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Quantifying Angular Correlations between the Atomic Lattice and the Superlattice of Nanocrystals Assembled with Directional Linking

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Deutsches Elektronen-Synchrotron DESY, Notkestraße 85, D-22607 Hamburg, Germany
National Research Nuclear University MEPhI (Moscow Engineering Physics Institute), Kashirskoe shosse 31, 115409 Moscow, Russia
§ European XFEL GmbH, Holzkoppel 4, D-22869 Schenefeld, Germany
Eberhard Karls Universität Tübingen, Geschwister-Scholl-Platz, D-72074 Tübingen, Germany
Cite this: Nano Lett. 2017, 17, 6, 3511–3517
Publication Date (Web):May 9, 2017
Copyright © 2017 American Chemical Society

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    We show that the combination of X-ray scattering with a nanofocused beam and X-ray cross correlation analysis is an efficient way for the full structural characterization of mesocrystalline nanoparticle assemblies with a single experiment. We analyze several hundred diffraction patterns at individual sample locations, that is, individual grains, to obtain a meaningful statistical distribution of the superlattice and atomic lattice ordering. Simultaneous small- and wide-angle X-ray scattering of the same sample location allows us to determine the structure and orientation of the superlattice as well as the angular correlation of the first two Bragg peaks of the atomic lattices, their orientation with respect to the superlattice, and the average orientational misfit due to local structural disorder. This experiment is particularly advantageous for synthetic mesocrystals made by the simultaneous self-assembly of nanocrystals and surface-functionalization with conductive ligands. While the structural characterization of such materials has been challenging so far, the present method now allows correlating the mesocrystalline structure with optoelectronic properties.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.nanolett.7b00584.

    • Description of the sample preparation, details of the X-ray scattering experiment, the X-ray cross-correlation analysis, the evaluation of the model cross-correlation function, and a comment on the effect of orientational disorder between atomic lattices. Figure S1: Analysis of the angular averaged signal in SAXS region. Figure S2: Evaluation of the angle 2β between two {112}SL peaks for the bct structure. Figure S3: Spatially resolved map of misorientation between the superlattice and atomic lattice. Figure S4: Illustration of the effect of atomic disorder in reciprocal space (PDF)

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