Efficient Radiative Pumping of Polaritons in a Strongly Coupled Microcavity by a Fluorescent Molecular Dye

  • Richard T. Grant
    Department of Physics and Astronomy The University of Sheffield Hicks Building, Hounsfield Road Sheffield S3 7RH UK
  • Paolo Michetti
    Institute of Theoretical Physics Technische Universität Dresden Zellescher Weg 17 01062 Dresden Germany
  • Andrew J. Musser
    Department of Physics and Astronomy The University of Sheffield Hicks Building, Hounsfield Road Sheffield S3 7RH UK
  • Pascal Gregoire
    Département de Physique Université de Montréal C.P. 6128, Succ. centre‐ville Montréal H3C 3J7 Canada
  • Tersilla Virgili
    IFN ISMAC and ISTM – CNR Milano Milan 20132 Italy
  • Eleonora Vella
    Département de Physique Université de Montréal C.P. 6128, Succ. centre‐ville Montréal H3C 3J7 Canada
  • Marco Cavazzini
    IFN ISMAC and ISTM – CNR Milano Milan 20132 Italy
  • Kyriacos Georgiou
    Department of Physics and Astronomy The University of Sheffield Hicks Building, Hounsfield Road Sheffield S3 7RH UK
  • Francesco Galeotti
    IFN ISMAC and ISTM – CNR Milano Milan 20132 Italy
  • Caspar Clark
    Helia Photonics Livingston EH54 7EJ UK
  • Jenny Clark
    Department of Physics and Astronomy The University of Sheffield Hicks Building, Hounsfield Road Sheffield S3 7RH UK
  • Carlos Silva
    Département de Physique Université de Montréal C.P. 6128, Succ. centre‐ville Montréal H3C 3J7 Canada
  • David G. Lidzey
    Department of Physics and Astronomy The University of Sheffield Hicks Building, Hounsfield Road Sheffield S3 7RH UK

抄録

<jats:p>The optical properties of a series of strongly coupled microcavities containing the fluorescent molecular dye BODIPY‐Br (bromine‐substituted boron‐dipyrromethene) dispersed into a transparent dielectric matrix are explored, with each cavity having a different exciton–photon detuning. Using temperature dependent emission, time‐resolved spectroscopy, white‐light reflectivity, and measurements of fluorescence quantum yield, the population of polaritons is explored along the lower polariton branch. It is found that both the cavity fluorescence quantum efficiency and the distribution of polariton states along the lower polariton branch is a function of exciton–photon detuning. Importantly, it is shown that in the most negatively detuned cavities, the emission quantum efficiency approaches that of a control (noncavity) film. A simple fitting model is developed, which is based upon direct radiative pumping of polariton states along the lower polariton branch and used it to obtain an excellent agreement with measured photoluminescence as a function of temperature and exciton–photon detuning, and qualitative agreement with the measured photoluminescence quantum efficiency. The radiative pumping mechanism indicates that to facilitate the formation of a nonequilibrium polariton condensate in strongly‐coupled microcavities containing dispersed molecular dyes, it is important to utilize materials having high fluorescent quantum efficiency and fast radiative rates.</jats:p>

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