Journal
ACS NANO
Volume 7, Issue 8, Pages 7352-7369Publisher
AMER CHEMICAL SOC
DOI: 10.1021/nn403035s
Keywords
colloidal nanocrystals; copper sulfide; covellite; shape control; localized surface plasmon resonance; discrete dipole approximation; transient absorption spectroscopy
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Funding
- Italian Ministry of Education, University and Research through project AEROCOMP [DM48391]
- Fondazione Cariplo [2010-0612]
- European Research Council (ERC) [207441]
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In the realm of semiconductor nanomaterials, a crystal lattice heavily doped with cation/anion vacancies or ionized atomic impurities is considered to be a general prerequisite to accommodating excess free carriers that can support localized surface plasmon resonance (LSPR). Here, we demonstrate a surfactant-assisted nonaqueous route to anisotropic copper sulfide nanocrystals, selectively trapped in the covellite phase, which can exhibit intense, size-tunable LSPR at near-infrared wavelengths despite their stoichiometric, undoped structure. Experimental extinction spectra are satisfactorily reproduced by theoretical calculations performed by the discrete dipole approximation method within the framework of the Drude-Sommerfeld model. The LSPR response of the nanocrystals and its geometry dependence are interpreted as arising from the inherent metallic-like character of covellite, allowed by a significant density of lattice-constitutional valence-band free holes. As a consequence of the unique electronic properties of the nanocrystals and of their monodispersity, coherent excitation of symmetric radial breathing modes is observed for the first time in transient absorption experiments at LSPR wavelengths.
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