Designing a 2D van der Waals oxide with lone-pair electrons as chemical scissor

Two-dimensional (2D) van der Waals (vdW) materials are known for their intriguing physical properties, but their rational design and synthesis remain a great challenge for chemists. In this work, we successfully synthesized a new non-centrosymmetric oxide, i.e. InSbMoO₆, with Sb³⁺ lone-pair electrons serving as chemical scissor to generate its 2D vdW crystal structure. Monolayer and few-layer InSbMoO₆ flakes are readily obtained via facile mechanical exfoliation. They exhibit strong second-harmonic generation (SHG) response with an effective second-order nonlinear optical susceptibility [Formula: see text]of 32.4 pm·V^-1. Meanwhile, the SHG response is in-plane anisotropic and directly proportional to the layer thickness, independent of layer parity. In addition, the InSbMoO₆ flakes exhibit excellent thermal and atmospheric stability, along with pronounced anisotropy in Raman spectroscopy. This work implies that using lone-pair electrons as chemical scissor is an effective strategy for designing and synthesizing new 2D vdW materials for integrated photonic applications.