Abstract
Surface plasmon polaritons (SPPs), optical excitations at the interface between a metal and a dielectric, carry significant potential for guiding and manipulating light on the nanoscale1,2,3. However, their weak optical nonlinearities hinder active device fabrication, for example, for all-optical switching4,5,6,7 or information processing8,9. Recently, strong optical dipole coupling has been demonstrated between SPPs and nonlinear quantum emitters with normal mode splittings of up to 700 meV (refs 1011121314–15). The predicted ultrafast energy transfer between quantum emitters and SPP fields could be a crucial microscopic mechanism for switching light by light on the nanoscale. Here, we present the first real-time observation of ultrafast Rabi oscillations in a J-aggregate/metal nanostructure, indicating coherent energy transfer between excitonic quantum emitters and SPP fields. We demonstrate coherent manipulation of the coupling energy by controlling the exciton density on a 10 fs timescale, which represents a step towards coherent, all-optical ultrafast plasmonic circuits and devices.
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Acknowledgements
The authors thank the Deutsche Forschungsgemeinschaft (SPP 1391 and DFG-NSF Materials World Network), Fondazione Cariplo (‘Engineering of optical nonlinearities in plasmonic metamaterials’), European Community (FP-7 INFRASTRUCTURES-2008-1, ‘Laserlab Europe II’, contract no. 228334 and FP-7 NMP ‘Cronos’) and the Korea Foundation for International Cooperation of Science and Technology (Global Research Laboratory project, K20815000003) for financial support. The authors also thank E. Sommer for preparing some of the figures.
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P.V., R.P., W.W. and C.L. designed and fabricated the hybrid nanostructures. All authors participated in conducting the experiments. R.P., P.V., W.W. and C.L. contributed to the theoretical modelling. All authors discussed the results and implications at all stages. P.V., R.P., G.C. and C.L. wrote the paper.
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Vasa, P., Wang, W., Pomraenke, R. et al. Real-time observation of ultrafast Rabi oscillations between excitons and plasmons in metal nanostructures with J-aggregates. Nature Photon 7, 128–132 (2013). https://doi.org/10.1038/nphoton.2012.340
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DOI: https://doi.org/10.1038/nphoton.2012.340
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