二次谐波产生
电介质
分子开关
混合材料
非线性光学
化学物理
化学
光谱学
材料科学
相变
光电子学
纳米技术
光学
分子
激光器
凝聚态物理
物理
有机化学
量子力学
作者
Ying Zeng,Chun‐Li Hu,Weijian Xu,Tengwu Zeng,Zhenke Zhu,Xiao‐Xian Chen,De‐Xuan Liu,Yujie Chen,Yue‐Biao Zhang,Wei‐Xiong Zhang,Xiaoming Chen
标识
DOI:10.1002/anie.202110082
摘要
Switching materials in channels of nonlinear optics (NLOs) are of particular interest in NLO material science. Numerous crystalline NLO switches based on structural phase transition have emerged, but most of them reveal a single-step switch between two different second-harmonic-generation (SHG) states, and only very rare cases involve three or more SHG states. Herein, we report a new organic-inorganic hybrid salt, (Me3 NNH2 )2 [CdI4 ], which is an unprecedented case of a reversible three-step NLO switch between SHG-silent, -medium, -low, and -high states, with high contrasts of 25.5/4.3/9.2 in a temperature range of 213-303 K. By using the combined techniques of variable-temperature X-ray single-crystal structural analyses, dielectric constants, solid-state 13 C nuclear magnetic resonance spectroscopy, and Hirshfeld surface analyses, we disclose that this four-state switchable SHG behavior is highly associated with the stepwise-changed molecular dynamics of the polar organic cations. This finding demonstrates well the complexity of molecular dynamics in simple hybrid salts and their potential in designing new advanced multistep switching materials.
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