The question of material stability is of fundamental importance to any analysis of system properties in condensed matter physics and materials science.The ability to evaluate chemical stability,i.e.,whether a stoichio...The question of material stability is of fundamental importance to any analysis of system properties in condensed matter physics and materials science.The ability to evaluate chemical stability,i.e.,whether a stoichiometry will persist in some chemical environment,and structure selection,i.e.what crystal structure a stoichiometry will adopt,is critical to the prediction of materials synthesis,reactivity and properties.Here,we demonstrate that density functional theory,with the recently developed strongly constrained and appropriately normed(SCAN)functional,has advanced to a point where both facets of the stability problem can be reliably and efficiently predicted for main group compounds,while transition metal compounds are improved but remain a challenge.SCAN therefore offers a robust model for a significant portion of the periodic table,presenting an opportunity for the development of novel materials and the study of fine phase transformations even in largely unexplored systems with little to no experimental data.展开更多
Disordered multicomponent systems attract great interest due to their engineering design flexibility and subsequent rich space of properties.However,detailed characterization of the structure and atomic correlations r...Disordered multicomponent systems attract great interest due to their engineering design flexibility and subsequent rich space of properties.However,detailed characterization of the structure and atomic correlations remains challenging and hinders full navigation of these complex spaces.A lattice cluster expansion is one tool to obtain configurational and energetic resolution.While in theory a cluster expansion can be applied to any system of any dimensionality,the method has primarily been used in binary systems or ternary alloys.Here we apply cluster expansions in high-component ionic systems,setting up the largest cluster expansion ever attempted to our knowledge.In doing so,we address and discuss challenges specific to high-component ionic systems,namely charge state assignments,structural relaxations,and rank-deficient systems.We introduce practical procedures to make the fitting and analysis of complex systems tractable,providing guidance for future computational studies of disordered ionic systems.展开更多
基金Y.Z.,H.P.,J.P.P.and J.S.acknowledge the support from the Center for the Computational Design of Functional Layered Materials,an Energy Frontier Research Center funded by the US Department of Energy(DOE),Office of Science,Basic Energy Sciences(BES),under award No.DE-SC0012575.
文摘The question of material stability is of fundamental importance to any analysis of system properties in condensed matter physics and materials science.The ability to evaluate chemical stability,i.e.,whether a stoichiometry will persist in some chemical environment,and structure selection,i.e.what crystal structure a stoichiometry will adopt,is critical to the prediction of materials synthesis,reactivity and properties.Here,we demonstrate that density functional theory,with the recently developed strongly constrained and appropriately normed(SCAN)functional,has advanced to a point where both facets of the stability problem can be reliably and efficiently predicted for main group compounds,while transition metal compounds are improved but remain a challenge.SCAN therefore offers a robust model for a significant portion of the periodic table,presenting an opportunity for the development of novel materials and the study of fine phase transformations even in largely unexplored systems with little to no experimental data.
基金The project was primarily funded by the U.S.Department of Energy,Office of Science,Office of Basic Energy Sciences,Materials Sciences and Engineering Division under Contract No.DE-AC02-05-CH11231(Materials Project program KC23MP)This work was also supported by the Energy Efficiency and Renewable Energy,Vehicle Technologies Office,under the Applied Battery Materials Program,of the U.S.Department of Energy under Contract No.DE-AC02-05CH11231L.B.L and Z.J.gratefully acknowledge financial support from the NSF Graduate Research Fellowship Program(GRFP)under contract no.1752814。
文摘Disordered multicomponent systems attract great interest due to their engineering design flexibility and subsequent rich space of properties.However,detailed characterization of the structure and atomic correlations remains challenging and hinders full navigation of these complex spaces.A lattice cluster expansion is one tool to obtain configurational and energetic resolution.While in theory a cluster expansion can be applied to any system of any dimensionality,the method has primarily been used in binary systems or ternary alloys.Here we apply cluster expansions in high-component ionic systems,setting up the largest cluster expansion ever attempted to our knowledge.In doing so,we address and discuss challenges specific to high-component ionic systems,namely charge state assignments,structural relaxations,and rank-deficient systems.We introduce practical procedures to make the fitting and analysis of complex systems tractable,providing guidance for future computational studies of disordered ionic systems.
