Proceedings of nanoGe Fall Meeting 2021 (NFM21)
DOI: https://doi.org/10.29363/nanoge.nfm.2021.220
Publication date: 23rd September 2021
Colloidal nanocrystals of different metals, semiconductors, magnets, and other functional materials can self-assemble into long-range ordered crystalline and quasicrystalline phases. However, insulating organic ligands present at nanocrytal surfaces prevent the development of extended electronic states (minibands) in ordered supercrystalline materials. Here we report self-assembly of nanocrystals with compact and conductive inorganic ligands,6 with optical and electronic measurements confirming strong electronic coupling between neighboring nanocrystals and showing evidence of metallic transport. Structural characterization of the resulting all-inorganic assemblies reveals faceted supercrystalline structures with a high degree of internal crystalline order. The assembly of charge-stabilized nanocrystals can be rationalized and navigated using phase diagrams computed for spherical particles interacting through short range attractive potentials. nanocrystals with large static dielectric constants have a unique propensity to form long-range ordered structures because of image-charge induced ion structuring and short-range repulsive forces that prevent gelation and glass formation. The assembly occurs in proximity to a binodal line separating two metastable colloidal fluids, and the conditions can be tuned to enable either one-step nucleation of supercrystalline solids or non-classical two-step nucleation. We envision that the ability to grow all-inorganic long range ordered assemblies of strongly coupled nanoscale building blocks demonstrated in this work, combined with already available synthesis toolset for engineering nanocrystal size, shape, and functionality, will offer endless possibilities for engineering hierarchical solids.
This work was supported by the Office of Basic Energy Sciences, the U.S. Department of Energy, under Award No. DE-SC0019375, and by MICCoM, as part of the Computational Materials Sciences Program funded by the US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division, through Argonne National Laboratory, under contract DE-AC02-06CH11357. J. P. was supported as part of the Center for Advanced Materials for Energy Water Systems (AMEWS), an Energy Frontier Research Center funded by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES).
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