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

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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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