Multi-phonon Raman scattering in semiconductor nanocrystals: importance of non-adiabatic transitions

Physics – Condensed Matter – Mesoscale and Nanoscale Physics

Scientific paper

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16 pages, 2 figures, E-mail addresses: devreese@uia.ua.ac.be, fomin@uia.ua.ac.be, fwise@ccmr.cornell.edu, accepted for publica

Scientific paper

10.1103/PhysRevB.65.075316

Multi-phonon Raman scattering in semiconductor nanocrystals is treated taking into account both adiabatic and non-adiabatic phonon-assisted optical transitions. Because phonons of various symmetries are involved in scattering processes, there is a considerable enhancement of intensities of multi-phonon peaks in nanocrystal Raman spectra. Cases of strong and weak band mixing are considered in detail. In the first case, fundamental scattering takes place via internal electron-hole states and is participated by s- and d-phonons, while in the second case, when the intensity of the one-phonon Raman peak is strongly influenced by the interaction of an electron and of a hole with interface imperfections (e. g., with trapped charge), p-phonons are most active. Calculations of Raman scattering spectra for CdSe and PbS nanocrystals give a good quantitative agreement with recent experimental results.

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