From Ce(IO3)4 to CeF2(IO3)2: fluorinated homovalent substitution simultaneously enhances SHG response and bandgap for mid-infrared nonlinear optics. Issue 28 (29th June 2021)

• Record Type: Journal Article
• Authors: Wu, Tianhui; Jiang, Xingxing; Wu, Chao; Sha, Hongyuan; Wang, Zujian; Lin, Zheshuai; Huang, Zhipeng; Long, Xifa; Humphrey, Mark G.; Zhang, Chi
• Is Part Of: Journal of materials chemistry. Volume 9:Issue 28(2021)
• Page Start: 8987
• Page End: 8993
• Publication Date: 2021-06-29
• Subjects: Materials -- Periodicals; Chemistry, Analytic -- Periodicals; Optical materials -- Research -- Periodicals; Electronics -- Materials -- Research -- Periodicals; 543.0284
• DOI: 10.1039/d1tc01883c
• Languages: English
• ISSNs: 2050-7526

Abstract

Abstract : An efficient mid-IR NLO material, CeF2 (IO3 )2, was rationally designed using a fluorinated homovalent substitution strategy. 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 )2 to achieve the simultaneous enhancement of an enlarged phase-matchable SHG response that is 8 times that of KH2 PO4 (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 )2 exhibits a high thermal stability (∼430 °C) and a wide transparent region (0.43–6.46 μm), suggesting that CeF2 (IO3 )2 is a promising mid-IR NLO material. First-principles simulations reveal that the difference in linear and nonlinear optical properties between Ce(IO3 )4 and CeF2 (IO3 )2 is mainly attributed to the divergent anisotropies of the cerium-centered polyhedra.