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The authors synthesized and characterized a series of rare-earth bilayer equilateral triangular-lattice single crystals, $R_2\text{O}_2\text{Se}$ ($R = \text{Sm, Eu, Tb–Lu}$), to investigate how geometric frustration, interlayer coupling, and strong single-ion anisotropy govern magnetic ground states. Magnetic susceptibility and specific-heat measurements reveal predominantly antiferromagnetic interactions across the family, highlighted by pronounced $1/2$ magnetization plateaus in $\text{DyOSe}$ and $\text{HoOSe}$ under $c$-axis fields. In $\text{HoOSe}$, resolving three critical fields mapped out a rich field-temperature phase diagram containing five distinct magnetic phases, establishing these materials as a chemically tunable playground for exotic spin textures.
Geometric frustration in rare-earth bilayers unlocks field-induced $1/2$ magnetization plateaus and a five-phase magnetic landscape in $\text{HoOSe}$, proving that chemical tuning can cleanly switch between complex quantum spin states.
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.