Partial Isovalent Anion Substitution to Access Remarkable Second-Harmonic Generation Response: A Generic and Effective Strategy for Design of Infrared Nonlinear Optical Materials,Chemistry of Materials

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Partial Isovalent Anion Substitution to Access Remarkable Second-Harmonic Generation Response: A Generic and Effective Strategy for Design of Infrared Nonlinear Optical Materials
Chemistry of Materials ( IF 7.2 ) Pub Date : 2020-06-04 , DOI: 10.1021/acs.chemmater.0c02011
Mao-Yin Ran _{1,

2} , Zuju Ma ₃ , Hong Chen ₁ , Bingxuan Li ₄ , Xin-Tao Wu ₁ , Hua Lin ₁ , Qi-Long Zhu ₁

Affiliation

Nonlinear optical (NLO) materials have received unprecedented attention owing to their capability of frequency conversion in the photoelectric fields. Yet, how to acquire a crystal with a noncentrosymmetric (NCS) structure is still a grand challenge for the NLO material. Herein, a new quaternary NCS oxychalcogenide, SrGeOSe₂, was successfully designed and synthesized using the known centrosymmetric SrGeO₃ as a maternal structure through a generic partial isovalent anion substitution (PIAS) strategy. SrGeOSe₂ belongs to the NCS space group P2₁2₁2₁ (no.19) and features a one-dimensional (1D) chain made by heteroligand [GeO₂Se₂] asymmetric building units. Such a new compound exhibits desirable comprehensive performance, which suggests a promising IR-NLO material: type-I phase-matching feature, strong powder second-harmonic generation intensity (d_ij = 1.3 × commercial AgGaS₂), and giant powder laser-induced damage threshold (36 × commercial AgGaS₂). Furthermore, the systematic theoretical investigations have been performed for the deep understanding of the correlation between the NCS structure and the NLO property. More importantly, this work pioneers a new molecular engineering strategy for NCS compounds that could be extended to other NLO materials.

中文翻译：

部分等价阴离子取代获得显着的二次谐波产生响应：红外非线性光学材料设计的通用有效策略

非线性光学（NLO）材料由于其在光电领域的频率转换能力而受到了前所未有的关注。然而，如何获得具有非中心对称（NCS）结构的晶体仍然是NLO材料面临的巨大挑战。本文中，通过通用的部分等价阴离子取代（PIAS）策略，使用已知的中心对称SrGeO ₃作为母体结构，成功设计并合成了新的四元NCS氧硫族化物SrGeOSe ₂。SrGeOSe ₂属于NCS空间群P 2 ₁ 2 ₁ 2 ₁（第19号），具有由杂配体[GeO ₂ Se构成的一维（1D）链。₂ ]不对称的建筑单元。这种新化合物表现出令人满意的综合性能，这表明有希望的IR-NLO材料：I型相匹配特征，强大的粉末二次谐波产生强度（d _ij = 1.3×商业AgGaS ₂）和巨大的激光诱导激光粉末损伤阈值（36×商业AgGaS ₂）。此外，已经进行了系统的理论研究，以加深对NCS结构和NLO性质之间相关性的了解。更重要的是，这项工作开创了NCS化合物新的分子工程策略，该策略可以扩展到其他NLO材料。

更新日期：2020-07-14

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