“…Nonlinear optical (NLO) materials are critical to the development of advanced photonic technologies such as laser optics, all-optical devices, signal processing, higher harmonics, and terahertz generation. , Two-dimensional (2D) materials have magical structures that lead to their unique electronic, optical, and mechanical properties, satisfying the growing demands for small size, strong response, high efficiency, compactness, and broadband in NLO materials. , Graphene, the pioneer of 2D material, has been extensively studied as an NLO material for various photonic devices. , Subsequently, a series of 2D materials in the phase of metallic and semiconductor, such as topological insulators (e.g., Bi 2 Se 3 , Sb 2 Te 3 , and Bi 2 Te 3 ), transition metal dichalcogenides (e.g., MoS 2 and WS 2 ), and black phosphorus (BP), have been demonstrated to exhibit fascinating NLO characteristics …”