Structural Modulation of Nitrate Group with Cations to Affect SHG Responses in RE(OH)2NO3 (RE = La, Y, and Gd): New Polar Materials with Large NLO Effect after Adjusting pH Values of Reaction Systems

等结构 结晶学 空间组 离子半径 双折射 二次谐波产生 镧系元素 化学 氢氧化物 材料科学 热液循环 无机化学 群(周期表) 晶体结构 离子 衍射 X射线晶体学 光学 物理 有机化学 地震学 地质学 激光器
作者
Yunxia Song,Min Luo,Chensheng Lin,Ning Ye
出处
期刊:Chemistry of Materials [American Chemical Society]
卷期号:29 (2): 896-903 被引量:125
标识
DOI:10.1021/acs.chemmater.6b05119
摘要

A series of rare-earth hydroxide nitrate crystals (La(OH)2NO3, Y(OH)2NO3, and Gd(OH)2NO3) have been synthesized through adjusting pH values of reaction systems under the subcritical hydrothermal condition. All the titled compounds were isostructural with the noncentrosymmetric space group P21 (No. 4) with layer structure, containing [REO9] (RE = La,Y, and Gd) polyhedra in each layer. The polyhedra were stacked on top of each other and further connected with zigzag strings of edge sharing to form infinite corrugated sheets that parallel to the a–c plane. The [NO3] groups that presented two different orientation (A and B) project into the space between the layers. In this study, the angle θ between two different orientation [NO3] groups was defined. With the decrease of ionic radii from La3+, Gd3+ to Y3+, the θ was increased, which led to different second harmonic generation (SHG) effects on lanthanide hydroxide nitrates. The powder SHG measurements revealed that La(OH)2NO3, Gd(OH)2NO3, and Y(OH)2NO3 were phase-matchable in the visible and UV region and feature large SHG responsed that are approximately 5, 5.5, and 5.6 times that of KH2PO4 (KDP), respectively. Additionally, these title compounds had wide transparent regions from UV to near IR and larger birefringence, suggesting that these crystals were promising UV NLO materials. And their electronic structures and optical properties were calculated based on DFT methods.
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