期刊
CHEMISTRY OF MATERIALS
卷 32, 期 16, 页码 6906-6915出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.0c01971
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]
- 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]
- National and Shanghai Postdoctoral Program for Innovative Talents [BX201800216, 2018192]
Combining a wide band gap, strong second-harmonic generation (SHG), and good phase matchability into a single structure is an ongoing challenge in the design of nonlinear optical (NLO) materials. Herein, we report the first examples of fluorinated gallium selenites AGa(3)F(6)(SeO3)(2) [A = Rb (RGFS), Cs (CGFS)] by introducing fluorinated main-group metal octahedra [GaO2F4] into the metal selenite system. The two new compounds are isostructural (noncentrosymmetric space group P6(3)mc) and feature interesting hexagonal tungsten oxide (HTO)-type [Ga3F6(SeO3)(2)](infinity) layers, with alkali metal cations acting as linkers between these layers while also maintaining charge balance. Photophysical studies demonstrate that RGFS and CGFS exhibit strong phase-matchable SHG responses [5.6 x KH2PO4 (RGFS) and 5.4 x KH2PO4 (CGFS) at 1064 nm], high laser damage thresholds [39.37 MW/cm(2) (RGFS), 41.59 MW/cm(2) (CGFS) at 1064 nm, 10 ns pulses, 1 Hz repetition rate], wide band gaps [3.57 eV (RGFS), 3.65 eV (CGFS), the latter the highest value among polar HTO-type selenites or tellurites], and large birefringences (0.097 and 0.092 at 546 nm for RGFS and CGFS, respectively); the two compounds simultaneously exhibit multiple key NLO parameters for practical applications in the near-ultraviolet and mid-infrared region. The critical role of the [GaO2F4](5-) groups in the linear and NLO responses in the two materials has been elucidated by first-principles studies. Our report demonstrates that introducing fluorinated main-group metal octahedra into metal selenite systems can lead to promising multicomponent selenite NLO materials.
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