The Biodesign Institute and Department of Chemistry and Biochemistry, Arizona State University, Tempe, Arizona 85287, USA.
J Am Chem Soc. 2012 Oct 24;134(42):17424-7. doi: 10.1021/ja3081023. Epub 2012 Oct 10.
The assembly and isolation of DNA oligonucleotide-functionalized gold nanoparticles (AuNPs) has become a well-developed technology that is based on the strong bonding interactions between gold and thiolated DNA. However, achieving DNA-functionalized semiconductor quantum dots (QDs) that are robust enough to withstand precipitation at high temperature and ionic strength through simple attachment of modified DNA to the QD surface remains a challenge. We report the synthesis of stable core/shell (1-20 monolayers) QD-DNA conjugates in which the end of the phosphorothiolated oligonucleotide (5-10 nucleotides) is "embedded" within the shell of the QD. These reliable QD-DNA conjugates exhibit excellent chemical and photonic stability, colloidal stability over a wide pH range (4-12) and at high salt concentrations (>100 mM Na(+) or Mg(2+)), bright fluorescence emission with quantum yields of up to 70%, and broad spectral tunability with emission ranging from the UV to the NIR (360-800 nm).
DNA 寡核苷酸功能化金纳米粒子(AuNPs)的组装和分离已经成为一种成熟的技术,其基础是金与巯基化 DNA 之间的强键合相互作用。然而,通过简单地将修饰后的 DNA 附着到 QD 表面,实现足够稳定的 DNA 功能化半导体量子点(QDs),以在高温和高离子强度下不发生沉淀,仍然是一个挑战。我们报告了稳定的核/壳(1-20 单层)QD-DNA 缀合物的合成,其中磷硫代寡核苷酸(5-10 个核苷酸)的末端“嵌入”在 QD 的壳层内。这些可靠的 QD-DNA 缀合物表现出优异的化学和光子稳定性、在宽 pH 范围(4-12)和高盐浓度(>100mM Na(+)或 Mg(2+))下的胶体稳定性、高达 70%的明亮荧光发射量子产率,以及从紫外到近红外(360-800nm)的宽光谱可调谐性。