AMnAs3S6 (A = Cs, Rb): Phase-Matchable Infrared Nonlinear Optical Functional Motif [As3S6]3- Obtained via Surfactant-Thermal Method
AMnAs3S6 (A = Cs, Rb): Phase-Matchable Infrared Nonlinear Optical Functional Motif [As3S6]3- Obtained via Surfactant-Thermal Method
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AMnAs3S6 (A = Cs, Rb)：相位匹配的红外非线性光学功能基序 [As3S6]3 — 通过表面活性剂 — 热法获得
DOI：
10.1021/acsami.0c15812
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发表时间：
2020-12-02
影响因子：
9.5
通讯作者：
Guo, Guo-Cong
中科院分区：
文献类型：
--
作者：
Ye, Run;Liu, Bin-Wen;Guo, Guo-Cong
探索具有非线性光学活性的功能基元对于合理设计具有广阔应用前景的红外非线性光学材料具有重要意义。与典型的四面体MQ（4）（M = IIB，III，IV金属; Q = S，Se）基序相比，MQ（3）（M = As，Sb）金字塔结构有利于提高二次谐波产生（SHG）效率，但由于其光学各向异性过大，常常阻碍相位匹配（PM）。首次采用表面活化-热合成法在MQ（3）体系中实现了PM，合成了共价-离子混合型红外非线性光学材料。获得了两种新的硫代砷酸盐AMnAs（3）S（6）（A = Cs，Rb），它们具有与商用AGS相当的PM倍频效率和比AGS高一个数量级的激光损伤阈值。[As 3S 6]（3-）结构单元是一个前所未有的具有NLO活性的功能基元，这对设计具有高倍频效率的新型红外NLO化合物具有重要意义。此外，表面吸附-热合成方法为合成新型红外非线性光学材料提供了一种新的一般性策略。
Exploration of a new nonlinear optical (NLO)-active functional motif is important in the rational design of promising infrared (IR) NLO materials. Compared with typical tetrahedral MQ(4) (M = IIB, III, IV metals; Q = S, Se) motifs, MQ(3) (M = As, Sb) pyramids favor high second-harmonic generation (SHG) efficiency while frequently hindering phase matching (PM) because of excessively large optical anisotropy. The surfactant-thermal method was first adopted to achieve PM in MQ(3)-containing systems and synthesize mixed covalent-ionic IR NLO materials. Two new thioarsenates of AMnAs(3)S(6) (A = Cs, Rb) exhibiting strong PM SHG efficiencies comparable to commercial AGS and laser-induced damage thresholds of one order higher than AGS were obtained. The [As3S6](3-) unit in their structures is an unprecedented NLO-active functional motif; which can be useful in designing new IR NLO compounds with large SHG efficiency. In addition, the surfactant-thermal method provides a new general strategy for synthesizing new IR NLO materials.