We have investigated the diameter dependence of the Raman spectra of lead selenide nanocrystals. The first-order Raman peak at about 136 cm −1 and its second-order overtone at twice this wavenumber move up in energy with decreasing nanocrystal diameter. This anomalous behavior is interpreted in terms of quantum confinement of the longitudinal optical (LO) phonon whose frequency displays a minimum at in the dispersion of bulk PbSe. We perform ab initio calculations of the phonons of PbSe slabs with up to 15 layers. The LO mode perpendicular to the slab shifts indeed upwards with decreasing layer thickness, thus validating the interpretation of the anomalous radius dependence of the Raman spectra in terms of quantum confinement.
Semiconductor PbSe/CdSe core-shell nanocrystals (NCs) in a double barrier tunnel junction have been investigated by means of scanning tunneling spectroscopy at low temperature. From the analysis of the differential conductance peak position as a function of the potential distribution in both potential barriers, we demonstrate a unipolar transport regime for a large amount of NCs. The same charge carriers are injected on both sides of the zero-conductance gap, and the peaks observed at higher energy arise from the charging of the NCs. Similar results are obtained for CdSe/CdS dot-in-rod NCs, indicating that the addition of a shell favors transitions between different charge states rather than single particle excited states. Further characterization of the PbSe/CdSe core-shell NCs by x-ray photoemission spectroscopy reveals that the variations in the transport properties from NC to NC are explained by the occurrence of unprotected PbSe facets that have different orientations in the junction.
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