title: High-Dimensional Atomistic Neural Network Potentials for Molecule-Surface Interactions: HCl Scattering from Au(111).
abstract: Ab initio molecular dynamics (AIMD) simulations of molecule-surface scattering allow first-principles characterization of the dynamics. However, the large number of density functional theory calculations along the trajectories is very costly, limiting simulations of long-time events and giving rise to poor statistics. To avoid this computational bottleneck, we report here the development of a high-dimensional molecule-surface interaction potential energy surface (PES) with movable surface atoms, using a machine learning approach. With 60 degrees of freedom, this PES allows energy transfer between the energetic impinging molecule and thermal surface atoms. Classical trajectory calculations for the scattering of DCl from Au(111) on this PES are found to agree well with AIMD simulations, with ∼105-fold acceleration. Scattering of HCl from Au(111) is further investigated and compared with available experimental results.
authors.affiliation: Department of Chemistry and Chemical Biology, University of New Mexico , Albuquerque, New Mexico 87131, United States.|Department of Mechanical Engineering, Massachusetts Institute of Technology , Cambridge, Massachusetts 02139, United States.
authors.forename: Brian
authors.initials: B
authors.lastname: Kolb
authors.affiliation: Department of Chemical Physics, University of Science and Technology of China , Hefei, Anhui 230026, China.
authors.forename: Xuan
authors.initials: X
authors.lastname: Luo
authors.affiliation: Department of Chemical Physics, University of Science and Technology of China , Hefei, Anhui 230026, China.
authors.forename: Xueyao
authors.initials: X
authors.lastname: Zhou
authors.affiliation: Department of Chemical Physics, University of Science and Technology of China , Hefei, Anhui 230026, China.
authors.forename: Bin
authors.identifier: http://orcid.org/0000-0003-2696-5436
authors.initials: B
authors.lastname: Jiang
authors.affiliation: Department of Chemistry and Chemical Biology, University of New Mexico , Albuquerque, New Mexico 87131, United States.
authors.forename: Hua
authors.identifier: http://orcid.org/0000-0001-9901-053X
authors.initials: H
authors.lastname: Guo