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Tailoring hot-exciton emission and lifetimes in semiconducting nanowires via whispering-gallery nanocavity plasmons

Nature Materials volume 10, pages 669–675 (2011)Cite this article

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Abstract

The manipulation of radiative properties of light emitters coupledwith surface plasmons is important for engineering new nanoscale optoelectronic devices, including lasers, detectorsand single photon emitters1,2,3,4,5,6,7,8. However, so far the radiative rates of excited states in semiconductors and molecular systems have been enhanced only moderately, typically by a factor of 10–50, producing emission mostly from thermalizedexcitons2,6,9,10,11. Here, we show the generation of dominant hot-exciton emission, that is, luminescence from non-thermalized excitons that are enhanced by the highly concentrated electromagnetic fields supported by the resonant whispering-gallery plasmonic nanocavities of CdS–SiO2–Ag core–shell nanowire devices. By tuning the plasmonic cavity size to match the whispering-gallery resonances, an almost complete transition from thermalized exciton to hot-exciton emission can be achieved, which reflects exceptionally high radiative rate enhancement of >103 and sub-picosecond lifetimes. Core–shell plasmonic nanowires are an ideal test bed for studying and controlling strong plasmon–exciton interaction at the nanoscale and opens new avenues for applications in ultrafast nanophotonic devices.

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Figure 1: Core–shell nanowire plasmonic nanocavity.
Figure 2: Hot-exciton emission from plasmonic nanowires.
Figure 3: Temperature- and polarization-dependent properties of the hot-exciton emission.
Figure 4: Size-dependent properties of the whispering-gallery plasmon nanocavity.

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Acknowledgements

We thank N. Engheta for discussions and A. Exarhos for helping to build the optical Kerr gate system. Time-resolved photoluminescence work was supported by the Department of Energy BES under Award No. DESC0002158. The remaining work was supported by the US Army Research Office under Grant No. W911NF-09-1-0477, National Institutes of Health through the NIH Director’s New Innovator Award Program, 1-DP2-7251-01, and the Nano/Bio Interface Center through NSF-NSEC-DMR08-32802. C.O.A. is supported by the NBIC through the NSF IGERT DGE02-21664.

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Authors and Affiliations

  1. Department of Materials Science and Engineering, University of Pennsylvania, Philadelphia, Pennsylvania 19104, USA

    Chang-Hee Cho, Carlos O. Aspetti, Sung-Wook Nam & Ritesh Agarwal

  2. Department of Physics and Astronomy, University of Pennsylvania, Philadelphia, Pennsylvania 19104, USA

    Michael E. Turk & James M. Kikkawa

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  1. Chang-Hee Cho
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  2. Carlos O. Aspetti
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Contributions

C-H.C. and R.A. developed the concept and design of the devices. C-H.C. carried out the device fabrication and steady-state optical measurements. C.O.A. performed the numerical simulations. M.E.T. and J.M.K. performed the time-resolved photoluminescence measurements. S-W.N. performed the transmission electron microscope measurement. C-H.C., C.O.A. and R.A. analysed the results and wrote the manuscript.

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Correspondence to Ritesh Agarwal.

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Cho, CH., Aspetti, C., Turk, M. et al. Tailoring hot-exciton emission and lifetimes in semiconducting nanowires via whispering-gallery nanocavity plasmons. Nature Mater 10, 669–675 (2011). https://doi.org/10.1038/nmat3067

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