Six-Dimensional State-to-State Quantum Dynamics of H_(2)/D_(2) Scattering from Cu(100):Validity of Site-Averaging Model  

Cu(100)表面上H_(2)/D_(2)散射的六维态-态量子动力学研究:位点平均模型的有效性

作　　者：Liang Zhang Lingjun Zhu Bin Jiang 张良;朱玲君;蒋彬(中国科学技术大学化学物理系,安徽省表面与界面化学与能源催化重点实验室,合肥230026)

机构地区：[1]Department of Chemical Physics,Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes,University of Science and Technology of China,Hefei 230026,China

出　　处：《Chinese Journal of Chemical Physics》2022年第1期143-152,I0063,I0064,共12页化学物理学报（英文）

基　　金：supported by the National Natural Science Foundation of China(No.22073089 and No.22033007)。

摘　　要：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.

关 键 词：State-to-state scattering Quantum dynamics Surface Site-averaging 

分 类 号：O641.1[理学—物理化学]