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J Am Chem Soc. 2019 Apr 10;141(14):6013-6021. doi: 10.1021/jacs.9b01033. Epub 2019 Apr 1.

Controlling Nanoparticle Orientations in the Self-Assembly of Patchy Quantum Dot-Gold Heterostructural Nanocrystals.

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Department of Chemistry , Brown University , Providence , Rhode Island 02912 , United States.
Department of Chemistry , University of Utah , Salt Lake City , Utah 84112 , United States.
Department of Material Science and Engineering , University of Florida , Gainesville , Florida 32611 , United States.
Max Planck Institute for the Structure and Dynamics of Matter , Hamburg 22761 , Germany.
Heinrich Petter Institute-Leibniz Institute for Experimental Virology , Hamburg 20251 , Germany.
Center for Nanoscale Materials , Argonne National Laboratory , Argonne , Illinois 60439 , United States.
Department of Chemistry , University of Connecticut , Storrs , Connecticut 06269 , United States.
National Synchrotron Light Source II , Brookhaven National Laboratory , Upton , New York 11973 , United States.
Cornell High Energy Synchrotron Source , Cornell University , Ithaca , New York 14853 , United States.


Self-assembly of nanocrystals is a promising route for creating macroscale materials that derive function from the properties of their nanoscale building blocks. While much progress has been made assembling nanocrystals into different superlattices, controlling the relative orientations of nanocrystals in those lattices remains a challenge. Here, we combine experiments with computer simulations to study the self-assembly of patchy heterostructural nanocrystals (HNCs), consisting of near-spherical quantum dots decorated with regular arrangements of small gold satellites, into close-packed superlattices with pronounced orientational alignment of HNCs. Our simulations indicate that the orientational alignment is caused by van der Waals interactions between gold patches and is sensitive to the interparticle distance in the superlattice. We demonstrate experimentally that the degree and type of orientational alignment can be controlled by changing ligand populations on HNCs. This study provides guidance for the design and fabrication of nanocrystal superlattices with enhanced structural control.


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