期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 143, 期 11, 页码 4138-4142出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c00416
关键词
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资金
- National Natural Science Foundation of China [51432006]
- Ministry of Education of China for the Changjiang Innovation Research Team [IRT14R23]
- State Administration of Foreign Experts Affairs [B13025]
- Innovation Program of Shanghai Municipal Education Commission
- National and Shanghai Postdoctoral Program for Innovative Talents [BX201800216, 2018192]
- Australian Research Council [DP170100411]
- Ministry of Education [B13025]
In this study, a novel tetravalent rare-earth metal fluorinated sulfate CeF2(SO4) was reported, with unique structure and outstanding second-harmonic generation (SHG) and birefringence properties. This research provides a new paradigm for the design and synthesis of high-performance nonlinear optical (NLO) materials.
Second-harmonic generation (SHG) response and birefringence are two critically important properties of nonlinear optical (NLO) materials. However, the simultaneous optimization of these two key properties remains a major challenge because of their contrasting microstructure requirements. Herein, we report the first tetravalent rare-earth metal fluorinated sulfate, CeF2(SO4). Its structure features novel net-like layers constructed by highly distorted [Ce4F4] polyhedra, which are further interconnected by [SO4] tetrahedra to form a three-dimensional structure. CeF2(SO4) exhibits the strongest SHG effect (8 times that of KH2PO4) and the largest birefringence for sulfate-based NLO materials, the latter exceeding the birefringent limit for oxides. Theoretical calculations and crystal structure analysis reveal that the unusually large SHG response and giant birefringence can be attributed to the introduction of the highly polarizable fluorinated [CeO4F4] polyhedra as well as the favorable alignment of [CeO4F4] polyhedra and [SO4] tetrahedra. This research affords a new paradigm for the designed synthesis of high-performance NLO materials.
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