Selective Amplification of the Topological Hall Signal in Cr ₂ Te ₃ : The Role of Molecular Exchange Coupling

Layered magnetic transition-metal chalcogenides (TMCs) are a focal point of research, revealing a variety of intriguing magnetic and topological ground states. Within this family of TMCs, chromium telluride has garnered significant attention because of its excellent tunability in magnetic response, owing to the presence of competing magnetic exchange interactions. We here demonstrate the manipulation of magnetic anisotropy in ultrathin Cr 2 Te 3 films through growth engineering leading to a controlled transition from in-plane to out-of-plane orientation with an intermediate noncoplanar magnetic ground phase characterized by a topological Hall effect. Moreover, interfacing these films with vanadyl phthalocyanine (VOPc) molecules prominently enhances the noncoplanar magnetic phase, attributing its presence to the competing interfacial magnetic exchange interactions over the spin–orbit-driven interfacial effects. These findings pave the way for the realization of novel topological spintronic devices through interface-modulated exchange coupling.