Synergistic Control of Valley Splitting in WSeTe/VSeTe van der Waals Heterostructures via Magnetic Proximity Effect and Intrinsic Electric Polarization

Efficient manipulation of valley degree of freedom in two‐dimensional (2D) materials is crucial for developing next‐generation information devices. This work demonstrates a dual‐modulation strategy that integrates magnetic proximity effect with intrinsic electric polarization to significantly enhance valley splitting in Janus WSeTe/VSeTe heterostructures. First‐principles calculations reveal that the intrinsic electric polarization of ferromagnetic VSeTe promotes intralayer spin‐selective charge transfer and strengthens the interfacial atomic magnetic moments. As a result, a maximum valley splitting of 24 meV is achieved in WSeTe. Further reducing the interlayer spacing strengthens the coupling effect, ultimately realizing a remarkable valley splitting of 128 meV and an equivalent magnetic field of 1686 T. This study establishes a highly efficient multifield coupling approach for valley manipulation and provides a novel design perspective for 2D valleytronic devices.