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    Title: A3BBi(P2O7)2 (A = Rb, Cs;B = Pb, Ba): Isovalent Cation Substitution to Sustain Large Second-Harmonic Generation Responses
    Authors: Qi, Lu;Chen, Zhaohui;Shi, Xuerui;Zhang, Xiaodong;Jing, Qun;Li, Na;Jiang, Zhongqi;Zhang, Bingbing;Lee, Ming-Hsien
    Date: 2020-10-13
    Issue Date: 2021-05-07 12:10:31 (UTC+8)
    Abstract: Exploring novel photoelectric functional materials via chemical substitution-oriented design is an effective strategy, which can be expanded to the discovery of high-performance UV nonlinear optical (NLO) materials. Two new NLO pyrophosphates, Rb3BaBi(P2O7)2 (I) and Cs3BaBi(P2O7)2 (II), are rationally developed by a cation substitution technique based on A3PbBi(P2O7)2 (A = Rb and Cs), of which I inherits the large second-harmonic generation (SHG) response (exptl 2.5 × KDP; calcd 2.9 × KDP) and moderate birefringence (0.025@1064 nm) accompanied by a broadened UV transparent region. Compounds I and II are isomeric and exhibit different Ba–P–O frameworks. Especially, I possesses a large SHG effect benefiting from the favorable pentagonal-net topological structure. Detailed theory calculations elucidate the origin of the linear and nonlinear optical properties of the compounds. The insights obtained from the atomic-level module adjustment involving lone-pair-active optical anisotropy are useful for designing more efficient UV NLO materials.
    Relation: Chemistry of Materials 32(19), p.8713-8723
    DOI: 10.1021/acs.chemmater.0c03383
    Appears in Collections:[Graduate Institute & Department of Physics] Journal Article

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