsorption configurations slightly outperform traditional scaling relationships. In general, these results suggest it may be possible to vastly reduce the number of adsorption configurations one needs for training and validation datasets by supplementing said data with the adsorption configurations of composite atoms or smaller molecular fragments.