From H12C4N2CdI4 to H11C4N2CdI3: a highly polarizable CdNI3 tetrahedron induced a sharp enhancement of second harmonic generation response and birefringence

四面体 卤化物 双折射 材料科学 极化率 二次谐波产生 带隙 相(物质) 非线性光学 金属卤化物 金属 光电子学 结晶学 物理 化学 光学 无机化学 分子 非线性系统 激光器 有机化学 量子力学 冶金
作者
Huai-Yu Wu,Chun‐Li Hu,Miao-Bin Xu,Qianqian Chen,Nan Ma,Xiao‐Ying Huang,Ke‐Zhao Du,Jin Chen
出处
期刊:Chemical Science [Royal Society of Chemistry]
卷期号:14 (35): 9533-9542 被引量:15
标识
DOI:10.1039/d3sc03052k
摘要

In this study, we identify a novel class of second-order nonlinear optical (NLO) crystals, non-π-conjugated piperazine (H10C4N2, PIP) metal halides, represented by two centimeter-sized, noncentrosymmetric organic-inorganic metal halides (OIMHs), namely H12C4N2CdI4 (P212121) and H11C4N2CdI3 (Cc). H12C4N2CdI4 is the first to be prepared, and its structure contains a CdI4 tetrahedron, which led to a poor NLO performance, including a weak and non-phase-matchable second harmonic generation (SHG) response of 0.5 × KH2PO4 (KDP), a small birefringence of 0.047 @1064 nm and a narrow bandgap of 3.86 eV. Moreover, H12C4N2CdI4 is regarded as the model compound, and we further obtain H11C4N2CdI3via the replacement of CdI4 with a highly polarizable CdNI3 tetrahedron, which results in a sharp enhancement of SHG response and birefringence. H11C4N2CdI3 exhibits a promising NLO performance including 6 × KDP, 4.10 eV, Δn = 0.074 @1064 nm and phase matchability, indicating that it is the first OIMH to simultaneously exhibit strong SHG response (>5 × KDP) and a wide bandgap (>4.0 eV). Our work presents a novel direction for designing high-performance NLO crystals based on organic-inorganic halides and provides important insights into the role of the hybridized tetrahedron in enhancing the SHG response and birefringence.
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