Multidirectional Sliding Ferroelectricity of Rhombohedral‐Stacked InSe for Reconfigurable Photovoltaics and Imaging Applications

Abstract Through the stacking technique of 2D materials, the interfacial polarization can be switched by an interlayer sliding, known as sliding ferroelectricity, which is advantageous in ultra‐thin thickness, high switching speed, and high fatigue resistance. However, uncovering the relationship between the sliding path and the polarization state in rhombohedral‐stacked materials remains a challenge, which is the key to 2D sliding ferroelectricity. Here, layer‐dependent multidirectional sliding ferroelectricity in rhombohedral‐stacked InSe (γ‐InSe) is reported via dual‐frequency resonance tracking piezoresponse force microscopy and conductive atomic force microscopy. The graphene/γ‐InSe/graphene tunneling device exhibits a tunable bulk photovoltaic effect with a photovoltaic current density of ≈15 mA cm⁻² due to multiple polarization states. The generation of dome‐like domain walls is observed experimentally, which is attributed to the multidirectional sliding‐induced domains based on the theoretical calculations. Furthermore, the ferroelectric polarization in γ‐InSe ensures that the tunneling device has a high photo responsivity of ≈255 A W⁻¹ and a fast response time for real‐time imaging. The work not only provides insights into the multidirectional sliding ferroelectricity of rhombohedral‐stacked 2D materials but also highlights their potential for tunable photovoltaics and imaging applications.