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Tuning magnetic properties in layered van der Waals (vdW) materials hascaptured a significant attention due to the efficient control of ground-statesby heterostructuring and external stimuli. Electron doping by electrostaticgating, interfacial charge transfer and intercalation is particularly effectivein manipulating the exchange and spin-orbit properties, resulting in a controlof Curie temperature ($T_{\text{C}}$) and magnetic anisotropy. Here, wediscover an uncharted role of intercalation to generate magnetic frustration.As a model study, we intercalate Na atoms into the vdW gaps of pristineCr$_2$Ge$_2$Te$_6$ (CGT) where generated magnetic frustration leads to emergingspin-glass states coexisting with a ferromagnetic order. A series of dynamicmagnetic susceptibility measurements/analysis confirms the formation ofmagnetic clusters representing slow dynamics with a distribution of relaxationtimes. The intercalation also modifies other macroscopic physical parametersincluding the significant enhancement of $T_{\text{C}}$ from 66\,K to 240\,Kand the switching of magnetic easy-hard axis direction. Our study identifiesintercalation as a unique route to generate emerging frustrated spin states insimple vdW crystals.

Spin-glass states generated in a van der Waals magnet by alkali-ion intercalation