A Lanthanum Ammonium Sulfate Double Salt with a Strong SHG Response and Wide Deep‐UV Transparency. (23rd December 2021)

• Record Type: Journal Article
• Authors: Wu, Chao; Jiang, Xingxing; Hu, Yilei; Jiang, Chunbo; Wu, Tianhui; Lin, Zheshuai; Huang, Zhipeng; Humphrey, Mark G.; Zhang, Chi
• Is Part Of: Angewandte Chemie. Volume 134:Number 6(2022)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2021-12-23
• Subjects: Deep-ultraviolet -- Hetero-cations -- Nonlinear optics -- Structure–property relationships -- Sulfates; Chemistry -- Periodicals; 540
• DOI: 10.1002/ange.202115855
• Languages: English
• ISSNs: 0044-8249

Abstract

Abstract: The targeted synthesis of deep‐ultraviolet (deep‐UV) nonlinear optical (NLO) materials, especially those with non‐π‐conjugated sulfates, has experienced considerable difficulties due to the need to reconcile the oft‐competing requirements for deep‐UV transparency and strong second‐harmonic generation (SHG). We report herein the designed synthesis of the first rare‐earth metal‐based deep‐UV sulfate La(NH4 )(SO4 )2 by a double‐salt strategy involving introduction of complementary cations, together with optical studies that reveal a short‐wavelength deep‐UV absorption edge (below 190 nm) and the strongest SHG response among deep‐UV NLO sulfates (2.4×KDP). Theoretical calculations and crystal structure analysis suggest that the excellent balance between SHG response and deep‐UV transparency can be attributed to a synergistic interaction of the hetero‐cations La 3+ and [NH4 ] +, which optimize alignment of the [SO4 ] tetrahedra and highly polarizable [LaO8 ] polyhedra. Abstract : The first rare‐earth metal‐based deep‐UV sulfate La(NH4 )(SO4 )2, which exhibits a short‐wavelength deep‐UV absorption edge (below 190 nm) and the strongest SHG response among deep‐UV NLO sulfates (2.4×KDP), has been successfully synthesized by a double‐salt strategy involving introduction of complementary cations.