期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 61, 期 26, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202203104
关键词
Band Gap Engineering; Nonlinear Optics; Oxyfluorides; Structure-Property Relationships; Transition-Metal
资金
- National Natural Science Foundation of China [51432006, 52002276]
- Ministry of Education of China for the Changjiang Innovation Research Team [IRT14R23]
- Ministry of Education
- State Administration of Foreign Experts Affairs for the 111 Project [B13025]
- Innovation Program of Shanghai Municipal Education Commission
- Australian Research Council [DP170100411]
This study successfully constructed a non-centrosymmetric nonlinear optical material KNOF, with an extremely high F/O ratio, exhibiting an extremely wide band gap and a strong SHG response, as well as sufficient birefringence for applications. The dominant roles of partially fluorinated and totally fluorinated clusters in achieving an enlarged band gap in KNOF have been clarified by first-principles calculations.
The development of nonlinear optical (NLO) materials has been hindered by competing microstructure requirements: the need to simultaneously engineer a large hyperpolarizability (a large second-harmonic generation (SHG)) and a wide HOMO-LUMO gap (a wide band gap). Herein, a non-centrosymmetric transition-metal (TM) oxyfluoride K-5(NbOF4)(NbF7)(2) (KNOF) with an extremely high F/O ratio is constructed in high yield. KNOF exhibits an extremely wide band gap (5.88 eV) and a strong powder SHG response (4.0xKH(2)PO(4))-both being the largest values for TM-centered oxyfluorides-as well as a birefringence sufficient for applications. The dominant roles of the partially fluorinated [NbO2F4] and totally fluorinated [NbF7] groups in achieving the enlarged band gap in KNOF have been clarified by first-principles calculations. Our results suggest that maximizing the fluorine content of oxyfluorides may unlock the promise of short-wavelength-transparent materials with exceptional NLO performance.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据