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Probing the mechanisms of large Purcell enhancement in plasmonic nanoantennas

Abstract

To move nanophotonic devices such as lasers and single-photon sources into the practical realm, a challenging list of requirements must be met, including directional emission1,2,3,4,5, room-temperature and broadband operation6,7,8,9, high radiative quantum efficiency1,4 and a large spontaneous emission rate7. To achieve these features simultaneously, a platform is needed for which the various decay channels of embedded emitters can be fully understood and controlled. Here, we show that all these device requirements can be satisfied by a film-coupled metal nanocube system with emitters embedded in the dielectric gap region. Fluorescence lifetime measurements on ensembles of emitters reveal spontaneous emission rate enhancements exceeding 1,000 while maintaining high quantum efficiency (>0.5) and directional emission (84% collection efficiency). Using angle-resolved fluorescence measurements, we independently determine the orientations of emission dipoles in the nanoscale gap. Incorporating this information with the three-dimensional spatial distribution of dipoles into full-wave simulations predicts time-resolved emission in excellent agreement with experiments.

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Figure 1: Directional plasmonic nanopatch antenna.
Figure 2: Experimental demonstration of large spontaneous emission rate enhancement.
Figure 3: Gap thickness dependence of spontaneous emission rates.
Figure 4: Fluorescence intensity enhancement with high quantum efficiency.

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Acknowledgements

The authors thank A. Rose, R. Hill and A. Baron for discussions. This work was supported by the Lord Foundation of North Carolina and the Air Force Office of Scientific Research (contract no. FA9550-12-1-0491).

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Contributions

G.M.A. and M.H.M. conceived and designed the experiments. G.M.A. performed the experiments. C.A., G.M.A. and C.C. performed the simulations. G.M.A., C.A. and M.H.M. analysed the data. T.B.H. synthesized the Ag nanocubes. G.M.A., T.B.H., C.F. and J.H. fabricated and characterized the samples. G.M.A., C.A. and M.H.M. wrote the manuscript with input from all authors. M.H.M. and D.R.S. supervised the project.

Corresponding author

Correspondence to Maiken H. Mikkelsen.

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The authors declare no competing financial interests.

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Akselrod, G., Argyropoulos, C., Hoang, T. et al. Probing the mechanisms of large Purcell enhancement in plasmonic nanoantennas. Nature Photon 8, 835–840 (2014). https://doi.org/10.1038/nphoton.2014.228

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