| Summary: | The manipulation of valley splitting has potential applications in valleytronics, which lacks in pristine two-dimensional (2D) InSe. Here, we demonstrate that valley physics in InSe can be activated via the magnetic proximity effect exerted by ferromagnetic FeI<sub>2</sub> substrate with spin-orbit coupling. The valley splitting energy can reach 48 meV, corresponding to a magnetic exchange field of ~800 T. The system also presents magnetic anisotropy behavior with its easy magnetization axis tunable from in-plane to out-of-plane by the stacking configurations and biaxial tensile strain. The <i>d</i>-orbital-resolved magnetic anisotropic energy contributions indicate that the tensile strain effect arises from the increase of hybridization between minority Fe <i>d<sub>xy</sub></i> and <inline-formula><math display="inline"><semantics><mrow><msub><mi>d</mi><mrow><msup><mi>x</mi><mn>2</mn></msup><mo>−</mo><msup><mi>y</mi><mn>2</mn></msup></mrow></msub></mrow></semantics></math></inline-formula> states. Our results reveal that the magnetic proximity effect is an effective approach to stimulate the valley properties in InSe to extend its spintronic applications, which is expected to be feasible in other group-III monochalcogenides.
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