The phenomena of localized surface plasmon resonances (LSPRs) has been broadly studied and is a property of nanomaterials that can be used to enhance or enable a wide variety of technologies including cancer treatment, light-driven catalysis, and ultrasensitive detection. While most widely-observed and studied in noble metal nanomaterials, a much broader selection of nanoscale materials may exhibit LSPRs. Recently, degenerately doped colloidal semiconductor nanoparticles have been identified as one such class of alternative plasmonic nanomaterials. Unlike their noble metal counterparts, a powerful way to tune plasmonic properties of doped semiconductor nanoparticles is by controlling their charge carrier density. Therefore, methods to control and measure carrier density in these materials is crucial to their development and design. Both extrinsic and intrinsic particle features may be manipulated to alter carrier densities, and the resulting concentrations are typically measured using a Drude model interpretation of the particle extinction spectrum. Here, we track and quantify carrier density in a well-studied non-noble metal plasmonic system, copper selenide (Cu2-xSe), using 77Se solid state NMR spin lattice relaxation measurements as a function of particle oxidation. Further, 77Se NMR simultaneously provides critical information about the structural evolution of these particles as a function of progressive oxidation. Importantly, we find that 77Se NMR spectroscopy is a sensitive technique able to identify and measure carrier density in Cu2-xSe systems that are metallic, but that do not yet show optically discernable plasmonic features.

Correlating carrier density and emergent plasmonic features in Cu2-xSe nanoparticles

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.