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.
Mirkin, Chad A.
中科院分区:
材料科学1区
文献类型:
--
作者:
Hurst, Sarah J.;Hill, Haley D.;Macfarlane, Robert J.;Wu, Jinsong;Dravid, Vinayak P.;Mirkin, Chad A.

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多价dna功能化金纳米颗粒缀合物(DNA-Au NPs)已被证明在各种组装,[1-3]生物诊断,[4-6]和纳米治疗[7-10]应用中非常有用。它们的广泛使用是由于:1)它们新颖的杂化性质和2)以相对单分散的形式合成它们的宏观数量的直接方法。[1,11,12]在某些应用中,DNA - au NPs的效用依赖于它们通过DNA杂交组装成聚合聚集体的能力(方案1A)这个反应伴随着伴随的由红到蓝的颜色变化,这是520 nm处纳米粒子表面等离子体共振(SPR)带的衰减和红移的结果(对于15 nm的纳米粒子)当温度高于连接金纳米颗粒的双链DNA键的熔化温度时,聚合物结构去杂化,与分散颗粒相关的光谱特征被恢复,并且观察到一个单一的,高度合作的熔化转变。与相同序列的自由双工DNA相比,熔化转变发生在更高的温度和更窄的温度范围内。[1,14,15]这些纳米粒子聚集体的结构非常复杂,人们已经努力阐明连接杂化生物无机粒子偶联物的DNA相互作用的性质。[15-20]最近,人们已经确定,传统的(如沃森-克里克)和非传统的(如g -四重体)[21-23]DNA相互作用(其结合强度本质上不同)可用于诱导纳米颗粒聚集。这些相互作用通常随机分布在整个聚合结构中。如果聚集体是由不同强度的双链结合在一起,用于监测去杂化的实验只对最强的链接敏感,这些链接使颗粒保持为聚集体的一部分。换句话说,如果一个粒子通过一种以上的相互作用与其他粒子相连,光谱测量只检测到强相互作用的破坏,这导致粒子从聚集体中释放出来。因此,对于这种类型的结构,只观察到一次熔融转变(方案1A)。事实上,当聚合体由经过复杂序列修饰的粒子形成时,人们必须考虑所有类型的相互作用,这些相互作用可能导致粒子在聚合体中组装和结合。
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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发表时间: 1996-08-15
期刊: NATURE
影响因子: 64.8
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