PbGaF(SeO)Cl：通过异价取代实现能带工程策略以扩大带隙同时保持强二次谐波产生响应
PbGaF(SeO)Cl: Band Engineering Strategy by Aliovalent Substitution for Enlarging Bandgap while Keeping Strong Second Harmonic Generation Response.
作者信息
You Fengguang, Liang Fei, Huang Qian, Hu Zhanggui, Wu Yicheng, Lin Zheshuai
机构信息
Technical Institute of Physics and Chemistry, Chinese Academy of Sciences , Beijing 100190 , China.
University of Chinese Academy of Sciences , Beijing 100190 , China.
出版信息
J Am Chem Soc. 2019 Jan 16;141(2):748-752. doi: 10.1021/jacs.8b11485. Epub 2018 Nov 30.
Wide bandgap and strong second-order generation (SHG) effect are two crucial but contradictory conditions for practical nonlinear optical (NLO) materials. Herein, a new NLO crystal PbGaF(SeO)Cl (I) containing novel functional (GaOF) octahedra is designed and synthesized by a rational band engineering strategy with aliovalent substitution. Benefiting from the removal of transition metal cations and the introduction of bridged F anions, I exhibits the widest bandgap among all reported phase-matchable NLO selenites. Meanwhile, a strong SHG response more than 4.5 times of KHPO (KDP) is maintained. The dominate role of the (GaOF) groups to the enlarged bandgap in I are elucidated by first-principles studies.
宽带隙和强二次谐波产生（SHG）效应是实用非线性光学（NLO）材料的两个关键但相互矛盾的条件。在此，通过具有异价取代的合理能带工程策略，设计并合成了一种含有新型功能（GaOF）八面体的新型NLO晶体PbGaF(SeO)Cl（I）。得益于过渡金属阳离子的去除和桥连F阴离子的引入，I在所有报道的可相位匹配的NLO亚硒酸盐中表现出最宽的带隙。同时，保持了比KHPO（KDP）强4.5倍以上的强SHG响应。通过第一性原理研究阐明了（GaOF）基团对I中扩大带隙的主导作用。
Zotero 插件