Heyne Benjamin, Arlt Kristin, Geßner André, Richter Alexander F, Döblinger Markus, Feldmann Jochen, Taubert Andreas, Wedel Armin
Fraunhofer IAP, Geiselbergstraße 69, 14476 Potsdam, Germany.
Photonics and Optoelectronics, Nano-Institute Munich and Department of Physics, Ludwig-Maximilians-Universität (LMU), Königinstraße 10, 80539 Munich, Germany.
Nanomaterials (Basel). 2020 Sep 17;10(9):1858. doi: 10.3390/nano10091858.
Highly luminescent indium phosphide zinc sulfide (InPZnS) quantum dots (QDs), with zinc selenide/zinc sulfide (ZnSe/ZnS) shells, were synthesized. The QDs were modified via a post-synthetic ligand exchange reaction with 3-mercaptopropionic acid (MPA) and 11-mercaptoundecanoic acid (MUA) in different MPA:MUA ratios, making this study the first investigation into the effects of mixed ligand shells on InPZnS QDs. Moreover, this article also describes an optimized method for the correlation of the QD size vs. optical absorption of the QDs. Upon ligand exchange, the QDs can be dispersed in water. Longer ligands (MUA) provide more stable dispersions than short-chain ligands. Thicker ZnSe/ZnS shells provide a better photoluminescence quantum yield (PLQY) and higher emission stability upon ligand exchange. Both the ligand exchange and the optical properties are highly reproducible between different QD batches. Before dialysis, QDs with a ZnS shell thickness of ~4.9 monolayers (ML), stabilized with a mixed MPA:MUA (mixing ratio of 1:10), showed the highest PLQY, at ~45%. After dialysis, QDs with a ZnS shell thickness of ~4.9 ML, stabilized with a mixed MPA:MUA and a ratio of 1:10 and 1:100, showed the highest PLQYs, of ~41%. The dispersions were stable up to 44 days at ambient conditions and in the dark. After 44 days, QDs with a ZnS shell thickness of ~4.9 ML, stabilized with only MUA, showed the highest PLQY, of ~34%.
合成了具有硒化锌/硫化锌(ZnSe/ZnS)壳层的高发光磷化铟锌硫化物(InPZnS)量子点(QDs)。通过与3-巯基丙酸(MPA)和11-巯基十一烷酸(MUA)以不同的MPA:MUA比例进行合成后配体交换反应对量子点进行修饰,使本研究成为对混合配体壳层对InPZnS量子点影响的首次研究。此外,本文还描述了一种量子点尺寸与量子点光吸收相关性的优化方法。配体交换后,量子点可分散在水中。较长的配体(MUA)比较短链配体提供更稳定的分散体。更厚的ZnSe/ZnS壳层在配体交换后提供更好的光致发光量子产率(PLQY)和更高的发射稳定性。配体交换和光学性质在不同量子点批次之间具有高度可重复性。在透析前,具有约4.9单层(ML)硫化锌壳层、用MPA:MUA混合(混合比例为1:10)稳定的量子点显示出最高的PLQY,约为45%。透析后,具有约4.9 ML硫化锌壳层、用MPA:MUA混合且比例为1:10和1:100稳定的量子点显示出最高的PLQY,约为41%。在环境条件下和黑暗中,分散体在长达44天内保持稳定。44天后,仅用MUA稳定的具有约4.9 ML硫化锌壳层的量子点显示出最高的PLQY,约为34%。