Role of Symmetry Breaking on the Optical Transitions in Lead-Salt Quantum Dots

Authors

    Authors

    G. Nootz; L. A. Padilha; P. D. Olszak; S. Webster; D. J. Hagan; E. W. Van Stryland; L. Levina; V. Sukhovatkin; L. Brzozowski;E. H. Sargent

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    Abbreviated Journal Title

    Nano Lett.

    Keywords

    Quantum-dots; two-photon absorption; inversion symmetry; selection; rules; nonlinear spectroscopy; PBSE NANOCRYSTALS; ELECTRONIC-STRUCTURE; Chemistry, Multidisciplinary; Chemistry, Physical; Nanoscience &; Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed Matter

    Abstract

    The influence of quantum confinement on the one- and two-photon absorption spectra (1PA and 2PA) of PbS and PbSe semiconductor quantum dots (QDs) is investigated. The results show 2PA peaks at energies where only 1PA transitions are predicted and 1PA peaks where only 2PA transitions are predicted by the often used isotropic k.p four-band envelope function formalism. The first experimentally identified two-photon absorption peak coincides with the energy:of the first one photon allowed transition. This first two photon peak cannot be explained by band anisotropy, verifying that the inversion symmetry of the wave functions is broken and relaxation of the parity selection rules has to be taken into account to explain optical transitions in lead-salt QDs. Thus, while the band anisotropy of the bulk semiconductor plays a role in the absorption spectra, especially for the more anisotropic PbSe QDs, a complete model of the absorption spectra, for both 1PA and 2PA, must also include symmetry breaking of the quantum confined wave functions. These studies clarify the controversy of the origin of spectral features in lead-salt QDs.

    Journal Title

    Nano Letters

    Volume

    10

    Issue/Number

    9

    Publication Date

    1-1-2010

    Document Type

    Article

    Language

    English

    First Page

    3577

    Last Page

    3582

    WOS Identifier

    WOS:000281498200061

    ISSN

    1530-6984

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