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A Hybrid Antiperovskite with Strong Linear and Second‐Order Nonlinear Optical Responses

Von Wiley-VCH zur Verfügung gestellt

Hybrid halide antiperovskite Cs3Cl(HC3N3S3) could not only double the frequency of incident ray with very strong SHG response but also divide an incident ray into polarized o ray and e ray with exceptionally large birefringence.


Abstract

Antiperovskites have been studied since the 1980s because of their rich physical and chemical properties, but their linear and second-order nonlinear optical responses remain largely unknown. Here we report a new polar crystal, Cs3Cl(HC3N3S3) (I), which features a quasi-one-dimensional antiperovskite structure composed of ClCs6 polyhedra and A-site [HC3N3S3]2− rings. To our best knowledge, this kind of antiperovskite structure is reported for the first time. Remarkably, I exhibits a very strong nonlinear optical response up to 11.4 times that of the benchmark KH2PO4 and exceptionally large birefringence of 0.52. The first-principles calculations and structural analyses reveal that [HC3N3S3]2− is the “material gene” while the antiperovskite structural feature making it in a favorable arrangement. This work provides a new structural platform for the rational design of integrated optoelectronic materials with linear and second-order nonlinear optical responses.

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