Vectorial near-field coupling

Abstract

The coherent exchange of optical near fields between two neighbouring dipoles plays an essential role in the optical properties, quantum dynamics and thus the function of many naturally occurring and artificial nanosystems. These interactions are challenging to quantify experimentally. They extend over only a few nanometres and depend sensitively on the detuning, dephasing and relative orientation (that is, the vectorial properties) of the coupled dipoles. Here, we introduce plasmonic nanofocusing spectroscopy to record coherent light scattering spectra with 5 nm spatial resolution from the apex of a conical gold nanotaper. The apex is excited solely by evanescent fields and coupled to plasmon resonances in a single gold nanorod. We resolve resonance energy shifts and line broadenings as a function of dipole distance and relative orientation. We demonstrate how these phenomena arise from mode couplings between different vectorial components of the interacting optical near fields, specifically from the coupling of the nanorod to both transverse and longitudinal polarizabilities of the taper apex.

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Fig. 1: Plasmonic nanofocusing scattering spectroscopy of individual gold nanorods.
Fig. 2: High-spatial-resolution plasmonic nanofocusing spectra of a single gold nanorod.
Fig. 3: Distance-dependent plasmonic nanofocusing spectra of an individual gold nanorod.
Fig. 4: Fano line analysis of high-spatial-resolution plasmonic nanofocusing spectra recorded on a single gold nanorod.
Fig. 5: Coupled dipole simulations of plasmonic nanofocusing spectra of a single gold nanorod.

Data availability

The data that support the plots within this paper and other findings of this study are available from the corresponding author upon reasonable request.

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Acknowledgements

The authors acknowledge financial support by the Deutsche Forschungsgemeinschaft (SPP1839 ‘Tailored Disorder’, grant LI 580/12 and SPP1840 ‘QUTIF’ grant LI 580/13), the Korea Foundation for International Cooperation of Science and Technology (Global Research Laboratory project, K20815000003) and the German–Israeli Foundation (GIF grant no. 1256 and 1074-49.10/2009). M.E. thanks the Studienstiftung des Deutschen Volkes (German Scholarship Foundation) for a PhD scholarship and the Deutsche Forschungsgemeinschaft (project 401390650). The authors thank V. Smirnov for performing supporting finite element method calculations and H. Kollmann for providing high-resolution SEM images of individual gold nanorods. The authors thank N. Talebi for discussions and supporting numerical calculations.

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Contributions

J.W. and G.W. prepared the nanorod samples. M.E. and S.F.B. built the SNOM set-up, prepared the nanofocusing SNOM tapers and conducted the SNOM experiments. M.E., S.F.B. and C.L. analysed the data. M.E., C.L. and R.V. performed the theoretical modelling. C.L. initiated the project, M.E. and C.L. co-wrote the manuscript. J.Z., A.C., A.K. and J.H.Z. performed the broadband tip characterization experiments and analysed these data together with M.E. and C.L. All authors discussed the results and commented on the manuscript.

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Correspondence to Christoph Lienau.

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Supplementary Figs. 1–15. Supplementary Table 1

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Esmann, M., Becker, S.F., Witt, J. et al. Vectorial near-field coupling. Nat. Nanotechnol. 14, 698–704 (2019). https://doi.org/10.1038/s41565-019-0441-y

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