Dual-Switch Control of a Layer-Locked Anomalous Valley Hall Effect in a Sliding Ferroelectric Antiferromagnet

Abstract: The integration of ferroelectric (FE) and antiferromagnetic (AFM) orders in twodimensional (2D) materials provides a promising avenue for the nonvolatile control of coupled spin and valley degrees of freedom, a capability central to advancing spinvalleytronics. However, realizing a single material system where these quantum states can be independently and reversibly manipulated by distinct stimuli, a prerequisite for multifunctional devices, has remained elusive. Here, we demonstrate a dual-switch mechanism in bilayer VS2, a room-temperature FE-AFM system, that enables electrical and magnetic control of a layer-locked anomalous valley Hall effect (AVHE). First-principles calculations reveal that interlayer sliding breaks spatial inversion symmetry, inducing a switchable out-of-plane FE polarization that coexists with interlayer AFM. The spin-orbit coupled valley polarization can be reversibly switched either by FE polarization reversal or by a magnetic-field-induced spin-flip transition, confirming the existence of electrically and magnetically addressable valley states. The Berry curvature exhibits both valley-contrasting and layer-locked characteristics, which underpin a switchable Hall response. Notably, electric and magnetic switching are functionally equivalent in modulating valley, layer, and spin indices, revealing strong magnetoelectric coupling. This work establishes a multidegree-of-freedom operational paradigm in 2D multiferroics and opens a viable design pathway toward multi-state memory and spin-valleytronic logic devices.