Combining DFT with ML to study size specific interactions between metal clusters and adsorbates

Abstract

To date, density functional theory (DFT) is one of the most accurate and yet practical theory to gain insight about materials properties. Although successful, the computational cost is the main hurdle even today. A way out is combining DFT with machine learning (ML) to reduce the computational cost without compromising accuracy. However, the success of this approach hinges on the correctness of the descriptors. In the present work, we demonstrate that, based on {\it only} interatomic distances as descriptors, our ML model predicts interaction energy between an adsorbate and Al cluster with absolute mean error (AME) $\sim$ 0.05 eV (or less) and reproduces the PES experienced by an incoming atom. Our extensive DFT calculations reveal that atoms experiencing identical environment within a cluster have identical interaction energy patterns. Further, we demonstrate that our model is not specific to Al clusters, and could be applied to clusters of different elements as well. Its application to compute PES experienced by various test atoms and molecules in the vicinity of different clusters proves the transferability of the model not just to clusters of different elements but also to various molecules. The descriptors chosen are invariant to rotation, translation, and permutation yet very simple to compute is one of the most crucial points of the present work.