2D AgVP2Se6 with Layer‐Independent and Strong In‐Plane Anisotropic Second Harmonic Generation

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Abstract Exploring 2D nonlinear optical (NLO) materials that exhibit layer‐independence and in‐plane anisotropy of second‐harmonic generation (SHG) is of great importance to the fundamental studies and further development of polarization‐sensitive optoelectronics. However, such exploration remains challenging because it requires the corresponding bulk materials to have broken inversion symmetry as well as low‐lattice symmetry. Here, it is shown that AgVP2Se6 can be a novel 2D NLO anisotropic material with the experimental demonstration of the layer‐irrelevant and in‐plane anisotropic NLO process. Nanoflakes of AgVP2Se6 are successfully prepared by mechanical exfoliation method. The thickness‐ and polarization‐dependent SHG measurement reveal that as‐exfoliated AgVP2Se6 nanoflakes exhibit layer‐independence and strong in‐plane anisotropy of SHG with the anisotropic factor up to 56.38. Moreover, temperature‐dependent Raman spectroscopy reveals that 2D AgVP2Se6 nanoflakes exhibit interlayer interactions stronger than that of graphene, which is helpful in reducing interlayer slip and detachment. These attributes make 2D AgVP2Se6 promising in polarization‐sensitive nanophotonic applications.

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