3 years ago

Coexistence of Strong Second Harmonic Generation Response and Wide Band Gap in AZn4Ga5S12 (A=K, Rb, Cs) with 3D Diamond-like Frameworks

Coexistence of Strong Second Harmonic Generation Response and Wide Band Gap in AZn4Ga5S12 (A=K, Rb, Cs) with 3D Diamond-like Frameworks
Li-Ming Wu, Ju-Song Yu, Xin-Tao Wu, Yu-Jun Zheng, Hong Chen, Hua Lin
Mid-infrared (MIR, 2–20 μm) second-order nonlinear optical (NLO) materials with outstanding performances are of great importance in laser science and technology. However, the enormous challenge to design and synthesize an excellent MIR NLO material lies in achieving simultaneously a strong second harmonic generation (SHG) response [dij >0.6 × AgGaS2 (AGS)] and wide band gap (Eg>3.5 eV). Herein three new MIR NLO materials, AZn4Ga5S12 (A=K, Rb, Cs) are reported, which crystallize in the KCd4Ga5S12-type structure and adopt a 3D diamond-like framework (DLF) consisting of MS4 (M=Zn/Ga) tetrahedra; achieving the desired balance with strong powder SHG response (1.2–1.4 × AGS) and wide band gap (Eg≈3.65 eV). Moreover, they also show large laser induced damage thresholds (LIDTs, 36 × AGS), a wide range of optical transparency (0.4–25 μm) and ultrahigh thermal stability (up to 1400 K). Upon analyzing the structure-property relationship of AXII4XIII5Q12 family, these 3D DLF structures can be used as a highly versatile and tunable platform for designing excellent MIR NLO materials. Trick of the light: Three new mid-infrared nonlinear optical sulfides, AZn4Ga5S12 (A=K, Rb, Cs), adopt a 3D diamond-like framework (DLF) structure, and achieve the desired balance with strong powder second harmonic generation response (1.2–1.4 × AgGaS2) and wide band gap (Eg≈3.65 eV).

Publisher URL: http://onlinelibrary.wiley.com/resolve/doi

DOI: 10.1002/chem.201701679

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