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One- and Two-Photon Absorption in CdS Nanodots and Wires: The Role of Dimensionality in the One- and Two-Photon Luminescence Excitation Spectrum

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    One- and Two-Photon Absorption in CdS Nanodots and Wires: The Role of Dimensionality in the One- and Two-Photon Luminescence Excitation Spectrum
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    ‡ Institute of Optics and Atomic Physics, Technical University of Berlin, Strasse des 17. Juni 135, 10623 Berlin, Germany
    ∥ Departament de Quimica Fisicai Analitica, Universitat Jaume I, Castelló de la Plana 12080, Spain
    # Institute for Physico-Chemical Problems, Belarusian State University, 220030 Minsk, Belarus
    * E-mail:[email protected]
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    The Journal of Physical Chemistry C

    Cite this: J. Phys. Chem. C 2015, 119, 2, 1260–1267
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    https://doi.org/10.1021/jp511346w
    Published December 18, 2014
    Copyright © 2014 American Chemical Society
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    Abstract

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    We investigate the spectral dependence of the linear and two-photon absorption of wurtzite CdS nanoparticles (dots and rods) by means of quantitative one- and two-photon photoluminescence excitation spectroscopy and effective mass theory modeling. Absolute two-photon absorption cross sections free from spectrally varying beam related uncertainties are obtained by means of a new reference dye-based method. The two-photon spectrum features of rods strongly differ from those of dots, due to the distinct energy structure of quasi-one-dimensional systems. The transversal confinement is found to dominate the energy of the absorption maxima while the longitudinal one dominates their absorption intensity. This suggests two-photon transition energy and intensity can be controlled independently in nanorods. For both geometries we observe a sizable spectral shift between the first one- and two-photon absorption maxima, which we conclude is inherent to the small rates of near-bandgap two-photon transitions rather than to the particular geometry of the absorber. The provided understanding of the spectral dependence of the two-photon absorption of CdS dots and rods is of strong interest for the design of nanocrystals with optimized two-photon absorption properties for bioimaging and phototherapy applications.

    Copyright © 2014 American Chemical Society

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    Details on the TP-PLE and ensemble calculations of the linear and two-photon absorption spectra. This material is available free of charge via the Internet at http://pubs.acs.org.

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    The Journal of Physical Chemistry C

    Cite this: J. Phys. Chem. C 2015, 119, 2, 1260–1267
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jp511346w
    Published December 18, 2014
    Copyright © 2014 American Chemical Society
    Request reuse permissions

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