Deep‐Ultraviolet Transparent Mixed Metal Sulfamates with Enhanced Nonlinear Optical Properties and Birefringence

Author:

Wang Xuefei1,Leng Xudong2,Kuk Yunseung1,Lee Jihyun1,Jing Qun2,Ok Kang Min1ORCID

Affiliation:

1. Department of Chemistry Sogang University Seoul 04107 Republic of Korea

2. Xinjiang Key Laboratory of Solid State Physics and Devices School of Physical Science and Technology Xinjiang University 777 Huarui Road Urumqi 830017 China

Abstract

AbstractEnhancing anisotropy through the controlled arrangement of anionic groups is essential for improving the nonlinear optical (NLO) performance of non‐π‐conjugated NLO materials. In this study, we present the successful synthesis of the first examples of mixed alkali metal‐alkaline earth metal sulfamate materials, including noncentrosymmetric Cs2Mg(NH2SO3)4 ⋅ 4H2O (1), as well as centrosymmetric K2Ca(NH2SO3)4 (2) and Rb2Ca(NH2SO3)4 (3). All three compounds feature promising deep ultraviolet cut‐off edges, notably 1 with a cut‐off edge below 180 nm. The synergy of Cs+ and Mg2+ cations in 1 facilitated the successful alignment of polar [NH2SO3] tetrahedra in a uniform orientation. Remarkably, 1 stands as the sole instance among reported sulfamate compounds with a co‐parallel anionic arrangement, yielding a very large dipole moment compared to other non‐π‐conjugated NLO materials. Moreover, the substantial dipole moment of 1 yields an enhanced second harmonic generation response, approximately 2.3 times that of KH2PO4, and a large birefringence of 0.054 at 546.1 nm. The approach of regulating the arrangement of anionic groups using aliovalent cations holds promise for advancing the exploration of non‐π‐conjugated NLO materials.

Funder

National Research Foundation of Korea

National Natural Science Foundation of China

Publisher

Wiley

Subject

General Chemistry,Catalysis

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