High-Throughput Search of Layered 4f-Materials

The development of multifunctional devices calls for the discovery of new layered materials with novel electronic properties. f-electron systems naturally host a rich set of competing and intertwining phases owning to the presence of strong spin-orbit coupling, electron-electron interactions, and hybridization between itinerant and local electrons. However, very little attention has been devoted to exploring the f-electron family of compounds for new promising layered material candidates. Here, we identify 295 rare earth compounds from across the lanthanide series of elements that exhibit a spectrum of chemical composition, crystal structures, and electronic properties. While most of the layered materials studied in the last ten years belong to the hexagonal or Kagome crystal systems, these structures represent only a minority of the 295 layered 4f compounds. Moreover, we find metallic and insulating systems with band gaps covering a 0.1 eV to 5.3 eV range which opens new possibilities in infrared quantum sensors, designer photocatalysts, and tunable transistors. The inclusion of 4f-states in a layered system also suggests the possibility of 2D confined heavy-fermion superconductivity and topological semimetals. Our 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.