Journal
INORGANIC CHEMISTRY
Volume 61, Issue 24, Pages 9205-9212Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.2c00759
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Funding
- Presidential Foundation of the China Academy of Engineering Physics [YZJJLX2019005]
- National Natural Science Foundation of China [U20A20210, 51972021]
- Fundamental Research Funds for the Central Universities [ZYGX2019Z005]
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A new noncentrosymmetric sulfide SrAgAsS4 was prepared through aliovalent substitution based on centrosymmetric SrGa2S4. The compound exhibits unique two-dimensional structure and shows strong second-harmonic generation response and moderate band gap, suggesting potential applications in functional materials design.
A new noncentrosymmetric (NCS) quaternary sulfide, SrAgAsS4, was obtained via the strategy of aliovalent substitution based on centrosymmetric (CS) SrGa2S4. The new compound features two-dimensional [AgAsS4](2-) layers, which are composed of alternately connected [AsS4] tetrahedra and [AgS4] tetrahedra. Importantly, SrAgAsS4 exhibits a strong phase-matched second-harmonic generation response (1.35 x AgGaS2 at 2100 nm) and has a suitable birefringence (0.15@2100 nm) and moderate band gap (2.31 eV). The first-principles calculations revealed the significant contribution of [AsS4] and [AgS4] tetrahedra to its optical properties. This work will promote the application of the aliovalent substitution strategy in the design of NCS-structure-based functional materials.
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