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Nanomanufacturing with DNA Origami: Factors Affecting the Kinetics and Yield of Quantum Dot Binding

机译:DNA折纸的纳米制造:影响量子点结合动力学和产量的因素。

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摘要

Molecularly directed self-assembly has the potential to become a nanomanufacturing technology if the critical factors governing the kinetics and yield of defect-free self-assembled structures can be understood and controlled. The kinetics of streptavidin-functionalized quantum dots binding to biontinylated DNA origami are quantitatively evaluated and to what extent the reaction rate and binding efficiency are controlled by the valency of the binding location, the biotin linker length, and the organization, and spacing of the binding locations on the DNA is shown. Yield improvement is systematically determined as a function of the valency of the binding locations and as a function of the quantum dot spacing. In addition, the kinetic studies show that the binding rate increases with increasing linker length, but that the yield saturates at the same level for long incubation times. The forward and backward reaction rate coefficients are determined using a nonlinear least squares fit to the measured binding kinetics, providing considerable physical insight into the factors governing this type of self-assembly process. It is found that the value of the dissociation constant, K_d, for the DNA-nanoparticle complex considered here is up to seven orders of magnitude larger than that of the native biotin-streptavidin complex. This difference is attributed to the combined effect that the much larger size of the DNA origami and the quantum dot have on the translational and rotational diffusion constants.
机译:如果能够理解和控制无缺陷自组装结构的动力学和产量的关键因素,分子定向自组装有潜力成为纳米制造技术。定量评估链霉亲和素官能化的量子点结合到生物素化的DNA折纸上的动力学,反应速度和结合效率在多大程度上受结合位置,生物素接头长度,组织和结合距离的化合价控制。显示了DNA上的位置。根据结合位置的化合价和量子点间距的函数系统地确定产率的提高。此外,动力学研究表明,结合速率随连接子长度的增加而增加,但是在较长的孵育时间下,产量会以相同的水平饱和。使用与所测结合动力学的非线性最小二乘拟合确定正向和反向反应速率系数,从而对控制这种类型的自组装过程的因素提供了可观的物理了解。发现此处考虑的DNA-纳米颗粒复合物的解离常数K_d的值比天然生物素-链霉亲和素复合物的解离常数K_d大七个数量级。这种差异归因于DNA折纸和量子点的更大尺寸对平移和旋转扩散常数的综合作用。

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  • 来源
    《Advanced Functional Materials》 |2012年第5期|p.1015-1023|共9页
  • 作者单位

    Center for Nanoscale Science and Technology National Institute of Standards and Technology Gaithersburg, MD 20899 Institute for Research in Electronics and Applied Physic University of Maryland, College Park, MD 20742;

    Center for Nanoscale Science and Technology National Institute of Standards and Technology Gaithersburg, MD 20899;

    Center for Nanoscale Science and Technology National Institute of Standards and Technology Gaithersburg, MD 20899;

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