bandgap, atomic layer feature, and anisotropic/isotropic character, rendering them promising candidate for electronic and optoelectronic applications beyond the scaling limit. [1,2] Transition metal dichalcogenides (TMDs), as the most investigated 2D semiconductors, exhibit a direct-indirect bandgap transition, rich excitonic states, and valley-spin degree of freedom, however, their device performance is significantly impeded by low carrier mobility and weak light absorption. [1,[3][4][5][6] Indium selenide (InSe), as a representative member of III-VI family, has been demonstrated advantages over TMDs for high-performance opto-/electronic applications, including field effect transistors, phototransistors, tunneling, and high-speed devices. [7][8][9][10][11] InSe retains high carrier mobility up to 10 4 cm 2 V −1 s −1 even down to a few-layer limit. [9] Moreover, it exhibits a direct bandgap character from bulk to few-layer, which locates in the infrared regime, bridging the optical gap between TMDs and other narrow-bandgap 2D semiconductors, e.g., black phosphorous and AsP. [11,12] Different from the case of TMDs, the absorption of which is attributed to their in-plane dipole contribution, the light absorption of InSe is mainly determined by its out-of-plane
Introduction2D semiconductors have attracted much attention due to their unique structures and electronic properties, such as well-defined