Abstract

Surface encoding of colloidal nanoparticles with DNA is fundamental for fields where recognition interaction is required, particularly controllable material self-assembly. However, regioselective surface encoding of nanoparticles is still challenging because of the difficulty associated with breaking the identical chemical environment on nanoparticle surfaces. Here we demonstrate the selective blocking of nanoparticle surfaces with a diblock copolymer (polystyrene-b-polyacrylic acid). By tuning the interfacial free energies of a ternary system involving the nanoparticles, solvent and copolymer, controllable accessibilities to the nanoparticles’ surfaces are obtained. Through the modification of the polymer-free surface region with single-stranded DNA, regioselective and programmable surface encoding is realized. The resultant interparticle binding potential is selective and directional, allowing for an increased degree of complexity of potential self-assemblies. The versatility of this regioselective surface encoding strategy is demonstrated on various nanoparticles of isotropic or anisotropic shape and a total of 24 distinct complex nanoassemblies are fabricated.

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The data that support the findings of this study are available from the corresponding author upon reasonable request.

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Change history

  • 12 December 2018

    In the version of this Article originally published, the diblock copolymer structure in Fig. 2a showed a single bond between the carbon and the oxygen atoms; it should have been a double bond. This has been corrected in all versions of the Article.

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Acknowledgements

This work is supported by the University of Chicago and the NSF CAREER Award (DMR-1555361) to Y.W. D.L. acknowledges the Martha Ann and Joseph A. Chenicek Graduate Research Fund and HHMI International Student Research Fellowship. This research used resources of the Center for Functional Nanomaterials at Brookhaven National Laboratory, which is supported by US DOE Office of Science Facilities under Contract DE-SC0012704. O.G. gratefully acknowledges the support by the US Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under grant no. DE-SC0008772.

Author information

Author notes

    • Gang Chen

    Present address: Department of Chemistry, University of Central Florida, Orlando, FL, USA

  1. These authors contributed equally: Gang Chen, Kyle J. Gibson

Affiliations

  1. Department of Chemistry, The University of Chicago, Chicago, IL, USA

    • Gang Chen
    • , Kyle J. Gibson
    • , Di Liu
    • , Huw C. Rees
    • , Jung-Hoon Lee
    •  & Yossi Weizmann
  2. Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, NY, USA

    • Weiwei Xia
    • , Ruoqian Lin
    • , Huolin L. Xin
    •  & Oleg Gang
  3. Department of Chemical Engineering, Columbia University, New York, NY, USA

    • Oleg Gang
  4. Department of Applied Physics and Applied Mathematics, Columbia University, New York, NY, USA

    • Oleg Gang

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Contributions

G.C. and Y.W. conceived the idea. G.C. and D.L. designed the experiments and developed the methodology. During the revision, H.C.R. and K.J.G. helped with the NP synthesis, K.J.G. performed the polymer encapsulation and self-assemblies, J.-H.L. helped with the microscopy. W.X., R.L. and H.L.X. performed the microscopy for the 3D tomograms. H.L.X. and O.G. analysed the data for the 3D reconstructions. Y.W. supervised the project. G.C., D.L., K.J.G., H.C.R. and Y.W. analysed the data and wrote the paper.

Competing interests

The authors declare no competing interests.

Corresponding author

Correspondence to Yossi Weizmann.

Supplementary information

  1. Supplementary Information

    Supplementary Video Legends 1–6, Supplementary Figures 1–37, Supplementary Tables 1 and 2 and Supplementary References

  2. Supplementary Video 1

    3D tomographic reconstruction of v-AuNC partially encapsulated nanostructure

  3. Supplementary Video 2

    Full rotation of 3D tomographic reconstruction of c-AuNC self-assembly with AuNS

  4. Supplementary Video 3

    Full rotation of 3D tomographic reconstruction of c-AuNC partially encapsulated nanostructure

  5. Supplementary Video 4

    Half rotation at slower speed of 3D tomographic reconstruction of c-AuNC partially encapsulated nanostructure

  6. Supplementary Video 5

    3D tomographic reconstruction showing detailed surface structure of the c-AuNC through a sliding partition plane

  7. Supplementary Video 6

    Full rotation of 3D tomographic reconstruction of c-AuNC self-assembly with AuNS

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DOI

https://doi.org/10.1038/s41563-018-0231-1