Rare-earth Bilayer Triangular Lattice as a Platform for Tunable Ground States and Field-induced Magnetic Phases

Abstract: Rare-earth bilayer triangular lattice (TL) antiferromagnets provide a versatile platform for realizing diverse magnetic states by combining geometric frustration, interlayer coupling, and strong single-ion anisotropy. Here, we report a family of R2O2Se (R = Sm, Eu, Tb-Lu; ROSe) single crystals featuring bilayer equilateral TLs. Magnetic susceptibility and specific-heat measurements reveal predominantly antiferromagnetic (AFM) interactions and diverse magnetic ground states across the series, including successive AFM transitions in TbOSe and single AFM transitions in SmOSe, DyOSe, HoOSe, and YbOSe. Notably, DyOSe and HoOSe exhibit pronounced 1/2 magnetization plateau-like features for fields along the c-axis, revealing field-induced magnetic states. In HoOSe, complementary thermodynamic and magnetization measurements resolve three critical fields and a rich field-temperature phase diagram containing five distinct magnetic phases. These results establish rare-earth bilayer TLs as a chemically tunable materials platform for accessing novel quantum spin states through the interplay of lattice geometry, single-ion anisotropy, and competing magnetic interactions.