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      Attractive versus repulsive excitonic interactions of colloidal quantum dots control blue-to red-shifting (and non-shifting) amplified spontaneous emission

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      Author(s)
      Cihan, A. F.
      Kelestemur, Y.
      Guzelturk, B.
      Yerli, O.
      Kurum, U.
      Yaglioglu, H. G.
      Elmali, A.
      Demir, Hilmi Volkan
      Date
      2013-11-21
      Source Title
      The Journal of Physical Chemistry Letters
      Print ISSN
      1948-7185
      Publisher
      American Chemical Society
      Volume
      4
      Issue
      23
      Pages
      4146 - 4152
      Language
      English
      Type
      Article
      Item Usage Stats
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      Abstract
      Tunable, high-performance, two-photon absorption (TPA)-based amplified spontaneous emission (ASE) from near-unity quantum efficiency colloidal quantum dots (CQDs) is reported. Besides the absolute spectral tuning of ASE, the relative spectral tuning of ASE peak with respect to spontaneous emission was shown through engineering excitonic interactions in quasi-type-II CdSe/CdS core/shell CQDs. With core shell size adjustments, it was revealed that Coulombic exciton-exciton interactions can be tuned to be attractive (type-I-like) or repulsive (type-II-like) leading to red- or blue-shifted ASE peak, respectively, and that nonshifting ASE can be achieved with the right core shell combinations. The possibility of obtaining ASE at a specific wavelength from both type-I-like and type-II-like CQDs was also demonstrated. The experimental observations were supported by parametric quantum-mechanical modeling, shedding light on the type-tunability. These excitonically engineered CQD-solids exhibited TPA-based ASE threshold as low as 6.5 mJ/cm(2) under 800 nm excitation, displaying one of the highest values of TPA cross-section of 44 660 GM.
      Keywords
      Inverted Core/shell Nanocrystals
      Semiconductor Nanocrystals
      Stimulated-emission
      Light Amplification
      Optical Gain
      Wave-guides
      Confinement
      Energy
      Dynamics
      Regime
      Permalink
      http://hdl.handle.net/11693/12383
      Published Version (Please cite this version)
      http://dx.doi.org/10.1021/jz402211m
      Collections
      • Department of Electrical and Electronics Engineering 3702
      • Department of Physics 2397
      • Institute of Materials Science and Nanotechnology (UNAM) 1930
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