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Molecular engineering of chiral colloidal liquid crystals using DNA origami

Nature Materials volume 16, pages 849–856 (2017)Cite this article

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Abstract

Establishing precise control over the shape and the interactions of the microscopic building blocks is essential for design of macroscopic soft materials with novel structural, optical and mechanical properties. Here, we demonstrate robust assembly of DNA origami filaments into cholesteric liquid crystals, one-dimensional supramolecular twisted ribbons and two-dimensional colloidal membranes. The exquisite control afforded by the DNA origami technology establishes a quantitative relationship between the microscopic filament structure and the macroscopic cholesteric pitch. Furthermore, it also enables robust assembly of one-dimensional twisted ribbons, which behave as effective supramolecular polymers whose structure and elastic properties can be precisely tuned by controlling the geometry of the elemental building blocks. Our results demonstrate the potential synergy between DNA origami technology and colloidal science, in which the former allows for rapid and robust synthesis of complex particles, and the latter can be used to assemble such particles into bulk materials.

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Figure 1: Origami-based cholesteric liquid crystals.
Figure 2: Origami filaments assemble into supramolecular 1D twisted ribbons.
Figure 3: Geometry of the constituent rods alone determines twisted-ribbon structure.
Figure 4: Mechanical properties of 1D twisted ribbons.
Figure 5: Phase diagram of an origami-depletant mixture.
Figure 6: Stimuli induced ribbon-to-membrane transition.

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Acknowledgements

We acknowledge support of NSF-MRSEC-1420382 and NSF-DMR-1609742 (to M.S., M.J.Z. and Z.D). We also acknowledge use of the Brandeis MRSEC optical microscopy and biosynthesis facility supported by NSF-MRSEC-1420382, as well as a Hans Fisher Senior Fellowship from TUM Institute of Advanced Study. This work was also supported by a European Research Council Starting Grant to H.D. (GA no. 256270) and by the Deutsche Forschungsgemeinschaft through grants provided via the TUM Institute of Advanced Study, the Cluster of Integrated Protein Science, the Nano Initiative Munich, and the Gottfried-Wilhelm-Leibniz Program (C.H.W., F.P. and H.D.).

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Authors and Affiliations

  1. Department of Physics, Brandeis University, Waltham, Massachusetts, 02454, USA

    Mahsa Siavashpouri, Mark J. Zakhary & Zvonimir Dogic

  2. Physik Department and Walter Schottky Institute, Technische Universität München, Am Coulombwall 4a, 85748 Garching, Germany

    Christian H. Wachauf, Florian Praetorius & Hendrik Dietz

  3. Institute for Advanced Study, Technische Universität München, Lichtenbergstraße 2a, 85748 Garching, Germany

    Hendrik Dietz

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  1. Mahsa Siavashpouri
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Contributions

H.D. and Z.D. conceived the experiments. M.S. and M.J.Z. performed initial experimental observations. M.S. performed all the experiments. C.H.W. designed and characterized origami filaments. Z.D., M.S., H.D., C.H.W. and M.J.Z. analysed the experimental data. F.P. developed methods to purify large quantities of scaffold and provided them for our studies. M.S., H.D. and Z.D. wrote the manuscript. All authors revised the manuscript.

Corresponding authors

Correspondence to Hendrik Dietz or Zvonimir Dogic.

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Siavashpouri, M., Wachauf, C., Zakhary, M. et al. Molecular engineering of chiral colloidal liquid crystals using DNA origami. Nature Mater 16, 849–856 (2017). https://doi.org/10.1038/nmat4909

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