Department of Materials Science and Engineering, Hongik University , Seoul 121-791, Korea.
ACS Nano. 2014 May 27;8(5):4893-901. doi: 10.1021/nn500852g. Epub 2014 Apr 25.
Green CdSe@ZnS quantum dots (QDs) of 9.5 nm size with a composition gradient shell are first prepared by a single-step synthetic approach, and then 12.7 nm CdSe@ZnS/ZnS QDs, the largest among ZnS-shelled visible-emitting QDs available to date, are obtained through the overcoating of an additional 1.6 nm thick ZnS shell. Two QDs of CdSe@ZnS and CdSe@ZnS/ZnS are incorporated into the solution-processed hybrid QD-based light-emitting diode (QLED) structure, where the QD emissive layer (EML) is sandwiched by poly(9-vinlycarbazole) and ZnO nanoparticles as hole and electron-transport layers, respectively. We find that the presence of an additional ZnS shell makes a profound impact on device performances such as luminance and efficiencies. Compared to CdSe@ZnS QD-based devices the efficiencies of CdSe@ZnS/ZnS QD-based devices are overwhelmingly higher, specifically showing unprecedented values of peak current efficiency of 46.4 cd/A and external quantum efficiency of 12.6%. Such excellent results are likely attributable to a unique structure in CdSe@ZnS/ZnS QDs with a relatively thick ZnS outer shell as well as a well-positioned intermediate alloyed shell, enabling the effective suppression of nonradiative energy transfer between closely packed EML QDs and Auger recombination at charged QDs.
首先通过一步合成法制备了尺寸为 9.5nm 的具有组成梯度壳的绿色 CdSe@ZnS 量子点(QDs),然后通过包覆额外的 1.6nm 厚的 ZnS 壳得到了迄今为止在 ZnS 壳层中可见发光 QD 中最大的 12.7nm CdSe@ZnS/ZnS QDs。两种 CdSe@ZnS 和 CdSe@ZnS/ZnS 的 QD 被掺入溶液处理的混合 QD 基发光二极管(QLED)结构中,其中 QD 发射层(EML)分别被聚(9-乙烯基咔唑)和 ZnO 纳米粒子夹在孔和电子传输层之间。我们发现,额外的 ZnS 壳的存在对器件性能,如亮度和效率,产生了深远的影响。与基于 CdSe@ZnS QD 的器件相比,基于 CdSe@ZnS/ZnS QD 的器件的效率高得多,具体表现为前所未有的峰值电流效率 46.4cd/A 和外量子效率 12.6%。如此优异的结果可能归因于 CdSe@ZnS/ZnS QD 中独特的结构,具有相对较厚的 ZnS 外壳和位置良好的中间合金壳,能够有效抑制紧密堆积的 EML QD 之间的非辐射能量转移和带电 QD 的俄歇复合。