Data-driven models for ground and excited states for Single Atoms on Ceria

作     者：Julian Geiger Albert Sabadell-Rendón Nathan Daelman Núria López 

作者机构：Institute of Chemical Research of Catalonia(ICIQ)The Barcelona Institute of Science and Technology(BIST)Avinguda Països Catalans 1643007TarragonaSpain Universitat Rovira i VirgiliAvinguda Catalunya3543002TarragonaSpain 

出 版 物：《npj Computational Materials》 (计算材料学（英文）)

年 卷 期：2022年第8卷第1期

页      面：1636-1643页

核心收录：

学科分类：081704[工学-应用化学] 07[理学] 070304[理学-物理化学(含∶化学物理)] 08[工学] 0817[工学-化学工程与技术] 0703[理学-化学] 

基　　金：This work was funded by the Generalitat de Catalunya and the European Union under Grant 2020_FI_B 00266 the Spanish Ministry of Economy and Competitiveness under the Mineco POP grant BES-2016-076361 the Ministry of Science and Innovation(Ref.No.RTI2018-101394-BI00) 

主　　题：theory excited states 

摘      要：Ceria-based single-atom catalysts present complex electronic structures due to the dynamic electron transfer between the metal atoms and the semiconductor oxide *** these materials implies retrieving all states in these electronic ensembles,which can be limiting if done via density functional ***,we propose a data-driven approach to obtain a parsimonious model identifying the appearance of dynamic charge transfer for the single atoms(SAs).We first constructed a database of(701)electronic configurations for the group 9–11 metals on CeO_(2)(100).Feature Selection based on predictive Elastic Net and Random Forest models highlights eight fundamental variables:atomic number,ionization potential,size,and metal coordination,metal–oxygen bond strengths,surface strain,and Coulomb *** these variables a Bayesian algorithm yields an expression for the adsorption energies of SAs in ground and low-lying excited *** work paves the way towards understanding electronic structure complexity in metal/oxide interfaces.