Engineering Magnetic Phases of Layered Antiferromagnets by Interfacial Charge Transfer.

Van der Waals heterostructures composed of distinct layered materials can display behaviors entirely different from those of each individual layer due to interfacial coupling. Here we investigate the manipulation of magnetic phases in two-dimensional magnets through interfacial charge transfer in heterostructures of magnetic and nonmagnetic layers. This is demonstrated by first-principles calculations, which unveil a transition toward the ferromagnetic phase by stacking antiferromagnetic bilayer CrSBr on graphene. Using an effective model consisting of two electronically coupled single layers, we show that the antiferromagnetic to ferromagnetic magnetic phase transition occurs due to interfacial charge transfer, which enhances ferromagnetism. We further reveal that the magnetic phase transition can also be induced by electron and hole carriers and demonstrate that the phase transition is a spin-canting process. This allows for precise gate-control of noncollinear magnetism on demand. Our work predicts interfacial charge transfer as a potent mechanism to tune magnetic phases in van der Waals heterostructures and creates opportunities for spintronic applications.