Emergent Spin Fluctuation and Structural Metastability in Self‐Intercalated Cr1+xTe2${\rm Cr}_{1+x}{\rm Te}_2$ Compounds

ABSTRACT Intercalated van der Waals (vdW) magnetic materials host unique magnetic properties due to the interplay of competing interlayer and intralayer exchange couplings, which depend on the intercalant concentration within the van der Waals gaps. Magnetic vdW compound chromium telluride, , has demonstrated rich magnetic phases at various Cr concentrations, such as the coexistence of ferromagnetic and antiferromagnetic phases in (equivalently, ). The compound is created by intercalating 0.25 Cr atom per unit cell within the van der Waals gaps of . In this work, we report a notably increased Curie Temperature and an emergent in‐plane spin fluctuation by slightly reducing the concentration of Cr intercalants in . Moreover, the intercalated Cr atoms form a metastable 22 supercell structure that can be manipulated by electron beam irradiation. This work offers a promising approach to tuning magnetic and structural properties by adjusting the concentration of intercalated magnetic atoms.