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Single-crystal Winterbottom constructions of nanoparticle superlattices


Colloidal nanoparticle assembly methods can serve as ideal models to explore the fundamentals of homogeneous crystallization phenomena, as interparticle interactions can be readily tuned to modify crystal nucleation and growth. However, heterogeneous crystallization at interfaces is often more challenging to control, as it requires that both interparticle and particle–surface interactions be manipulated simultaneously. Here, we demonstrate how programmable DNA hybridization enables the formation of single-crystal Winterbottom constructions of substrate-bound nanoparticle superlattices with defined sizes, shapes, orientations and degrees of anisotropy. Additionally, we show that some crystals exhibit deviations from their predicted Winterbottom structures due to an additional growth pathway that is not typically observed in atomic crystals, providing insight into the differences between this model system and other atomic or molecular crystals. By precisely tailoring both interparticle and particle–surface potentials, we therefore can use this model to both understand and rationally control the complex process of interfacial crystallization.

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Fig. 1: Substrate growth of crystals into Winterbottom shapes.
Fig. 2: Salt concentration effects on crystal growth.
Fig. 3: DNA loading effects on Winterbottom shape.
Fig. 4: Deviations from Winterbottom construction.
Fig. 5: Fcc and AlB2 crystal growth on substrates.

Data availability

The data supporting the findings of this study are available within this article and its Supplementary Information. SEM images used to create datasets are available at


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Fabrication of substrates was performed at the Materials Technology Laboratory at MIT. AFM and SEM characterization were performed at Draper. D.J.L. was supported by a Draper Fellowship. L.Z.Z. acknowledges support from the National Science Foundation Graduate Research Fellowship Program under grant no. NSF 1122374. We thank P.J. Santos for production of the gold nanoparticles used in this work. This work was supported by the following awards: the Air Force Office of Scientific Research’s Young Investigator Research Program (grant no. FA9550–17–1–0288); the Defense Advanced Research Projects Agency and the Office of Naval Research (contract no. FA8650-15-C-7543); the US Army Research Office under cooperative agreement no. W911NF-19-2-0026 for the Institute for Collaborative Biotechnologies.

Author information




Experiments were designed by D.J.L., D.J.D.C. and R.J.M. D.J.L. conducted experiments. D.J.L. and L.Z.Z. performed data analysis. D.J.L., L.Z.Z., D.J.D.C. and R.J.M. wrote the manuscript.

Corresponding author

Correspondence to Robert J. Macfarlane.

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The authors declare no competing interests.

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Supplementary information

Supplementary information

Supplementary methods, Notes 1 and 2, Figs. 1–20, Table 1 and references.

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Lewis, D.J., Zornberg, L.Z., Carter, D.J.D. et al. Single-crystal Winterbottom constructions of nanoparticle superlattices. Nat. Mater. 19, 719–724 (2020).

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