Synthetically programmable DNA binding domains in aggregates of DNA-functionalized gold nanoparticles.
Synthetically programmable DNA binding domains in aggregates of DNA-functionalized gold nanoparticles.
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DOI:
10.1002/smll.200900568
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发表时间:
2009-10
期刊:
影响因子:
13.3
通讯作者:
Mirkin, Chad A.
中科院分区:
文献类型:
--
作者:
Hurst, Sarah J.;Hill, Haley D.;Macfarlane, Robert J.;Wu, Jinsong;Dravid, Vinayak P.;Mirkin, Chad A.
Polyvalent DNA-functionalized gold nanoparticle conjugates (DNA–Au NPs) have proven useful in a variety of assembly,[1–3] biodiagnostic,[4–6] and nanotherapeutic [7–10] applications. Their widespread use is a consequence of: 1) their novel hybridization properties and 2) straightforward methods for synthesizing macroscopic quantities of them in relatively monodisperse form.[1, 11, 12] In some applications, the utility of DNA–Au NPs relies on their ability to assemble via DNA hybridization into polymeric aggregates (Scheme 1A).[1] This reaction is accompanied by a concomitant red-to-blue color change, a consequence of the dampening and red-shifting of the nanoparticle surface plasmon resonance (SPR) band at $520 nm (for a 15-nm nanoparticle).[13] As the temperature is increased above the melting temperature of the duplex DNA linkages connecting the gold nanoparticles, the polymeric structure dehybridizes, the spectroscopic signature associated with the dispersed particles is restored, and a single, highly cooperative melting transition is observed. The melting transition occurs at a higher temperature and over a more narrow temperature range than free duplex DNA of the same sequence.[1, 14, 15]The structure of these nanoparticle aggregates is highly complex, and efforts have been made to elucidate the nature of the DNA interactions connecting the hybrid bioinorganic particle conjugates.[15–20] Recently, it has been determined that an assortment of traditional (ie, Watson–Crick) and nontraditional (eg, G-quadruplex)[21–23] DNA interactions (which are inherently different in binding strength) can be used to induce nanoparticle aggregation. These interactions are often randomly distributed throughout the aggregate structure. If the aggregate is held together by duplexes of varying strengths, the experiment used to monitor dehybridization is only sensitive to the strongest links, which keep the particles as part of the aggregate. In other words, if a particle is connected to other particles by more than one type of interaction, the spectroscopic measurement only detects the breaking of the strong interaction, which results in release of the particle from the aggregate. Consequently, for this type of structure, only a single melting transition is observed (Scheme 1A). Indeed, when aggregates form from particles modified with complex sequences, one must consider all of the types of interaction that can result in particle assembly and incorporation in the aggregate.
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影响因子:
64.8
作者:
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通讯作者:
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