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Pushing Nonlinear Optical Oxides into the Mid-Infrared Spectral Region Beyond 10 μm: Design, Synthesis, and Characterization of La3SnGa5O14

  • Haichao Lan
    Haichao Lan
    State Key Laboratory of Crystal Materials and Institute of Crystal Materials, Shandong University, Jinan 250100, China
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    • , 
  • Fei Liang
    Fei Liang
    Key Lab of Functional Crystals and Laser Technology, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing 100190, China
    University of Chinese Academy of Sciences, Beijing 100190, China
    More by Fei Liang
    Orcidhttp://orcid.org/0000-0002-4932-1329
    • , 
  • Xingxing Jiang
    Xingxing Jiang
    Key Lab of Functional Crystals and Laser Technology, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing 100190, China
    More by Xingxing Jiang
    • , 
  • Cong Zhang
    Cong Zhang
    New Materials Institute, Shandong Academy of Sciences, Jinan 250014, China
    More by Cong Zhang
    • , 
  • Haohai Yu*
    Haohai Yu
    State Key Laboratory of Crystal Materials and Institute of Crystal Materials, Shandong University, Jinan 250100, China
    *[email protected]
    More by Haohai Yu
    • , 
  • Zheshuai Lin*
    Zheshuai Lin
    Key Lab of Functional Crystals and Laser Technology, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing 100190, China
    University of Chinese Academy of Sciences, Beijing 100190, China
    *[email protected]
    More by Zheshuai Lin
    Orcidhttp://orcid.org/0000-0002-9829-9893
    • , 
  • Huaijin Zhang*
    Huaijin Zhang
    State Key Laboratory of Crystal Materials and Institute of Crystal Materials, Shandong University, Jinan 250100, China
    *[email protected]
    More by Huaijin Zhang
    • , 
  • Jiyang Wang
    Jiyang Wang
    State Key Laboratory of Crystal Materials and Institute of Crystal Materials, Shandong University, Jinan 250100, China
    More by Jiyang Wang
    • , and 
  • Yicheng Wu
    Yicheng Wu
    Key Lab of Functional Crystals and Laser Technology, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing 100190, China
    Institute of Functional Crystal Materials, Tianjin University of Technology, Tianjin 300384, China
    More by Yicheng Wu
Cite this: J. Am. Chem. Soc. 2018, 140, 13, 4684–4690
Publication Date (Web):February 19, 2018
https://doi.org/10.1021/jacs.8b01009
Copyright © 2018 American Chemical Society
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Abstract

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Mid-infrared (mid-IR) coherent light is crucial for several applications in science as well as daily life, and its development especially in powerful augmentation is constrained by the availability of nonlinear optical (NLO) materials. The development of useful mid-IR NLO materials is limited by the requirements of a wide mid-IR transparent window, high laser damaged threshold (LDT), and strong NLO effect. It is common knowledge that oxides are not suitable mid-IR NLO materials, as their IR absorption cutoff wavelengths are usually <6 μm; however, their LDTs and NLO effects can be large. Herein, we focused on langasite oxides and built structure-composition-property maps that describe the NLO properties in these materials by combining computational property prediction and experimental characterization. Accordingly, rational molecular design was performed, a new member of the langasite family, La3SnGa5O14 (LGSn), was synthesized, and single crystals were grown. The produced material exhibits the widest transparent region (0.27–11.0 μm) among available oxides, the largest LDT (846 MW/cm2) among materials that are transparent to 10 μm, and the strongest SHG effect among langasites. The discovery of LGSn facilitates the application of oxides as NLO crystals in the mid-IR spectral region beyond 10 μm. More generally, the developed strategy could be used to guide and accelerate the systematic discovery of functional materials through understanding the key structure-composition-property relationships using the predictive power of computational tools.

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