High-Throughput Search and Prediction of New Two-Dimensional 4f-Materials

The development of next-generation microelectronics, signal processing, and data storage systems calls for the discovery of new two-dimensional (2D) materials with novel electronic functionalities that can be miniaturized and monolithically integrated with silicon. f-electron systems promote a rich set of novel phases of matter that emerge from the intertwining and competition of spin–orbit coupling, electron–electron interactions, and the hybridization between itinerant and local electrons, however, very little attention has been devoted to exploring the 4f compounds for new promising 2D materials. To address this gap in the field we employ a high-throughput search leveraging an all-electron first-principles treatment to identify and predict the electronic properties of new 2D rare earth compounds. Applying our search to the major international materials databases yields ~300 candidate compounds from across the lanthanide series of elements, exhibiting a spectrum of lattice symmetries, electronic structure, and topological states. This study serves as a springboard to further systematic theoretical investigation of correlation driven properties of the 4f and other 2D materials composed of heavy elements.