Weigert Florian, Müller Anja, Häusler Ines, Geißler Daniel, Skroblin Dieter, Krumrey Michael, Unger Wolfgang, Radnik Jörg, Resch-Genger Ute
Division 1.2 Biophotonics, Federal Institute for Material Research and Testing (BAM), Richard-Willstätter-Str. 11, 12489, Berlin, Germany.
Division 6.1 Surface Analysis and Interfacial Chemistry, Federal Institute for Material Research and Testing (BAM), Unter den Eichen 44-46, 12203, Berlin, Germany.
Sci Rep. 2020 Nov 26;10(1):20712. doi: 10.1038/s41598-020-77530-z.
Controlling thickness and tightness of surface passivation shells is crucial for many applications of core-shell nanoparticles (NP). Usually, to determine shell thickness, core and core/shell particle are measured individually requiring the availability of both nanoobjects. This is often not fulfilled for functional nanomaterials such as many photoluminescent semiconductor quantum dots (QD) used for bioimaging, solid state lighting, and display technologies as the core does not show the application-relevant functionality like a high photoluminescence (PL) quantum yield, calling for a whole nanoobject approach. By combining high-resolution transmission electron microscopy (HR-TEM) and X-ray photoelectron spectroscopy (XPS), a novel whole nanoobject approach is developed representatively for an ultrabright oleic acid-stabilized, thick shell CdSe/CdS QD with a PL quantum yield close to unity. The size of this spectroscopically assessed QD, is in the range of the information depth of usual laboratory XPS. Information on particle size and monodispersity were validated with dynamic light scattering (DLS) and small angle X-ray scattering (SAXS) and compared to data derived from optical measurements. In addition to demonstrating the potential of this novel whole nanoobject approach for determining architectures of small nanoparticles, the presented results also highlight challenges faced by different sizing and structural analysis methods and method-inherent uncertainties.
控制核壳纳米颗粒(NP)表面钝化壳的厚度和紧密性对于其许多应用至关重要。通常,为了确定壳层厚度,需要分别测量核以及核/壳颗粒,这就要求同时具备这两种纳米物体。对于功能性纳米材料,如许多用于生物成像、固态照明和显示技术的光致发光半导体量子点(QD),这一要求往往无法满足,因为其核不具备与应用相关的功能,如高光致发光(PL)量子产率,因此需要采用整体纳米物体方法。通过结合高分辨率透射电子显微镜(HR-TEM)和X射线光电子能谱(XPS),针对一种超亮的油酸稳定化厚壳CdSe/CdS量子点,开发了一种新颖的整体纳米物体方法,该量子点的PL量子产率接近1。这种通过光谱评估的量子点的尺寸,处于常规实验室XPS信息深度范围内。通过动态光散射(DLS)和小角X射线散射(SAXS)验证了颗粒尺寸和单分散性信息,并与光学测量得到的数据进行了比较。除了展示这种新颖的整体纳米物体方法在确定小纳米颗粒结构方面的潜力外,所呈现的结果还突出了不同尺寸和结构分析方法面临的挑战以及方法固有的不确定性。