期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 142, 期 24, 页码 10641-10645出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.0c04738
关键词
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资金
- NSF of China [21921001, 21827813, 21701176]
- strategic priority research program of the CAS [XDB20010100, YJKYYQ20180006]
- NSF of Fujian province [2018J05034]
Noncentrosymmetry (NCS) is a prerequisite for second-order nonlinear optical (NLO) materials. In this work, a new polycation-substitution-induced centrosymmetry (CS)-to-NCS transformation strategy was applied in CS RbGaS2, affording two novel NCS salt-inclusion chalcogenides: [ABa(2)Cl][Ga4S8] (A = Rb, 1; Cs, 2). Remarkably, they exhibit the key merits of both Vis and IR NLO candidates, including strong phase-matchable second harmonic generation intensities (10.4-15.3 x KH2PO4 at 1064 nm; 0.9-1.0 x AgGaS2 at 1910 nm), high laser-induced damage thresholds (11-12 x AgGaS2), and a wide transparent window. Their prominent NLO performances originate from the orderly packing of T2-supertetrahedral Ga4S10 motifs resulting from the template effect of acentric polycation [ClA(2)Ba(3)](7+). The CS-to-NCS transformation first realized by polycation-substitution-induced NLO-functional motif ordering provides an effective approach for designing new NLO materials.
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