Pb18O8Cl15I5: A Polar Lead Mixed Oxyhalide with Unprecedented Architecture and Excellent Infrared Nonlinear Optical Properties

Pb18O8Cl15I5: A Polar Lead Mixed Oxyhalide with Unprecedented Architecture and Excellent Infrared Nonlinear Optical Properties
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Pb18O8Cl15I5:一种极性铅混合卤氧化物,具有前所未有的结构和优异的红外非线性光学性能

DOI:
10.1002/anie.202009541
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发表时间:
2020-09-25
影响因子:
16.6
通讯作者:
Ok, Kang Min
Ok, Kang Min
中科院分区:
化学1区
文献类型:
--
作者:
Chen, Xinglong;Jing, Qun;Ok, Kang Min

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为了开发高性能红外非线性光学材料,我们采用合理的元素组成设计策略,研究了PbO-PbCl_2-PbI(2)体系。通过这样做,我们发现了一种新的极性铅混合卤氧化物,Pb 18 O 8 Cl 15 I5,第一个合成的金属卤氧化物结合Cl(-)和I-。Pb(18)O(8)Cl(15)I(5)显示出前所未有的结构特征,具有两种不同尺寸类型的氧心Pb-O单元,即[O 4Pb 8](8+)簇和[OPb 2](2+)链。在室温条件下成功地生长了厘米级Pb(18)O(8)Cl(15)I(5)单晶。值得注意的是,Pb(18)O(8)Cl(15)I(5)满足高性能IR NLO材料的所有基本但严格的标准,表现出最宽的IR透明度(高达16.0 μ m)、强的二次谐波产生响应(1.05 × AgGaS(2))、上级双折射(636 nm处为0.086)和高的激光诱导损伤阈值(8.5 × AgGaS(2))。
To develop high-performance nonlinear optical (NLO) materials for infrared (IR) applications, we have applied a rational element-composition design strategy and investigated the unexplored PbO-PbCl2-PbI(2)system. By doing so, we discovered a new polar lead mixed oxyhalide, Pb18O8Cl15I5, the first synthetic metal oxyhalide combining both Cl(-)and I-. Pb(18)O(8)Cl(15)I(5)reveals an unprecedented structural feature with two different dimensional types of oxocentered Pb-O units, namely, [O4Pb8](8+)clusters and [OPb2](2+)chains. Centimeter-sized single crystals of Pb(18)O(8)Cl(15)I(5)have been successfully grown under ambient conditions. Remarkably, Pb(18)O(8)Cl(15)I(5)satisfies all fundamental yet rigorous criteria for high-performance IR NLO materials, exhibiting the widest IR transparency (up to 16.0 mu m) among oxide-based crystals, strong second-harmonic generation response (1.05xAgGaS(2)), superior birefringence (0.086 at 636 nm), and a high laser-induced damage threshold (8.5xAgGaS(2)).