Non-centrosymmetric (NCS) and polar materials capable of exhibiting many important functional properties are indispensable for electro-optical technologies, yet their rational structural design remains a significant challenge. Here, we report a "group grafting" strategy for designing the first multi-chromophore selenophosphate, CsIn(InSe)(PSe), that crystallizes in a NCS and polar space group of Cm. The structure features a unique basic building unit (BBU) [In(InSe)(PSe)], formed through "grafting [InSe] supertetrahedra on the root of [In(PSe)] groups". Theoretical calculations confirm that this [In(InSe)(PSe)] BBU can achieve a "1+1>2" combination of properties from two chromophores, [InSe] supertetrahedron and ethane-like [PSe] dimer. That makes CsIn(InSe)(PSe) exhibit excellent linear and nonlinear optical (NLO) properties, including a strong second harmonic generation (SHG) response (~6×AgGaS), a large band gap (2.45 eV), broad infrared (IR) transmission (up to 19.5 μm), a significant birefringence (0.26 @1064 nm) as well as the congruently-melting property at ~700 °C. Therefore, CsIn(InSe)(PSe) will be a promising NLO crystal, especially in the IR region, and this research also demonstrates that "group grafting" will be an effective strategy for constructing novel polar BBUs with multi-chromophore to design NCS structures and high-performance IR NLO materials.
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