Na2Ge2Se5: A highly nonlinear optical material

Na2Ge2Se5: A highly nonlinear optical material
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DOI:
10.1016/j.jssc.2012.05.038
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发表时间:
2012-11-01
影响因子:
3.3
通讯作者:
Kanatzidis, Mercouri G.
Kanatzidis, Mercouri G.
中科院分区:
化学3区
文献类型:
--
作者:
Chung, In;Song, Jung-Hwan;Kanatzidis, Mercouri G.

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我们报告了一个综合的实验和理论研究的二维极性硒锗酸盐化合物Na 2Ge 2Se 5,它具有很强的非线性光学(NLO)的二次谐波产生响应在可见光和红外区域。该化合物是I型相位匹配的,具有接近5290 pm V-1的大的SHG系数chi((2)),这在相位匹配的NLO材料中是第二高的。它还可以作为NLO混频器,通过差频产生辐射。该化合物从可见光(0.521 μ m)到远红外(18.2 μ m)是光学透明的,并且全等熔融。从头算密度泛函理论能带结构计算表明,异常大的二阶光学非线性归因于晶体结构的二维特征。报道了Na_2Ge_2Se_(4.55)Te_(0.45)和Na_2Ge_(1.64)Sn_(0.36)Se_(5)衍生物的拉曼光谱、红外光谱、光学吸收光谱、差热分析、非线性光学性质以及热膨胀行为的研究。(C)2012 Elsevier Inc. All rights reserved.
We report an integrated experimental and theoretical study of the two-dimensional polar selenogermanate compound Na2Ge2Se5, which exhibits strong nonlinear optical (NLO) second harmonic generation response in the visible and infrared region. The compound is type-I phase-matchable with a large SHG coefficient chi((2))approximate to 5290 pm V-1, which is the second highest among the phase-matchable NLO materials. It also performs as an NLO frequency mixer to produce radiation via difference frequency generation. The compound is optically transparent from the visible (0.521 mu m) to the far IR (18.2 mu m) and melts congruently. Ab initio density functional theory band structure calculations show that the unusually large second-order optical nonlinearity is attributed to the two-dimensional character of the crystal structure. Raman, IR and optical absorption spectroscopy, differential thermal analysis, NLO properties of derivatives of Na2Ge2Se4.55Te0.45 and Na2Ge1.64Sn0.36Se5 and thermal expansion behavior studies are also reported. (C) 2012 Elsevier Inc. All rights reserved.