Zorn Gilad, Dave Shivang R, Weidner Tobias, Gao Xiaohu, Castner David G
National ESCA and Surface Analysis Center for Biomedical Problems, The Department of Chemical Engineering.
National ESCA and Surface Analysis Center for Biomedical Problems, The Department of Bioengineering, University of Washington, Seattle, WA 98195-1653.
Surf Sci. 2016 Jun;648:339-344. doi: 10.1016/j.susc.2015.10.013.
Surface engineering advances of semiconductor quantum dots (QDs) have enabled their application to molecular labeling, disease diagnostics and tumor imaging. For biological applications, hydrophobic core/shell QDs are transferred into aqueous solutions through the incorporation of water-solubility imparting moieties, typically achieved via direct exchange of the native surface passivating ligands or indirectly through the adsorption of polymers. Although polymeric encapsulation has gained wide acceptance, there are few reports addressing the characterization of the adsorbed polymers and existing theoretical analyses are typically based on simple geometric models. In this work, we experimentally characterize and quantify water-soluble QDs prepared by adsorption of amphiphilic poly(maleic anhydride--1-tetradecene) (PMAT, MW~9000) onto commercially available CdSe/CdS/ZnS (CdSe/CdS/ZnS-PMAT). Using x-ray photoelectron spectroscopy (XPS) we determined that ~15 PMAT molecules are adsorbed onto each QD and sum frequency generation (SFG) vibrational spectra was utilized to investigate the mechanism of interaction between PMAT molecules and the QD surface. Importantly, when employed together, these techniques constitute a platform with which to investigate any polymer-nanoparticle complex in general.
半导体量子点(QDs)的表面工程进展使其能够应用于分子标记、疾病诊断和肿瘤成像。对于生物应用,疏水性核壳量子点通过引入赋予水溶性的部分被转移到水溶液中,这通常通过直接交换天然表面钝化配体或间接通过聚合物吸附来实现。尽管聚合物封装已被广泛接受,但很少有报道涉及对吸附聚合物的表征,现有的理论分析通常基于简单的几何模型。在这项工作中,我们通过将两亲性聚(马来酸酐 - 1 - 十四碳烯)(PMAT,分子量约9000)吸附到市售的CdSe/CdS/ZnS(CdSe/CdS/ZnS - PMAT)上来对水溶性量子点进行实验表征和定量。使用X射线光电子能谱(XPS),我们确定每个量子点上吸附了约15个PMAT分子,并利用和频产生(SFG)振动光谱来研究PMAT分子与量子点表面之间的相互作用机制。重要的是,当一起使用时,这些技术构成了一个总体上可用于研究任何聚合物 - 纳米颗粒复合物的平台。