From Ce(IO3)4to CeF2(IO3)2: fluorinated homovalent substitution simultaneously enhances SHG response and bandgap for mid-infrared nonlinear optics

Tianhui Wu, Xingxing Jiang, Chao Wu, Hongyuan Sha, Zujian Wang, Zheshuai Lin, Zhipeng Huang, Xifa Long, Mark G. Humphrey, Chi Zhang*

*Corresponding author for this work

    Research output: Contribution to journalArticlepeer-review

    12 Citations (Scopus)

    Abstract

    Efficient mid-infrared (mid-IR) nonlinear optical (NLO) crystals are highly desirable, but it remains extremely challenging to simultaneously achieve a strong second harmonic generation (SHG) response, a large optical bandgap, and wide optical transparency in a material. In this work, a fluorinated homovalent substitution strategy has been put forward and this strategy leads to a new cerium fluorinated iodate, CeF2(IO3)2, which is designed based on a noncentrosymmetric cerium iodate, Ce(IO3)4. The introduction of Fions enables CeF2(IO3)2to achieve the simultaneous enhancement of an enlarged phase-matchable SHG response that is 8 times that of KH2PO4(KDP) and a bandgap of 2.90 eV compared to its parent Ce(IO3)4(0.9× KDP and 2.17 eV, respectively). CeF2(IO3)2exhibits a high thermal stability (∼430 °C) and a wide transparent region (0.43-6.46 μm), suggesting that CeF2(IO3)2is a promising mid-IR NLO material. First-principles simulations reveal that the difference in linear and nonlinear optical properties between Ce(IO3)4and CeF2(IO3)2is mainly attributed to the divergent anisotropies of the cerium-centered polyhedra.

    Original languageEnglish
    Pages (from-to)8987-8993
    Number of pages7
    JournalJournal of Materials Chemistry C
    Volume9
    Issue number28
    DOIs
    Publication statusPublished - 28 Jul 2021

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