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      Observation of selective plasmon-exciton coupling in nonradiative energy transfer: donor-selective versus acceptor-selective plexcitons

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      Author(s)
      Ozel, T.
      Hernandez-Martinez, P. L.
      Mutlugun, E.
      Akin, O.
      Nizamoglu, S.
      Ozel, I. O.
      Zhang, Q.
      Xiong, Q.
      Demir, Hilmi Volkan
      Date
      2013-06
      Source Title
      Nano Letters
      Print ISSN
      1530-6984
      Publisher
      American Chemical Society
      Volume
      13
      Issue
      7
      Pages
      3065 - 3072
      Language
      English
      Type
      Article
      Item Usage Stats
      370
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      535
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      Abstract
      We report selectively plasmon-mediated nonradiative energy transfer between quantum dot (QD) emitters interacting with each other via Forster-type resonance energy transfer (FRET) under controlled plasmon coupling either to only the donor QDs (i.e., donor-selective) or to only the acceptor QDs (i.e., acceptor-selective). Using layer-by-layer assembled colloidal QD nanocrystal solids with metal nanoparticles integrated at carefully designed spacing, we demonstrate the ability to enable/disable the coupled plasmon-exciton (plexciton) formation distinctly at the donor (exciton departing) site or at the acceptor (exciton feeding) site of our choice, while not hindering the donor exciton-acceptor exciton interaction but refraining from simultaneous coupling to both sites of the donor and the acceptor in the FRET process.. In the case of donor-selective plexciton, we observed a substantial shortening in the donor QD lifetime from 1.33 to 0.29 ns as a result of plasmon-coupling to the donors and the FRET-assisted exciton transfer from the donors to the acceptors, both of which shorten the donor lifetime. This consequently enhanced the acceptor emission by a factor of 1.93. On the other hand, in the complimentary case of acceptor-selective plexciton, we observed a 2.70-fold emission enhancement in the acceptor QDs, larger than the acceptor emission enhancement of the donor-selective plexciton, as a result of the combined effects of the acceptor plasmon coupling and the FRET-assisted exciton feeding. Here we present the comparative results of theoretical modeling of the donor- and acceptor-selective plexcitons of nonradiative energy transfer developed here for the first time, which are in excellent agreement with the systematic experimental characterization. Such an ability to modify and control energy transfer through mastering plexcitons is of fundamental importance, opening up new applications for quantum dot embedded plexciton devices along with the development of new techniques in FRET-based fluorescence microscopy.
      Keywords
      Localized Plasmons
      Nonradiative Energy Transfer
      Excitons
      Metal Nanoparticles
      Semiconductor Quantum Dots
      Plexcitons
      Layer-by-layer Assembly
      Permalink
      http://hdl.handle.net/11693/12141
      Published Version (Please cite this version)
      http://dx.doi.org/10.1021/nl4009106
      Collections
      • Department of Electrical and Electronics Engineering 4011
      • Department of Physics 2550
      • Institute of Materials Science and Nanotechnology (UNAM) 2256
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