Predicting the Surface Phase Diagram of Ag(111) Using Ab Initio Grand Canonical Monte Carlo(PPT)

摘要

Current Surface Phase Diagram Prediction Techniques Are Biased and Inefficient:Current approaches: 1.Construct a small and chemically-intuitive set of reconstructions Problem: This set of reconstructions is biased by human-selection and therefore is not guaranteed to include the most stable reconstruction in nature Reuter,K.;Scheffler,M.Phys.Rev.B.2001,65,035406.2.Randomly construct a large set of reconstructions Problem: The phase space of all possible reconstructions is infinite and therefore exhaustive exploration is inefficient Pickard,C.J.;Needs,R.J.Phys.Rev.Lett.2006,97,045504.Pickard,C.J.;Needs,R.J.J.Phys.: Condens.Matter.2011,23,053201.3.Use of metaheuristics or hyperspatial optimization for crystal structure prediction Problem: Unable to provide mechanistic information about the natural evolution of the surface Oganov,A.R.;Glass,C.W.J.Chem.Phys.2006,124,244704.Wang,Y.;Lv,J.;Zhu,L.;Ma,Y.Phys.Rev.B.2010,82,094116.Ulissi,Z.W.;Singh,A.R.;Tsai,C.;Norskov,J.K.J.Phys.Chem.Lett.2016,7 (19),3931.Pickard,C.J.Phys.Rev.B.2019,99,054102.