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On the Formation of Honeycomb Superlattices from PbSe Quantum Dots: The Role of Solvent-Mediated Repulsion and Facet-to-Facet Attraction in NC Self-Assembly and Alignment.
van der Sluijs, Maaike M; Sanders, Dinja; Jansen, Kevin J; Soligno, Giuseppe; Vanmaekelbergh, Daniel; Peters, Joep L.
Afiliación
  • van der Sluijs MM; Condensed Matter and Interfaces, Debye Institute for Nanomaterials Science, University of Utrecht, Princetonplein 1, 3584 CC Utrecht, The Netherlands.
  • Sanders D; Condensed Matter and Interfaces, Debye Institute for Nanomaterials Science, University of Utrecht, Princetonplein 1, 3584 CC Utrecht, The Netherlands.
  • Jansen KJ; Condensed Matter and Interfaces, Debye Institute for Nanomaterials Science, University of Utrecht, Princetonplein 1, 3584 CC Utrecht, The Netherlands.
  • Soligno G; Condensed Matter and Interfaces, Debye Institute for Nanomaterials Science, University of Utrecht, Princetonplein 1, 3584 CC Utrecht, The Netherlands.
  • Vanmaekelbergh D; Condensed Matter and Interfaces, Debye Institute for Nanomaterials Science, University of Utrecht, Princetonplein 1, 3584 CC Utrecht, The Netherlands.
  • Peters JL; Condensed Matter and Interfaces, Debye Institute for Nanomaterials Science, University of Utrecht, Princetonplein 1, 3584 CC Utrecht, The Netherlands.
J Phys Chem C Nanomater Interfaces ; 126(2): 986-996, 2022 Jan 20.
Article en En | MEDLINE | ID: mdl-35087608
Semiconductor superstructures made from assembled and epitaxially connected colloidal nanocrystals (NCs) hold promise for crystalline solids with atomic and nanoscale periodicity, whereby the band structure can be tuned by the geometry. The formation of especially the honeycomb superstructure on a liquid substrate is far from understood and suffers from weak replicability. Here, we introduce 1,4-butanediol as an unreactive substrate component, which is mixed with reactive ethylene glycol to tune for optimal reactivity. It shows us that the honeycomb superlattice has a NC precursor state before oriented attachment occurs, in the form of a self-assembled hexagonal bilayer. We propose that the difference between the formation of the square or honeycomb superstructure occurs during the self-assembly phase. To form a honeycomb superstructure, it is crucial to stabilize the hexagonal bilayer in the presence of solvent-mediated repulsion. In contrast, a square superstructure benefits from the contraction of a hexagonal monolayer due to the absence of a solvent. A second experiment shows the very last stage of the process, where the increasing alignment of NCs is quantified using selected-area electron diffraction (SAED). The combination of transmission electron microscopy (TEM), SAED, and tomography used in these experiments shows that the (100)/(100) facet-to-facet attraction is the main driving force for NC alignment and attachment. These findings are validated by coarse-grained molecular dynamic simulations, where we show that an optimal NC repulsion is crucial to create the honeycomb superstructure.

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Phys Chem C Nanomater Interfaces Año: 2022 Tipo del documento: Article País de afiliación: Países Bajos Pais de publicación: Estados Unidos

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Phys Chem C Nanomater Interfaces Año: 2022 Tipo del documento: Article País de afiliación: Países Bajos Pais de publicación: Estados Unidos