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ABSTRACT 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 ₄₅₅^{ (2) }\ 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.
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