Nucleic acid-passivated semiconductor nanocrystals: biomolecular templating of form and function.
Nucleic acid-passivated semiconductor nanocrystals: biomolecular templating of form and function.
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DOI：
10.1021/ar900046n
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发表时间：
2010-02-16
影响因子：
18.3
通讯作者：
Kelley SO
中科院分区：
文献类型：
--
作者：
Ma N;Tikhomirov G;Kelley SO
明亮、光稳定的发光标记物是用于体外和体内生物事件成像的有力工具。半导体纳米晶体由于其高量子产率和可通过合成控制实现的光谱可调谐性而成为常用有机发光体的有吸引力的替代品。虽然常规合成方法通常产生具有优异生物成像性能的高质量纳米晶体，但配体交换和生物缀合对于使纳米晶体具有生物相容性和生物特异性是必要的。这些步骤可导致这些纳米晶体的光学特性的显著劣化。此外，通常需要惰性和无水条件的多步荧光团合成的复杂性阻止了这些发光体的许多最终用户产生他们自己的定制材料。我们试图简化半导体晶体管合成，并开发所有学科的科学家都能使用的合成路线。在寻找这种方法时，我们转向核酸作为可编程和通用的配体组，并发现这些生物分子确实适用于生物相容性半导体纳米晶体的制备。在这个帐户中，我们提出了一个总结，我们的工作核酸程序化的合成，导致在水溶液中的生物功能化的纳米晶体的一步合成的成功发展。我们首先讨论了核苷酸封端的镉和铅的硫族化物为基础的纳米晶体，以指导多核苷酸辅助合成的进一步调查所获得的结果。我们研究了单个核碱基及其结构在纳米晶体表面钝化和调制形态和光学特性中的作用。我们发现，纳米晶体的光学性质和形态高度影响核酸的结构和序列，以及反应条件。此外，使用活细胞的研究揭示了DNA钝化的CdS纳米晶体的低毒性和快速吸收，证明了它们适用于生物成像。最后，我们描述了一种新的方法，导致生产的生物功能化，DNA封端的纳米晶体在一个单一的步骤。嵌合DNA分子是这种策略的使能者，提供了纳米晶体钝化域和生物分子识别域。使用这种方法合成的纳米晶体具有良好的光谱特性以及对同源DNA、蛋白质和癌细胞靶标的高特异性。这种方法的发展可能使生物科学工作者更容易获得荧光团。
Bright, photostable luminescent labels are powerful tools for the imaging of biological events in vitro and in vivo. Semiconductor nanocrystals have emerged as attractive alternatives to commonly used organic lumophores due to their high quantum yields and the spectral tunability that can be achieved through synthetic control. While conventional synthetic methods generally yield high-quality nanocrystals with excellent properties for biological imaging, ligand exchange and biological conjugation are necessary to make nanocrystals biocompatible and biospecific. These steps can result in substantial deterioration of optical characteristic of these nanocrystals. Moreover, the complexity of multistep nanocrystal synthesis, typically requiring inert and anhydrous conditions, prohibits many end users of these lumiphores from generating their own custom materials. We sought to streamline semiconductor nanocrystal synthesis and develop synthetic routes that would be accessible to scientists from all disciplines. In search of such an approach we turned to nucleic acids as a programmable and versatile ligand set, and found that these biomolecules are indeed appropriate for biocompatible semiconductor nanocrystals preparation. In this account we present a summary of our work on nucleic acids-programmed nanocrystal synthesis that has resulted in the successful development of a one-step synthesis of biofunctionalized nanocrystals in aqueous solution. We first discuss results obtained with nucleotide-capped cadmium and lead chalcogenide-based nanocrystals that served to guide further investigation of polynucleotide-assisted synthesis. We investigate the roles of individual nucleobases and their structures in passivation of the surfaces of nanocrystals and modulating morphology and optical characteristics. We show that nanocrystals’ optical properties and morphologies are highly influenced by nucleic acid structures and sequences, as well as by reaction conditions. Moreover, studies using live cells reveal low toxicity and rapid uptake of DNA-passivated CdS nanocrystals, demonstrating their suitability for bioimaging. Finally, we describe a new approach that leads to the production of biofunctionalized, DNA-capped nanocrystals in a single step. Chimeric DNA molecules are the enablers of this strategy, providing both a domain for nanocrystals passivation and a domain for biomolecule recognition. Nanocrystals synthesized using this approach possess good spectral characteristics as well as high specificity to cognate DNA, protein, and cancer cell targets. The development of this approach may make nanocrystal lumiphores more readily accessible to those working in the biological sciences.
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