DNA-based self-assembly of chiral plasmonic nanostructures with tailored optical response
DNA-based self-assembly of chiral plasmonic nanostructures with tailored optical response
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DOI：
10.1038/nature10889
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发表时间：
2012-03-15
期刊：
影响因子：
64.8
通讯作者：
Liedl, Tim
中科院分区：
文献类型：
--
作者：
Kuzyk, Anton;Schreiber, Robert;Liedl, Tim
在长度尺度上与光波长相当或小于光波长的物质结构可以表现出不寻常的光学性质（1）。对于这种材料来说，特别有前途的组分是金属纳米结构，其中结构改变提供了一种简单的方法来调整它们的表面等离子体共振，从而使它们与光相互作用（2，3）。但是，在可见光谱范围内具有受控光学响应的等离子体材料的自上而下的制造仍然具有挑战性，因为光刻方法在分辨率和生成真正三维结构的能力方面受到限制（4，5）。分子自组装（6，7）提供了一种替代的自下而上的制造路线，不受这些限制的限制，并且DNA和肽定向组装已被证明是用于金属纳米颗粒以复杂和手性几何形状的受控排列的可行方法（8-14）。在这里，我们表明，DNA折纸（15，16）能够高产率生产等离子体结构，包含纳米级螺旋排列的纳米粒子。我们发现，与理论预测（17）一致，溶液中的结构在可见波长处表现出定义的圆二色性和旋光色散效应，这些效应源于定位精度优于2纳米的纳米颗粒的集体等离子体-等离子体相互作用。通过利用有机分子的手性形态和纳米颗粒的等离子体性质（18-20），或者甚至在不精确控制纳米颗粒的空间构型的情况下（12，21，22），已经实现了光谱的可见部分中的圆二色性效应。相比之下，我们的纳米粒子组件的光学响应是合理设计的，并在手性，颜色和强度可调-根据我们的理论模型。
Matter structured on a length scale comparable to or smaller than the wavelength of light can exhibit unusual optical properties(1). Particularly promising components for such materials are metal nanostructures, where structural alterations provide a straightforward means of tailoring their surface plasmon resonances and hence their interaction with light(2,3). But the top-down fabrication of plasmonic materials with controlled optical responses in the visible spectral range remains challenging, because lithographic methods are limited in resolution and in their ability to generate genuinely three-dimensional architectures(4,5). Molecular self-assembly(6,7) provides an alternative bottom-up fabrication route not restricted by these limitations, and DNA-and peptide-directed assembly have proved to be viable methods for the controlled arrangement of metal nanoparticles in complex and also chiral geometries(8-14). Here we show that DNA origami(15,16) enables the high-yield production of plasmonic structures that contain nanoparticles arranged in nanometre-scale helices. We find, in agreement with theoretical predictions(17), that the structures in solution exhibit defined circular dichroism and optical rotatory dispersion effects at visible wavelengths that originate from the collective plasmon-plasmon interactions of the nanoparticles positioned with an accuracy better than two nanometres. Circular dichroism effects in the visible part of the spectrum have been achieved by exploiting the chiral morphology of organic molecules and the plasmonic properties of nanoparticles(18-20), or even without precise control over the spatial configuration of the nanoparticles(12,21,22). In contrast, the optical response of our nanoparticle assemblies is rationally designed and tunable in handedness, colour and intensity-in accordance with our theoretical model.