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Achieving the full-wavelength phase-matching for efficient nonlinear optical frequency conversion in C(NH2)3BF4

Nature Photonics volume 17, pages 694–701 (2023)Cite this article

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Abstract

Phase-matching of light waves is a critical condition for maximizing the efficiency of nonlinear frequency conversion processes in nonlinear optical crystals; however, phase-matching, commonly achieved by tuning birefringence, is often difficult to achieve over a wide wavelength range. Here, full-wavelength phase-matching crystals that can avoid phase-mismatching across the entire optical transparency range are proposed. The anisotropic strength of bonding in the dimension of energy is confirmed theoretically to be the key to the full-wavelength phase-matching ability. We demonstrate that a crystal of guanidinium tetrafluoroborate (C(NH2)3BF4) can be phase-matched throughout its entire optical transparency range and is able to generate harmonic light as short as ~193.2 nm, which is close to its deep-ultraviolet cut-off edge. Importantly, this crystal is stable, cheap and efficient compared with commercially available nonlinear optical crystals for generation of 266 nm light. This work lays the foundation for finding a new class of crystals in which the phase-matching wavelength fully covers its optical transparency range, and also provides a high-performance crystal for generating light at 266 nm—the fourth-harmonic of a commercial 1,064 nm laser.

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Fig. 1: Crystal structure, microstructural analysis and as-grown single crystal.
Fig. 2: Linear and nonlinear optical properties of GFB crystal.
Fig. 3: Comparison of ultraviolet cut-off edge, shortest phase-matching wavelength and phase-matching wavelength loss.
Fig. 4: Tunable harmonic light generation of GFB crystal.
Fig. 5: Second-order NLO coefficients and structure–property relationship analysis.

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Data availability

The data that support the findings of this study are available from the corresponding author on reasonable requests.

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Acknowledgements

This work was financially supported by the National Key R&D Program of China (2021YFA0717800), National Natural Science Foundation of China (52002397, U2003131), West Light Foundation of CAS (XBZG-ZDSYS-202201, 2020-XBQNXZ-002), Young Elite Scientist Sponsorship Program by CAST (YESS20200068), Natural Science Foundation of Xinjiang (2022D01E087), Key Research and Development Program of Xinjiang (2022B01023-3), Key Research Program of Frontier Sciences, CAS (ZDBS-LY-SLH035), High-level Talent Project of Xinjiang Uygur Autonomous Region (2020000039), Xinjiang Tianshan Telent Program (2022TSYCCX0071), and CAS Project for Young Scientists in Basic Research (YSBR-024). We thank Z. Xu, S. Zhang and F. Zhang at Technical Institute of Physics and Chemistry, Chinese Academy of Sciences for their help with the tunable 193.2–200 nm light generation measurements; G. Zhang and B. Li at Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences for their help with 266 nm light generation and NLO coefficients test.

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Author notes

  1. These authors contributed equally: Miriding Mutailipu, Jian Han.

Authors and Affiliations

  1. Research Center for Crystal Materials, Xinjiang Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Urumqi, People’s Republic of China

    Miriding Mutailipu, Jian Han, Fuming Li, Junjie Li, Fangfang Zhang, Xifa Long, Zhihua Yang & Shilie Pan

  2. Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing, People’s Republic of China

    Miriding Mutailipu, Jian Han, Fuming Li, Junjie Li, Fangfang Zhang, Xifa Long, Zhihua Yang & Shilie Pan

  3. MIIT Key Laboratory of Advanced Display Materials and Devices, Institute of Optoelectronics and Nanomaterials, School of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing, People’s Republic of China

    Zhi Li

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Contributions

M. Mutailipu proposed the idea and performed the data analysis and paper writing. J. Han grew the single crystals. Z. Li developed the theoretical calculations. F. Li and Z. Yang performed data analysis of theoretical results. J. Li and F. Zhang assisted with the optical performance characterization. X. Long supervised the crystal growth and the laser output experiments. S. Pan conceived the idea and supervised the project. All of the authors discussed the results and commented on the manuscript.

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Correspondence to Shilie Pan.

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Nature Photonics thanks Gerard Aka and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Experimental, Figs. 1–21 and Tables 1–6.

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Mutailipu, M., Han, J., Li, Z. et al. Achieving the full-wavelength phase-matching for efficient nonlinear optical frequency conversion in C(NH2)3BF4. Nat. Photon. 17, 694–701 (2023). https://doi.org/10.1038/s41566-023-01228-7

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