Proceedings of nanoGe Fall Meeting 2018 (NFM18)
DOI: https://doi.org/10.29363/nanoge.nfm.2018.021
Publication date: 6th July 2018
Ultrathin colloidal semiconductor nanosheets with thickness in the strong quantum confinement regime are of particular interest, since they combine the extraordinary properties of 2D nanomaterials with versatility in terms of composition, size, shape, and surface control, and the prospects of solution processability. However, synthesis procedures for materials other than the prototypical Pb- and Cd- chalcogenides are still underdeveloped. Compound Cu-chalcogenides are an interesting class of materials, which have been attracting increasing attention as alternatives to Cd- and Pb-chalcogenides, since they have low toxicity, potentially lower costs, and a very wide range of compositions. This latter point makes them extremely versatile, capable not only of offering similar properties to those already demonstrated by Cd- and Pb-chalcogenide nanocrystals (such as PL tunability in the visible to NIR spectral range and high absorption coefficients), but also unprecedented features, such as plasmon resonances.
In this talk, we discuss recent work by our group on ultrathin (~2nm thick) nanosheets of both binary (Cu2-xA and Cu2-xA, A= S, Se) and ternary (CuInA2 and CuInA2) Cu-chalcogenides, with well-defined shape (triangular or hexagonal) and dimensions in the ~100 nm to ~1 µm range. The binary nanosheets form through 2D-constrained stack-templated nucleation and growth. The 2D-constraints are imposed by halide-stabilized lamellar Cu-thiolate (or Cu-selenoate) supramolecular complexes that act as soft-templates. Covellite Cu-rich CuInS2 nanosheets form via self-organization and oriented attachment of chalcopyrite CuInS2 nanocrystals, which is induced by a sudden change in the composition of the nanocrystal building blocks due to preferential extraction of In3+ by in-situ generated H2S. Primary amines play several essential roles in the formation of these nanosheets. CuInA2 nanosheets are also obtained by partial self-limited cation exchange in Cu2-xSe or In2S3 template nanosheets. Moreover, the charge carrier dynamics in ultrathin Cu2-xS nanosheets is studied with THz spectroscopy.
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