Anomalous quantum confinement of the longitudinal optical phonon mode in PbSe quantum dots
Author(s) -
Justin Habinshuti,
Ondřej Kilián,
O. Cristini,
Aldona Sashchiuk,
Ahmed Addad,
S. Turrell,
Efrat Lifshitz,
B. Grandidier,
Ludger Wirtz
Publication year - 2013
Publication title -
physical review b
Language(s) - English
Resource type - Journals
eISSN - 1538-4489
pISSN - 1098-0121
DOI - 10.1103/physrevb.88.115313
Subject(s) - phonon , condensed matter physics , quantum dot , raman spectroscopy , overtone , radius , bohr radius , ab initio , nanocrystal , physics , materials science , molecular physics , spectral line , optics , exciton , quantum mechanics , computer security , computer science
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
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