Bayesian optimization for the inverse scattering problem in quantum reaction dynamics

doi:10.1088/1367-2630/ab0099

	Bayesian optimization for the inverse scattering problem in quantum reaction dynamics
	Vargas-Hernández,R A 2; Guan,Y 1,3; Zhang,D H 1,3; Krems,R V 2
刊名	New Journal of Physics
	2019-02-28
卷号	21 期号:2
关键词	bayesian optimization gaussian processes inverse scattering problem
ISSN号	1367-2630
DOI	10.1088/1367-2630/ab0099
英文摘要	Abstract We propose a machine-learning approach based on Bayesian optimization to build global potential energy surfaces (PES) for reactive molecular systems using feedback from quantum scattering calculations. The method is designed to correct for the uncertainties of quantum chemistry calculations and yield potentials that reproduce accurately the reaction probabilities in a wide range of energies. These surfaces are obtained automatically and do not require manual fitting of the ab initio energies with analytical functions. The PES are built from a small number of ab initio points by an iterative process that incrementally samples the most relevant parts of the configuration space. Using the dynamical results of previous authors as targets, we show that such feedback loops produce accurate global PES with 30 ab initio energies for the three-dimensional H?+?H2 → H2 + H reaction and 290 ab inito energies for the six-dimensional OH + H2 → H2O?+?H reaction. These surfaces are obtained from 360 scattering calculations for H3 and 600 scattering calculations for OH3. We also introduce a method that quickly converges to an accurate PES without the a priori knowledge of the dynamical results. By construction, our method illustrates the lowest number of potential energy points (i.e. the minimum information) required for the non-parametric construction of global PES for quantum reactive scattering calculations.
语种	英语
出版者	IOP Publishing
WOS记录号	IOP:1367-2630-21-2-AB0099
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/165778]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
作者单位	1.University of Chinese Academy of Sciences, Beijing 100049, People's Republic of China 2.Department of Chemistry, University of British Columbia, Vancouver, BC V6T 1Z1, Canada 3.State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Science, Dalian 116023, People's Republic of China
推荐引用方式 GB/T 7714	Vargas-Hernández,R A,Guan,Y,Zhang,D H,et al. Bayesian optimization for the inverse scattering problem in quantum reaction dynamics[J]. New Journal of Physics,2019,21(2).
APA	Vargas-Hernández,R A,Guan,Y,Zhang,D H,&Krems,R V.(2019).Bayesian optimization for the inverse scattering problem in quantum reaction dynamics.New Journal of Physics,21(2).
MLA	Vargas-Hernández,R A,et al."Bayesian optimization for the inverse scattering problem in quantum reaction dynamics".New Journal of Physics 21.2(2019).