AgGa2PS6: A New Mid-Infrared Nonlinear Optical Material with a High Laser Damage Threshold and a Large Second Harmonic Generation Response
AgGa2PS6: A New Mid-Infrared Nonlinear Optical Material with a High Laser Damage Threshold and a Large Second Harmonic Generation Response
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AgGa2PS6：一种新型中红外非线性光学材料，具有高激光损伤阈值和大二次谐波产生响应
DOI：
10.1002/chem.201702632
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发表时间：
2017
影响因子：
4.3
通讯作者：
Mao Jiang-Gao
中科院分区：
文献类型：
--
作者：
Feng Jiang-He;Hu Chun-Li;Xu Xiang;Li Bing-Xuan;Zhang Ming-Jian;Mao Jiang-Gao
开发新型中红外（MIR）非线性光学（NLO）材料，克服商用MIR-NLO晶体（AgGaS 2、AgGaSe 2和ZnGeP 2）的低激光损伤阈值（LDT），同时保持较大的NLO极化率，是高功率MIR激光频率转换技术的必要条件。为了改善LDT，采用了增加晶格稳定性的新策略。在AgGaS 2（AGS）中引入了PS4四面体的强共价结构单元，从而分离出AgI-GaIII-PV-S体系中的第一个化合物AgGa 2 PS 6（Cc）。AgGa 2 PS 6晶体具有较高的倍频效率（1.0×AGS）和相位匹配能力，同时还具有较好的LDT（5.1×AGS），是一种很有前途的MIR-NLO晶体。此外，在AgGa 2 PS 6中发现了一种新的[Ga 2 PS 6]−三维框架，具有三角形通道，以及有趣的AgS 3单一三角形几何结构-这两种结构在已报道的硫化物中非常罕见。此外，理论计算，晶格能和热膨胀分析表明，PS4基团作出了很大的贡献，大的SHG效率和高的LDT。
To develop new mid‐infrared (MIR) nonlinear optical (NLO) materials, which can overcome the low laser damage threshold (LDT) of the commercial MIR‐NLO crystals (AgGaS2, AgGaSe2and ZnGeP2) and simultaneously keep the large NLO susceptibility, is necessary for high‐power MIR laser frequency conversion technology. To improve the LDT, a new strategy of increasing lattice stability was adopted. Here, the strongly covalent structural unit of the PS4tetrahedron was introduced into AgGaS2(AGS), and that led to the isolation of the first compound in AgI‐GaIII‐PV‐S system, namely, AgGa2PS6(Cc). It retains a large SHG efficiency (1.0×AGS) with phase‐matchable ability, and also exhibits an improved LDT (5.1×AGS), indicating AgGa2PS6is a new promising MIR‐NLO crystal. Moreover, a novel 3D framework of [Ga2PS6]−, with triangular‐shaped channels, as well as interesting single triangular geometry of AgS3—both of which are very rare in reported sulfides—was discovered in AgGa2PS6. Furthermore, theoretical calculations, and lattice energy and thermal expansions analyses suggest that the PS4group makes a large contribution to the large SHG efficiency and high LDT.