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DNA-based self-assembly of chiral plasmonic nanostructures with tailored optical response


Matter structured on a length scale comparable to or smaller than the wavelength of light can exhibit unusual optical properties1. 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 light2,3. 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 architectures4,5. Molecular self-assembly6,7 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 geometries8,9,10,11,12,13,14. Here we show that DNA origami15,16 enables the high-yield production of plasmonic structures that contain nanoparticles arranged in nanometre-scale helices. We find, in agreement with theoretical predictions17, 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 nanoparticles18,19,20, or even without precise control over the spatial configuration of the nanoparticles12,21,22. 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.

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Figure 1: Assembly of DNA origami gold nanoparticle helices and principle of circular dichroism.
Figure 2: Circular dichroism of self-assembled gold nanohelices.
Figure 3: Spectral tuning of circular dichroism by metal composition.
Figure 4: Optical rotatory dispersion of self-assembled gold nanohelices.

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We thank H. Dietz and G. Acuna for experimental advice and B. Yurke, E. Graugnard, J. O. Rädler and J. P. Kotthaus for discussions. We acknowledge J. Buchner and M. Rief for giving us access to their CD spectrometers, E. Herold for help with the CD measurements, and T. Martin and S. Kempter for assistance. We also thank D. M. Smith for carefully reading the manuscript. This work was funded by the Volkswagen Foundation, the DFG Cluster of Excellence NIM (Nanosystems Initiative Munich) and the NSF (USA).

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Authors and Affiliations



A.K., R.S., A.H., F.C.S., A.O.G. and T.L. designed the research. A.K., R.S. and E.-M.R. designed the nanostructures and performed CD measurements. G.P. produced and purified gold samples. A.H. and T.L. investigated ORD effects. Z.F. and A.O.G. performed theoretical calculations. A.K., R.S. and A.O.G. prepared the figures and A.K., R.S., A.H., F.C.S., A.O.G. and T.L. wrote the manuscript.

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Correspondence to Tim Liedl.

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The authors declare no competing financial interests.

Supplementary information

Supplementary Information

The file contains Supplementary Notes 1-10, which include Supplementary Theory, Supplementary Methods, Supplementary Data, Supplementary Figures 1-30 and Supplementary References. (PDF 5859 kb)

Supplementary Movie

The movie shows optical rotatory dispersion of dried nanohelices. The samples and set-up investigated here are also described in Supplementary Figure 26 – see Supplementary Information file. (MOV 5493 kb)

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Kuzyk, A., Schreiber, R., Fan, Z. et al. DNA-based self-assembly of chiral plasmonic nanostructures with tailored optical response. Nature 483, 311–314 (2012).

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