Smith Andrew M, Nie Shuming
Department of Biomedical Engineering, Georgia Institute of Technology and Emory University, 101 Woodruff Circle, Suite 2001, Atlanta, Georgia 30322, USA.
J Am Chem Soc. 2008 Aug 27;130(34):11278-9. doi: 10.1021/ja804306c. Epub 2008 Aug 5.
We report a new strategy to minimize the hydrodynamic size of quantum dots (QDs) and to overcome their colloidal stability and photobleaching problems based on the use of multifunctional and multidentate polymer ligands. A novel finding is that a balanced composition of thiol (-SH) and amine (-NH 2) coordinating groups grafted to a linear polymer chain leads to highly compact nanocrystals with exceptional colloidal stability, a strong resistance to photobleaching, and high fluorescence quantum yields. In contrast to the standing brushlike conformation of PEGylated dihydrolipoic acid molecules, mutlidentate polymer ligands can wrap around the QDs in a closed "loops-and-trains" conformation. This structure is highly stable thermodynamically and is responsible for the excellent colloidal and optical properties. We have optimized this process for the preparation of ultrastable CdTe nanocrystals and have found the strategy to be broadly applicable to a wide range of nanocrystalline materials and heterostructures. This work has led to a new generation of bright and stable QDs with small hydrodynamic diameters between 5.6 and 9.7 nm with tunable fluorescence emission from the visible (515 nm) to the near-infrared (720 nm). These QDs are well suited for molecular and cellular imaging applications in which the nanoparticle hydrodynamic size must be minimized.
我们报道了一种基于使用多功能多齿聚合物配体来最小化量子点(QD)流体动力学尺寸并克服其胶体稳定性和光漂白问题的新策略。一个新发现是,接枝到线性聚合物链上的硫醇(-SH)和胺(-NH₂)配位基团的平衡组成会导致形成高度致密的纳米晶体,具有出色的胶体稳定性、对光漂白的强抗性以及高荧光量子产率。与聚乙二醇化二氢硫辛酸分子的直立刷状构象不同,多齿聚合物配体可以以封闭的“环链”构象包裹在量子点周围。这种结构在热力学上高度稳定,并赋予了优异的胶体和光学性质。我们已经优化了制备超稳定碲化镉纳米晶体的这一过程,并发现该策略广泛适用于多种纳米晶体材料和异质结构。这项工作已产生了新一代明亮且稳定的量子点,其流体动力学直径小,在5.6至9.7纳米之间,荧光发射可从可见光(515纳米)调谐至近红外(720纳米)。这些量子点非常适合用于分子和细胞成像应用,其中纳米颗粒的流体动力学尺寸必须最小化。