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Polar organic-inorganic hybrid materials have been applied in ferroelectricity, as well as in devices based on nonlinear optical and piezoelectricity properties. Here, we used a rectangular pyramid structure of [VOCl4]2- to construct a polar compound (C5NH13Cl)2VOCl4 (1). Compound 1 crystallized in the monoclinic P21 space group. Coexistence of nonlinear optical switching behavior (space-group change from P21 to P21/n) and two-staged thermosensitive dielectric switching properties could be achieved under the stimulus of temperature. Our
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