High-dimensional atomistic neural network potential to study the alignment-resolved O2 scattering from highly oriented pyrolytic graphite

Abstract

A high dimensional and accurate atomistic neural network potential energy surface (ANN-PES) that describes the interaction between one O2 molecule and a highly oriented pyrolytic graphite (HOPG) surface has been constructed using the open-source package (aenet). The validation of the PES is performed by paying attention to static characteristics as well as by testing its performance in reproducing previous ab initio molecular dynamics simulation results. Subsequently, the ANN-PES is used to perform quasi-classical molecular dynamics calculations of the alignment-dependent scattering of O2 from HOPG. The results are obtained for 200 meV O2 molecules with different initial alignments impinging with a polar incidence angle with respect to the surface normal of 22.5° on a thermalized (110 and 300 K) graphite surface. The choice of these initial conditions in our simulations is made to perform comparisons to recent experimental results on this system. Our results show that the scattering of O2 from the HOPG surface is a rather direct process, that the angular distributions are alignment dependent, and that the final translational energy of end-on molecules is around 20% lower than that of side-on molecules. Upon collision with the surface, the molecules that are initially aligned perpendicular to the surface become highly rotationally excited, whereas a very small change in the rotational state of the scattered molecules is observed for the initial parallel alignments. The latter confirms the energy transfer dependence on the stereodynamics for the present system. The results of our simulations are in overall agreement with the experimental observations regarding the shape of the angular distributions and the alignment dependence of the in-plane reflected molecules.