In situ study of the formation mechanism of two-dimensional superlattices from PbSe nanocrystals

Jaco J. Geuchies, Carlo Van Overbeek, Wiel H. Evers, Bart Goris, Annick De Backer, Anjan P. Gantapara, Freddy T. Rabouw, Jan Hilhorst, Joep L. Peters, Oleg Konovalov, Andrei V. Petukhov, Marjolein Dijkstra, Laurens D A Siebbeles, Sandra Van Aert, Sara Bals, Daniel Vanmaekelbergh*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

163 Citations (Scopus)
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Oriented attachment of PbSe nanocubes can result in the formation of two-dimensional (2D) superstructures with long-range nanoscale and atomic order. This questions the applicability of classic models in which the superlattice grows by first forming a nucleus, followed by sequential irreversible attachment of nanocrystals, as one misaligned attachment would disrupt the 2D order beyond repair. Here, we demonstrate the formation mechanism of 2D PbSe superstructures with square geometry by using in situ grazing-incidence X-ray scattering (small angle and wide angle), ex situ electron microscopy, and Monte Carlo simulations. We observed nanocrystal adsorption at the liquid/gas interface, followed by the formation of a hexagonal nanocrystal monolayer. The hexagonal geometry transforms gradually through a pseudo-hexagonal phase into a phase with square order, driven by attractive interactions between the {100} planes perpendicular to the liquid substrate, which maximize facet-to-facet overlap. The nanocrystals then attach atomically via a necking process, resulting in 2D square superlattices.

Original languageEnglish
Pages (from-to)1248-1254
Number of pages7
JournalNature Materials
Issue number12
Publication statusPublished - 1 Dec 2016


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