Valleytronic devices show great promise for next-generation information technology, yet their practical development is limited by the lack of intrinsic ferrovalley materials. To address this issue, we propose an efficient bottom-up strategy to design high-performance two-dimensional (2D) ferrovalley materials, constructing a series of hexagonal metal–organic frameworks (MOFs) from trigonal bipyramidal TMCu4 magnetic clusters (TM = Ta, W, Os, Ir, Re) and organic linker C4H4P2. First principles calculations confirm that these 2D MOFs feature large magnetic anisotropy and robust spontaneous valley polarization. In particular, both freestanding and h-BN-supported Ir–W-based MOFs exhibit large Berry curvatures with opposite signs and distinct magnitudes at the K and K′ valleys. Furthermore, we demonstrate that the intrinsic valley polarization can be reversibly switched by external electric and magnetic fields, enabling potential applications in valleytronic devices.
Lian et al. (Tue,) studied this question.