期刊
JOURNAL OF MATERIALS CHEMISTRY C
卷 9, 期 43, 页码 15407-15414出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d1tc04498b
关键词
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资金
- National Natural Science Foundation of China [51778570, 51879230, 21771179, 22175175]
- Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China [2021ZR118]
- Natural Science Foundation of Fujian Province [2019J01133]
- Natural Science Basic Research Program of Shaanxi [2020JQ-710]
In this study, a quaternary non-centrosymmetric thioantimonate was designed and successfully synthesized through an aliovalent-cation-substitution-induced strategy. The compound exhibits a unique crystal structure and excellent optical properties, showing phase-matching ability in the infrared region. The research reveals the synergistic effects of different building motifs on the optical effects.
Non-centrosymmetric (NCS) structure is the precondition and foundation for the development of high-performance nonlinear optical (NLO) crystals. In this research, a quaternary NCS thioantimonate, K2Ag3Sb3S7, is designed through an aliovalent-cation-substitution-induced strategy based on the centrosymmetric (CS) parent compound K2Sb4S7 and successfully obtained through a facile surfactant-thermal technology. The unique crystal structure of K2Ag3Sb3S7 belongs to the orthorhombic space group Cmc2(1) (no. 36) and is made of charge-balanced K+ cations and two-dimensional (2D) anionic layers [Ag3Sb3S7](2-) constructed by the vertex-sharing of (infinity)[Ag3SbS5](4-) and (infinity)[SbS2](-) chains. Remarkably, K2Ag3Sb3S7 not only possesses a phase-matching (PM) ability in the IR region, but also displays a perfect balance between a high second-harmonic-generation (SHG) coefficient (1.5 x commercial AgGaS2) and a large laser-induced damage threshold (3.2 x commercial AgGaS2). Moreover, theoretical studies uncover that the synergistic effects of three types of asymmetric building motifs (i.e., [SbS3], [Sb2S5] and [Ag3S6]) contribute to the large SHG effect and birefringence (Delta n). This study not only demonstrates that aliovalent cation substitution can be a robust means of obtaining the NCS thioantimonates but also provides a deeper insight into the structure-property relationship of IR-NLO chalcogenides.
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