Six-dimensional quantum dynamics calculations for the state-to-state scattering of H_(2)/D_(2) on the rigid Cu(100)surface have been carried out using a time-dependent wave packet approach,based on an accurate neural ...Six-dimensional quantum dynamics calculations for the state-to-state scattering of H_(2)/D_(2) on the rigid Cu(100)surface have been carried out using a time-dependent wave packet approach,based on an accurate neural network potential energy surface fit for thousands of density functional theory data computed with the opt PBE-vd W density functional.The present results are compared with previous theoretical and experimental ones regarding to the rovibrationally(in)elastic scattering of H_(2) and D_(2) from Cu(100).In particular,we test the validity of the site-averaging approximation in this system by which the six-dimensional(in)elastic scattering probabilities are compared with the weighted average of four-dimensional results over fifteen fixed sites.Specifically,the site-averaging model reproduces vibrationally elastic scattering probabilities quite well,though less well for vibrationally inelastic results at high energies.These results support the use of the site-averaging model to reduce computational costs in future investigations on the state-to-state scattering dynamics of heavy diatomic or polyatomic molecules from metal surfaces,where full-dimensional calculations are too expensive.展开更多
基金supported by the National Natural Science Foundation of China(No.22073089 and No.22033007)。
文摘Six-dimensional quantum dynamics calculations for the state-to-state scattering of H_(2)/D_(2) on the rigid Cu(100)surface have been carried out using a time-dependent wave packet approach,based on an accurate neural network potential energy surface fit for thousands of density functional theory data computed with the opt PBE-vd W density functional.The present results are compared with previous theoretical and experimental ones regarding to the rovibrationally(in)elastic scattering of H_(2) and D_(2) from Cu(100).In particular,we test the validity of the site-averaging approximation in this system by which the six-dimensional(in)elastic scattering probabilities are compared with the weighted average of four-dimensional results over fifteen fixed sites.Specifically,the site-averaging model reproduces vibrationally elastic scattering probabilities quite well,though less well for vibrationally inelastic results at high energies.These results support the use of the site-averaging model to reduce computational costs in future investigations on the state-to-state scattering dynamics of heavy diatomic or polyatomic molecules from metal surfaces,where full-dimensional calculations are too expensive.
