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

作者：Mao‐Yin Ran, Zuju Ma, Hong Chen, Bingxuan Li, Xintao Wu, Hua Lin, Qi‐Long Zhu · 发表于：Chemistry of Materials · 年份：2020 · DOI：10.1021/acs.chemmater.0c02011 · 被引用次数：113 · 研究领域：Crystal Structures and Properties、Nonlinear Optical Materials Research、Photorefractive and Nonlinear Optics

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, SrGeOSe 2, was successfully designed and synthesized using the known centrosymmetric SrGeO 3 as a maternal structure through a generic partial isovalent anion substitution (PIAS) strategy. SrGeOSe 2 belongs to the NCS space group P 2 1 2 1 2 1 (no.19) and features a one-dimensional (1D) chain made by heteroligand [GeO 2 Se 2 ] 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 AgGaS 2 ), and giant powder laser-induced damage threshold (36 × commercial AgGaS 2 ). 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.