School of Chemistry and CRANN, University of Dublin , Trinity College, Dublin 2, Ireland.
ITMO University , St. Petersburg 197101, Russia.
ACS Nano. 2017 Sep 26;11(9):9207-9214. doi: 10.1021/acsnano.7b04199. Epub 2017 Aug 22.
Core/shell quantum dots (QDs) are of high scientific and technological importance as these nanomaterials have found a number of valuable applications. In this paper, we have investigated the dependence of optical activity and photoluminescence upon CdS shell thickness in a range of core-shell structured CdSe/CdS QDs capped with chiral ligands. For our study, five samples of CdSe/CdS were synthesized utilizing successive ion layer adsorption and reaction to vary the thickness of the CdS shell from 0.5 to 2 nm, upon a 2.8 nm diameter CdSe core. Following this, a ligand exchange of the original aliphatic ligands with l- and d-cysteine was carried out, inducing a chiroptical response in these nanostructures. The samples were then characterized using circular dichroism, photoluminescent spectroscopy, and fluorescence lifetime spectroscopy. It has been found that the induced chiroptical response was inversely proportional to the CdS shell thickness and showed a distinct evolution in signal, whereas the photoluminescence of our samples showed a direct relationship to shell thickness. In addition, a detailed study of the influence of annealing time on the optical activity and photoluminescence quantum yield was performed. From our work, we have been able to clearly illustrate the approach and strategies that must be used when designing optimal photoluminescent optically active CdSe/CdS core-shell QDs.
核壳量子点(QDs)具有很高的科学和技术重要性,因为这些纳米材料已经找到了许多有价值的应用。在本文中,我们研究了在具有手性配体的核壳结构 CdSe/CdS QD 中,CdS 壳厚度对光学活性和光致发光的依赖性。对于我们的研究,利用连续离子层吸附和反应合成了五组 CdSe/CdS 样品,以改变 CdS 壳的厚度从 0.5 到 2nm,CdSe 核的直径为 2.8nm。随后,对原始脂肪族配体进行了 l-和 d-半胱氨酸的配体交换,在这些纳米结构中诱导出手性响应。然后使用圆二色性、光致发光光谱和荧光寿命光谱对样品进行了表征。研究发现,诱导的手性响应与 CdS 壳厚度成反比,并显示出信号的明显变化,而我们的样品的光致发光与壳厚度呈直接关系。此外,还对退火时间对光学活性和光致发光量子产率的影响进行了详细研究。通过我们的工作,我们能够清楚地说明在设计最佳光致发光的光学活性 CdSe/CdS 核壳 QD 时必须采用的方法和策略。