Mutailipu Miriding, Li Fuming, Jin Congcong, Yang Zhihua, Poeppelmeier Kenneth R, Pan Shilie
CAS Key Laboratory of Functional Materials and Devices for Special Environments, Xinjiang Key Laboratory of Electronic Information Materials and Devices, Xinjiang Technical Institute of Physics & Chemistry, CAS, 40-1 South Beijing Road, Urumqi, 830011, China.
Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing, 100049, China.
Angew Chem Int Ed Engl. 2022 May 16;61(21):e202202096. doi: 10.1002/anie.202202096. Epub 2022 Mar 21.
Discovery of new efficient nonlinear optical (NLO) materials with large second-order nonlinearity for the short-wave ultraviolet spectral region (λ ≤266 nm, PM=phase-matching) is still very challenging. Herein, a new beryllium-free borate CaZn (BO ) with Sr Be B O (SBBO) double-layered like configuration was rationally designed, which not only preserves the structural merits but also eliminates the limitations of the SBBO crystal. CaZn (BO ) shows a large PM second harmonic generation (SHG) reponse of 3.8×KDP, which is 38 times higher than that of its barium analogue. This enhancement mainly originates from the [Zn O ] polar chains with a large net dipole moment and [BO ] units with a high NLO active density. Our findings show the great significance of the [ZnO ] tetrahedra introduced strategy to design beryllium-free SBBO-type NLO crystals and also verify the feasibility of using simple non-isomorphic substitution to induce giant second-order nonlinearity enhancement.
发现用于短波紫外光谱区域（λ≤266 nm，PM = 相位匹配）且具有大二阶非线性的新型高效非线性光学（NLO）材料仍然极具挑战性。在此，我们合理设计了一种具有类似SrBe₂B₂O₇（SBBO）双层结构的新型无铍硼酸盐CaZn(BO₃)₂，它不仅保留了结构优点，还消除了SBBO晶体的局限性。CaZn(BO₃)₂表现出3.8×KDP的大相位匹配二次谐波产生（SHG）响应，比其钡类似物高38倍。这种增强主要源于具有大净偶极矩的[ZnO₄]极性链和具有高NLO活性密度的[BO₃]单元。我们的研究结果表明引入[ZnO₄]四面体策略对于设计无铍SBBO型NLO晶体具有重要意义，同时也验证了使用简单的非同构取代来诱导大二阶非线性增强的可行性。
