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

doi:10.1039/d1tc01883c

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 journal › Article › peer-review

16 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 F⁻ions 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 language	English
Pages (from-to)	8987-8993
Number of pages	7
Journal	Journal of Materials Chemistry C
Volume	9
Issue number	28
DOIs	https://doi.org/10.1039/d1tc01883c
Publication status	Published - 28 Jul 2021

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

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 F−ions 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.",

author = "Tianhui Wu and Xingxing Jiang and Chao Wu and Hongyuan Sha and Zujian Wang and Zheshuai Lin and Zhipeng Huang and Xifa Long and Humphrey, {Mark G.} and Chi Zhang",

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T2 - fluorinated homovalent substitution simultaneously enhances SHG response and bandgap for mid-infrared nonlinear optics

AU - Wu, Tianhui

AU - Jiang, Xingxing

AU - Wu, Chao

AU - Sha, Hongyuan

AU - Wang, Zujian

AU - Lin, Zheshuai

AU - Huang, Zhipeng

AU - Long, Xifa

AU - Humphrey, Mark G.

AU - Zhang, Chi

PY - 2021/7/28

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AB - 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 F−ions 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.

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

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