Molecular Construction from AgGaS2 to CuZnPS4: Defect-Induced Second Harmonic Generation Enhancement and Cosubstitution-Driven Band Gap Enlargement,Chemistry of Materials

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Molecular Construction from AgGaS2 to CuZnPS4: Defect-Induced Second Harmonic Generation Enhancement and Cosubstitution-Driven Band Gap Enlargement
Chemistry of Materials ( IF 7.2 ) Pub Date : 2020-03-05 , DOI: 10.1021/acs.chemmater.0c00609
Zhuang Li _{1,

2} , Shengzi Zhang _{1,

2} , Zhiwei Huang ₃ , Li-Dong Zhao ₃ , Ece Uykur ₄ , Wenhao Xing _{1,

2} , Zheshuai Lin _{1,

2} , Jiyong Yao _{1,

2} , Yicheng Wu _{1,

5}

Affiliation

Herein, we offer a simple but crucial case for rational design and syntheses of infrared nonlinear optical (NLO) materials by employing state-of-the-art AgGaS₂ as a parent model. On the basis of inheriting structural advantages of AgGaS₂, an as-grown CuZnPS₄ crystal exhibits a sharply enlarged energy gap (3.0 eV) benefiting from the cosubstitution of Ag with lighter Cu/Zn. Remarkably, the valence electron distribution of CuZnPS₄ is optimized by bringing in cation vacancy defects, which significantly reinforce the second harmonic generation (SHG) (3 × AgGaS₂) and compensate for the adverse effect of band gap enlargement. Careful experimental and theoretical investigations illustrate that CuZnPS₄ strikes a desirable balance among a strong SHG response, good phase matchability, large band gap, high laser damage threshold, outstanding physicochemical stability, low melting point, and cost-effective but non-toxic composition, which might shed light on follow-up design and exploratory synthesis of NLO materials.

中文翻译：

从AgGaS ₂到CuZnPS _4的分子构建：缺陷诱导的第二谐波产生增强和共取代驱动的带隙扩大。

在此，我们通过采用最新的AgGaS ₂作为父模型，为合理设计和合成红外非线性光学（NLO）材料提供了一个简单但至关重要的案例。在继承AgGaS _2的结构优势的基础上，受益于Ag与较轻的Cu / Zn的共取代，生长的CuZnPS ₄晶体显示出急剧增大的能隙（3.0 eV）。值得注意的是，通过引入阳离子空位缺陷来优化CuZnPS ₄的价电子分布，这可以显着增强二次谐波（SHG）（3×AgGaS ₂）并补偿带隙增大的不利影响。仔细的实验和理论研究表明，CuZnPS ₄ 在强大的SHG响应，良好的相位匹配性，大的带隙，高的激光损伤阈值，出色的理化稳定性，低熔点以及经济高效但无毒的成分之间达到理想的平衡，这可能有助于后续设计NLO材料的探索性合成。

更新日期：2020-04-23

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