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Unveiling the dual role of silver-associated defects: the manipulators of luminescence and carrier dynamics in eco-friendly AgIn0.5Ga0.5S2

揭示银关联缺陷的双重作用: 环保型AgIn0.5Ga0.5S2 中 发光和载流子动力学的操纵者

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Abstract

AgIn0.5Ga0.5S2 has attracted extensive attention in many fields owing to environmental friendliness, low synthetic cost, flexible and adjustable components. Appropriate direct bandgap, no forbidden transition, and high exciton binding energy make it a promising luminescent material. The evolution of the multicomponent system enriches the photoelectric properties and makes its intrinsic defects more complex. Conversely, these defects have an important effect on the photoelectric properties, thus affecting its luminescent performance. However, the microscopic mechanism of point defects corresponding to luminescence observed in experiments is mostly unknown or inferred indirectly for such semiconductors. Here, the mechanism between the microscopic defects and luminescence of AgIn0.5Ga0.5S2 is systematically revealed. Thermodynamic stability shows that AgIn0.5Ga0.5S2 is metastable and has significant competition between the secondary phases. Furthermore, the calculated defect results demonstrate that Ag-associated defects are the behind-the-scenes manipulators. Two shallow-level defects (VAg and Agi) serve as carrier providers, while four deep-level antisite defects (AgIn, AgGa, InAg, and GaAg) act as carrier annihilators. Ultimately, the study of carrier dynamics reveals the adverse effects of four deep-level antisite defects on carriers’ radiative processes. These are intended to provide important guidance for the functional application of AgIn0.5Ga0.5S2 in the field of luminescence.

摘要

AgIn0.5Ga0.5S2 由于环境友好、合成成本低、成分灵活可调等优 点在许多领域受到广泛关注. 适当的直接带隙、无禁戒跃迁和高激子 结合能使其成为一种有前途的发光材料. 多组分体系的演化丰富了光 电特性, 并使其本征缺陷更加复杂. 反过来, 这些缺陷对光电性能有重 要影响, 从而影响其发光性能. 然而, 对于这类半导体, 在实验中观察到 的与发光相对应的点缺陷的微观机制大多是未知的或间接推断的. 本 工作系统地揭示了AgIn0.5Ga0.5S2 的微观缺陷与发光之间的机制. 热力 学稳定性表明AgIn0.5Ga0.5S2 是亚稳态的并且与次生相之间存在显著的 竞争. 此外, 计算的缺陷结果表明, 与银关联的缺陷是幕后操纵者. 两个 浅能级缺陷(VAg 和Agi)充当载流子提供者, 而四个深能级反位缺陷 (AgIn, AgGa, InAg 和GaAg)充当载流子湮灭者. 最后, 载流子动力学的研 究揭示了四种深能级反位缺陷对载流子辐射过程的不利影响. 这些旨 在为AgIn0.5Ga0.5S2 在发光领域的功能应用提供重要指导.

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Acknowledgements

This work was financially supported by the Natural Science Foundation of Jiangsu Province (BK20180071), the Fundamental Research Funds for the Central Universities (30919011109), Qing Lan Project of Jiangsu Province, and the Six Talent Peaks Project of Jiangsu Province (XCL-035).

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Authors and Affiliations

  1. MIIT Key Laboratory of Advanced Display Materials and Devices, School of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing, 210094, China

    Gaoyu Liu  (刘高豫), Lili Xu  (徐丽丽), Yang Hu  (胡扬), Xiaoming Li  (李晓明), Shengli Zhang  (张胜利) & Haibo Zeng  (曾海波)

  2. Department of Materials Science and Engineering, Korea University, Seoul, 02841, Republic of Korea

    Seokwoo Jeon

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  1. Gaoyu Liu  (刘高豫)
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  2. Lili Xu  (徐丽丽)
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  3. Yang Hu  (胡扬)
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  4. Xiaoming Li  (李晓明)
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  6. Shengli Zhang  (张胜利)
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Contributions

Author contributions Zeng H, Zhang S and Liu G conceived the idea and directed the project. Liu G analyzed the data and wrote the manuscript. All authors commented and revised the manuscript.

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Correspondence to Shengli Zhang  (张胜利) or Haibo Zeng  (曾海波).

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Conflict of interest The authors declare that they have no conflict of interest.

Additional information

Supplementary information Supporting data are available in the online version of the paper.

Gaoyu Liu is a PhD candidate at Nanjing University of Science and Technology. His current research focuses on defect regulation and carrier dynamics in eco-friendly luminescent semiconductors.

Shengli Zhang received his PhD degree from Beijing University of Chemical Technology in 2013. He then joined the MIIT Key Laboratory of Advanced Display Materials and Devices, Institute of Optoelectronics & Nanomaterials, Nanjing University of Science and Technology. His research interests are focused on electronic or optoelectronic devices and applications.

Haibo Zeng received his PhD degree from the Institute of Solid State Physics, Chinese Academy of Sciences in 2006. Now he is the leader of MIIT Key Laboratory of Advanced Display Materials and Devices, Institute ofOptoelectronics & Nanomaterials. His current research focuses on QDs (synthesis, optics, photodetectors and LEDs).

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40843_2023_2680_MOESM1_ESM.pdf

Supplementary materials: Unveiling the Dual Role of Silver-Associated Defects: The Manipulators of Luminescence and Carrier Dynamics in Eco-Friendly AgIn0.5Ga0.5S2

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Liu, G., Xu, L., Hu, Y. et al. Unveiling the dual role of silver-associated defects: the manipulators of luminescence and carrier dynamics in eco-friendly AgIn0.5Ga0.5S2. Sci. China Mater. 67, 214–222 (2024). https://doi.org/10.1007/s40843-023-2680-x

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