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Polariton-mediated energy transfer between organic dyes in a strongly coupled optical microcavity

Nature Materials volume 13, pages 712–719 (2014)Cite this article

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Abstract

Strongly coupled optical microcavities containing different exciton states permit the creation of hybrid-polariton modes that can be described in terms of a linear admixture of cavity-photon and the constituent excitons. Such hybrid states have been predicted to have optical properties that are different from their constituent parts, making them a test bed for the exploration of light–matter coupling. Here, we use strong coupling in an optical microcavity to mix the electronic transitions of two J-aggregated molecular dyes and use both non-resonant photoluminescence emission and photoluminescence excitation spectroscopy to show that hybrid-polariton states act as an efficient and ultrafast energy-transfer pathway between the two exciton states. We argue that this type of structure may act as a model system to study energy-transfer processes in biological light-harvesting complexes.

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Figure 1: Microcavity structure supporting hybrid organic polaritons.
Figure 2: Characterization of the individual J-aggregates and a blended film.
Figure 3: Hybrid-polariton emission, population and mixing coefficients.
Figure 4: Angle- and wavelength-dependent PLE of the k∥ = 0 LPB state, polariton absorption and relative relaxation efficiency into the LPB ground state.
Figure 5: Modelling of the polariton emission.

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Acknowledgements

We gratefully acknowledge R.T. Grant for the atomic force micrographs presented in the Supplementary Information. We acknowledge financial support for the work via the UK EPSRC through grant EP/G062404/1 and by the European Union through the FP7 funded project Icarus (237900).

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Author notes

  1. David M. Coles

    Present address: Present address: Department of Materials, University of Oxford, Parks Road, Oxford OX1 3PH, UK.,

Authors and Affiliations

  1. Department of Physics and Astronomy, University of Sheffield, Hicks Building, Hounsfield Road, Sheffield S3 7RH, UK

    David M. Coles & David G. Lidzey

  2. School of Physics and Astronomy, University of Southampton, Southampton SO17 1BJ, UK

    Niccolo Somaschi & Pavlos G. Lagoudakis

  3. IESL-FORTH, PO Box 1527, 71110 Heraklion, Crete, Greece

    Niccolo Somaschi

  4. Institute of Theoretical Physics, Technische Universität Dresden, 01062 Dresden, Germany

    Paolo Michetti

  5. Helia Photonics, Rosebank Park, Livingston EH54 7EJ, UK

    Caspar Clark

  6. IESL-FORTH, PO Box 1527, 71110 Heraklion, Crete, Greece

    Pavlos G. Savvidis

  7. Department of Materials Science and Technology, University of Crete, 71003 Heraklion, Crete, Greece

    Pavlos G. Savvidis

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Contributions

D.G.L. and D.M.C. conceived the experiment. Samples were prepared by C.C. and D.M.C. Steady-state measurements were performed by D.M.C. N.S. performed time-resolved measurements under the supervision of P.G.L. and P.G.S. The model was developed by P.M. All authors contributed to the interpretation of results and preparation of the manuscript.

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Correspondence to David G. Lidzey.

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The authors declare no competing financial interests.

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Coles, D., Somaschi, N., Michetti, P. et al. Polariton-mediated energy transfer between organic dyes in a strongly coupled optical microcavity. Nature Mater 13, 712–719 (2014). https://doi.org/10.1038/nmat3950

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