Hypotaxial growth of single-crystalline 2D antiferromagnetic Cr₂Se₃ with stoichiometric composition

Abstract

Chanyeol Park, Donghoon Moon, Jimin Jang, Changgu Lee, Gwan-Hyoung Lee

Recent progress in two-dimensional (2D) magnetism has intensified the search for scalable synthesis of van der Waals antiferromagnets, yet their large-area growth via chemical vapor deposition (CVD) remains a challenge due to phase instability and interface engineering complexities. Here, we report the successful large-area synthesis of high-quality single-crystalline Cr₂Se₃ thin films through a hypotaxial growth strategy. By selenizing a Cr film covered with monolayer graphene, Cr₂Se₃ grows hypotaxially by following the crystallographic orientation of the graphene, resulting in a highly aligned single-crystalline film. By controlling the thickness of the pre-deposited Cr layer on the substrate, we achieve Cr₂Se₃ films with tunable thickness, enabling systematic investigation of thickness-dependent antiferromagnetic properties. The hypotaxially grown Cr₂Se₃ films exhibit antiferromagnetic ordering with pronounced magnetic anisotropy, offering a compelling platform for 2D antiferromagnetic spintronics. Our results not only overcome long-standing limitations in the scalable synthesis of 2D antiferromagnets but also pave the way for their integration into future spin-based electronic and memory devices.