Abstract
When a drop of a colloidal solution of nanoparticles dries on a surface, it leaves behind coffee-stain-like rings of material with lace-like patterns or clumps of particles in the interior1,2,3,4,5,6. These non-uniform mass distributions are manifestations of far-from-equilibrium effects, such as fluid flows1 and solvent fluctuations during late-stage drying2. However, recently a strikingly different drying regime promising highly uniform, long-range-ordered nanocrystal monolayers has been found7,8. Here we make direct, real-time and real-space observations of nanocrystal self-assembly to reveal the mechanism. We show how the morphology of drop-deposited nanoparticle films is controlled by evaporation kinetics and particle interactions with the liquid–air interface. In the presence of an attractive particle–interface interaction, rapid early-stage evaporation dynamically produces a two-dimensional solution of nanoparticles at the liquid–air interface, from which nanoparticle islands nucleate and grow. This self-assembly mechanism produces monolayers with exceptional long-range ordering that are compact over macroscopic areas, despite the far-from-equilibrium evaporation process. This new drop-drying regime is simple, robust and scalable, is insensitive to the substrate material and topography, and has a strong preference for forming monolayer films. As such, it stands out as an excellent candidate for the fabrication of technologically important ultra thin film materials for sensors, optical devices and magnetic storage media.
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Acknowledgements
We thank M. Constantinides and R. Diamond for their help with early experiments. This work was supported by the UC-ANL Consortium for Nanoscience Research and by the NSF MRSEC program under DMR 0213745. X.-M.L. acknowledges support from the US Department of Energy, Basic Energy Sciences-Materials Sciences, under Contract W-31-109-ENG-38.
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Bigioni, T., Lin, XM., Nguyen, T. et al. Kinetically driven self assembly of highly ordered nanoparticle monolayers. Nature Mater 5, 265–270 (2006). https://doi.org/10.1038/nmat1611
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DOI: https://doi.org/10.1038/nmat1611
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