Branzi Lorenzo, Liang Jinming, Dee Garret, Kavanagh Aoife, Gun'ko Yurii K
School of Chemistry, CRANN and AMBER Research Centres, Trinity College Dublin, College Green, Dublin 2 D02 PN40, Ireland.
ACS Appl Mater Interfaces. 2024 Jul 17;16(28):37017-37027. doi: 10.1021/acsami.4c06433. Epub 2024 Jul 5.
In this work, the production of novel multishell silver indium selenide quantum dots (QDs) shelled with zinc selenide and zinc sulfide through a multistep synthesis precisely designed to develop high-quality red-emitting QDs is explored. The formation of the multishell nanoheterostructure significantly improves the photoluminescence quantum yield of the nanocrystals from 3% observed for the silver indium selenide core to 27 and 46% after the deposition of the zinc selenide and zinc sulfide layers, respectively. Moreover, the incorporation of the multishelled QDs in a poly(methyl methacrylate) (PMMA) matrix via in situ radical polymerization is investigated, and the role of thiol ligand passivation is proven to be fundamental for the stabilization of the QDs during the polymerization step, preventing their decomposition and the relative luminescence quenching. In particular, the role of interface chemistry is investigated by considering both surface passivation by inorganic zinc chalcogenide layers, which allows us to improve the optical properties, and organic thiol ligand passivation, which is fundamental to ensuring the chemical stability of the nanocrystals during in situ radical polymerization. In this way, it is possible to produce silver-indium selenide QD-PMMA composites that exhibit bright red luminescence and high transparency, making them promising for potential applications in photonics. Finally, it is demonstrated that the new silver indium selenide QD-PMMA composites can serve as an efficient color conversion layer for the production of red light-emitting diodes.
在这项工作中，我们探索了通过精心设计的多步合成法制备新型的、由硒化锌和硫化锌包覆的多壳层银铟硒量子点（QDs），以开发高质量的红色发光量子点。多壳层纳米异质结构的形成显著提高了纳米晶体的光致发光量子产率，从硒化银铟核量子点观察到的3%分别提高到沉积硒化锌层和硫化锌层后的27%和46%。此外，还研究了通过原位自由基聚合将多壳层量子点掺入聚甲基丙烯酸甲酯（PMMA）基质中，并且证明了硫醇配体钝化在聚合步骤中对量子点的稳定起着至关重要的作用，可防止其分解和相对发光猝灭。特别是，通过考虑无机硫属锌化物层的表面钝化（这使我们能够改善光学性质）和有机硫醇配体钝化（这对于确保原位自由基聚合过程中纳米晶体的化学稳定性至关重要）来研究界面化学的作用。通过这种方式，可以制备出具有明亮红色发光和高透明度的银铟硒量子点 - PMMA复合材料，使其在光子学领域具有潜在应用前景。最后，证明了新型银铟硒量子点 - PMMA复合材料可作为生产红色发光二极管的高效颜色转换层。
