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K5(W3O9F4)(IO3): An Efficient Mid-Infrared Nonlinear Optical Compound with High Laser Damage Threshold

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posted on 2019-12-13, 20:44 authored by Chao Wu, Lin Lin, Xingxing Jiang, Zheshuai Lin, Zhipeng Huang, Mark G. Humphrey, P. Shiv Halasyamani, Chi Zhang
The discovery of nonlinear optical (NLO) materials for generating coherent mid-infrared (mid-IR) light is critically important in developing laser technologies. However, all of the commercialized mid-IR crystals thus far possess problems that have hindered their application. We report herein a function-directing structural design strategy to afford a new type of mid-IR NLO material, using fluorinated 5d0-transition metal octahedra to construct a polar noncentrosymmetric material K5(W3O9F4)­(IO3). The Λ-shaped [W3O12F4]10– polyanion, consisting of distorted octahedra, not only guides the alignment of the [IO3] units but also serves as a new kind of NLO-active chromophore in the mid-IR, with K5(W3O9F4)­(IO3) possessing an optimal combination of large second-harmonic generation response (11 × KH2PO4@1064 nm and 0.5 × AgGaS2@2100 nm), wide visible and mid-IR transparency (0.32–10.5 μm), and a giant laser damage threshold (95 × AgGaS2). The important role of the [W3O12F4]10– polyanion in improving the NLO properties and extending the IR transparency region has been clarified through first-principles calculations. Our results suggest that the incorporation of fluorinated 5d0-transition metal chromophores into iodate materials may afford a viable route to novel promising mid-IR NLO materials with exceptional NLO functions.

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