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

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    Type
    Article
    Authors
    Nootz, Gero
    Padilha, Lazaro A.
    Olszak, Peter D.
    Webster, Scott
    Hagan, David J.
    Van Stryland, Eric W.
    Levina, Larissa
    Sukhovatkin, Vlad
    Brzozowski, Lukasz
    Sargent, Edward H. cc
    KAUST Grant Number
    KUS-I1-009-21
    Date
    2010-09-08
    Permanent link to this record
    http://hdl.handle.net/10754/599534
    
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    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. © 2010 American Chemical Society.
    Citation
    Nootz G, Padilha LA, Olszak PD, Webster S, Hagan DJ, et al. (2010) Role of Symmetry Breaking on the Optical Transitions in Lead-Salt Quantum Dots. Nano Lett 10: 3577–3582. Available: http://dx.doi.org/10.1021/nl1018673.
    Sponsors
    This material is based upon work supported in part by the U.S. Army Research Office under Contract/Grant 50372-CH-MUR, the Air Force Office of Sponsored Research MURI AFOSR Grant FA9550-06-1-0337, the DARPA ZOE program Grant W31R4Q-09-1-0012, and the Israel Ministry of Defense contract 993/54250-01 and by Award No. KUS-I1-009-21, made by King Abdullah University of Science and Technology (KAUST). We also would like to thank Frank W. Wise for helpful discussions.
    Publisher
    American Chemical Society (ACS)
    Journal
    Nano Letters
    DOI
    10.1021/nl1018673
    PubMed ID
    20734976
    ae974a485f413a2113503eed53cd6c53
    10.1021/nl1018673
    Scopus Count
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