二次谐波产生
钽
材料科学
紫外线
波长
光电子学
非线性光学
离子键合
相(物质)
光学
非线性系统
离子
化学
物理
激光器
冶金
有机化学
量子力学
作者
Yi Hu,Chao Wu,Xingxing Jiang,Kaining Duanmu,Zhipeng Huang,Zheshuai Lin,Mark G. Humphrey,Chi Zhang
标识
DOI:10.1002/anie.202315133
摘要
Abstract The development of urgently‐needed ultraviolet (UV)/deep‐UV nonlinear optical (NLO) materials has been hindered by contradictory requirements of the microstructure, in particular the need for a strong second‐harmonic generation (SHG) response as well as a short phase‐matching (PM) wavelength. We herein employ a “de‐covalency” band gap engineering strategy to adjust the optical linearity and nonlinearity. This has been achieved by assembling two types of transition‐metal (TM) polyhedra ([TaO 2 F 4 ] and [TaF 7 ]), affording the first tantalum‐based deep‐UV‐transparent NLO materials, A 5 Ta 3 OF 18 (A = K (KTOF), Rb (RTOF)). Experimental and theoretical studies reveal that the highly ionic bonds and strong electropositivity of tantalum in the two oxyfluorides induce record short PM wavelengths (238 (KTOF) and 240 (RTOF) nm) for d 0 ‐TM‐centered oxides, in addition to strong SHG responses (2.8 × KH 2 PO 4 (KTOF) and 2.6 × KH 2 PO 4 (RTOF)), and sufficient birefringences (0.092 (KTOF) and 0.085 (RTOF) at 546 nm). These results not only broaden the available strategies for achieving deep‐UV NLO materials by exploiting the currently neglected d 0 ‐TMs, but also push the shortest PM wavelength into the short‐wavelength UV region.
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