Abstract and subjects
Accelerating the search for functional materials is a challenging problem. Here we develop an informatics-guided ab initio approach to accelerate the design and discovery of noncentrosymmetric materials. The workflow integrates group theory, informatics and density-functional theory to uncover design guidelines for predicting noncentrosymmetric compounds, which we apply to layered Ruddlesden-Popper oxides. Group theory identifies how configurations of oxygen octahedral rotation patterns, ordered cation arrangements and their interplay break inversion symmetry, while informatics tools learn from available data to select candidate compositions that fulfil the group-theoretical postulates. Our key outcome is the identification of 242 compositions after screening similar to 3,200 that show potential for noncentrosymmetric structures, a 25-fold increase in the projected number of known noncentrosymmetric Ruddlesden-Popper oxides. We validate our predictions for 19 compounds using phonon calculations, among which 17 have noncentrosymmetric ground states including two potential multiferroics. Our approach enables rational design of materials with targeted crystal symmetries and functionalities.