Comparison of intermediate-range order in GeO$_2$ glass: molecular dynamics using machine-learning interatomic potential vs.\ reverse Monte Carlo fitting to experimental data

Abstract

The short and intermediate-range order in GeO$_2$ glass are investigated by molecular dynamics using machine-learning interatomic potential trained on ab initio calculation data and compared with reverse Monte Carlo fitting of neutron diffraction data. To characterize the structural differences in each model, the total/partial structure factors, coordination number, ring size and shape distributions, and persistent homology analysis were performed. These results show that although the two approaches yield similar two-body correlations, they can lead to three-dimensional models with very different short and intermediate-range ordering. A clear difference was observed especially in the ring distributions; RMC models exhibit a broad distribution in the ring size distribution, while neural network potential molecular dynamics yield much narrower ring distributions. This confirms that the density functional approximation in the ab initio calculations determines the preferred network assembly more strictly than RMC with simple coordination constraints and neutron diffraction data with isotope substitution.