Hotspot-mediated non-dissipative and ultrafast plasmon passage

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Abstract

Plasmonic nanoparticles hold great promise as photon handling elements and as channels for coherent transfer of energy and information in future all-optical computing devices1,2,3,4,5. Coherent energy oscillations between two spatially separated plasmonic entities via a virtual middle state exemplify electron-based population transfer, but their realization requires precise nanoscale positioning of heterogeneous particles6,7,8,9,10. Here, we show the assembly and optical analysis of a triple-particle system consisting of two gold nanoparticles with an inter-spaced silver island. We observe strong plasmonic coupling between the spatially separated gold particles, mediated by the connecting silver particle, with almost no dissipation of energy. As the excitation energy of the silver island exceeds that of the gold particles, only quasi-occupation of the silver transfer channel is possible. We describe this effect both with exact classical electrodynamic modelling and qualitative quantum-mechanical calculations. We identify the formation of strong hotspots between all particles as the main mechanism for the lossless coupling and thus coherent ultrafast energy transfer between the remote partners. Our findings could prove useful for quantum gate operations, as well as for classical charge and information transfer processes.

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Figure 1: Plasmonic transfer system.
Figure 2: Dark-field scattering spectra and simulations of the plasmonic transfer system.
Figure 3: Polarization-resolved measurements and calculations.
Figure 4: Full electromagnetic simulations of the plasmon transfer dynamics.
Figure 5: Quantum model.

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Acknowledgements

This work was funded by the Volkswagen Foundation, the DFG through the Nanosystems Initiative Munich (NIM), through the ERC Starting Grant ORCA (GA No: 336440). A.O.G. and L.V.B. acknowledge additional support from the US Army Research Office (W911NF-12-1-0407).

Author information

E.-M.R., A.O.G. and T.L. conceived the experiments and co-wrote the manuscript. E.-M.R. designed the structure and analysed the data. E.-M.R. and C.P. performed the experiments. L.V.B. and L.K.K. performed the simulations, A.O.G. developed the quantum model. All authors contributed to the interpretation and general discussion and reviewed the manuscript.

Correspondence to Alexander O. Govorov or Tim Liedl.

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The authors declare no competing financial interests.

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Roller, E., Besteiro, L., Pupp, C. et al. Hotspot-mediated non-dissipative and ultrafast plasmon passage. Nature Phys 13, 761–765 (2017) doi:10.1038/nphys4120

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