Spin Glass Behavior in Amorphous CrSiTe₃ Alloy

Owing to the intrinsically high crystallization temperatures, layered phase‐change materials, such as CrGeTe 3 and InGeTe 3 , are attracting attention for embedded memory applications. In addition to the electrical contrast, a major change in magnetic properties is observed in CrGeTe 3 upon switching from the crystalline to the amorphous state. Herein, a combined ab initio modeling and magnetic characterization study on the isostructural silicon parent compound of CrGeTe 3 , namely, CrSiTe 3 , are reported . Amorphous CrSiTe 3 has similar structural properties to amorphous CrGeTe 3 ; however, it shows a smaller energy difference between the ferromagnetic configuration and the random magnetic configuration, indicating a high probability of spin glass formation. Indeed, direct‐current and alternating‐current magnetic measurements show that the coercive force of amorphous CrSiTe 3 is higher than that of amorphous CrGeTe 3 . Therefore, the pinning effect of spins is enhanced in amorphous CrSiTe 3 , leading to a more robust spin glass state with a higher freezing temperature. The large magnetic contrast between the amorphous and crystalline phase could make CrSiTe 3 a potential candidate for phase‐change magnetic switching applications.