Abstract
Tomography has enabled the characterization of the Earth's interior, visualization of the inner workings of the human brain, and three-dimensional reconstruction of matter at the atomic scale. However, tomographic techniques that rely on optical excitation or detection are generally limited in their resolution by diffraction. Here, we introduce a tomographic technique—cathodoluminescence spectroscopic tomography—to probe optical properties in three dimensions with nanometre-scale spatial and spectral resolution. We first obtain two-dimensional cathodoluminescence maps of a three-dimensional nanostructure at various orientations. We then use the method of filtered back-projection to reconstruct the cathodoluminescence intensity at each wavelength. The resulting tomograms allow us to locate regions of efficient cathodoluminescence in three dimensions across visible and near-infrared wavelengths, with contributions from material luminescence and radiative decay of electromagnetic eigenmodes. The experimental signal can be further correlated with the radiative local density of optical states in particular regions of the reconstruction. We demonstrate how cathodoluminescence tomography can be used to achieve nanoscale three-dimensional visualization of light–matter interactions by reconstructing a three-dimensional metal–dielectric nanoresonator.
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Acknowledgements
The authors thank S. Sheikholeslami and A. Saleh for assistance with photoluminescence measurements, and J. Briggs and T. Narayan for scientific discussions. The authors also thank T. Carver for electron beam evaporation. A.C.A. acknowledges support from the Robert L. and Audrey S. Hancock Stanford Graduate Fellowship. J.A.D. acknowledges support from an Air Force Office of Scientific Research PECASE grant (FA9550-15-1-0006) and a National Science Foundation CAREER Award (DMR-1151231). Funding from a Department of Energy EERE Sunshot grant (no. DE-EE0005331) is also acknowledged. This work is part of the research programme of the Stichting voor Fundamenteel Onderzoek der Materie (FOM), which is supported financially by the Nederlandse Organisatie voor Wetenschappelijk Onderzoek (NWO). This work was funded by the European Research Council and is also part of NanoNextNL, a nanotechnology programme funded by the Dutch Ministry of Economic Affairs.
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A.C.A. fabricated samples and performed transmission electron microscopy, photoluminescence spectroscopy, tomographic reconstruction and electromagnetic simulations. A.C.A., B.J.M.B. and T.C. performed the cathodoluminescence microscopy, spectroscopy and scanning electron microscopy. A.G-E. performed boundary element method simulations. J.A.D. and A.P. guided and supervised the experiments and analysis. All authors analysed and interpreted the results and edited the manuscript.
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A.P. is co-founder and co-owner of Delmic BV, a startup company that is developing a commercial product based on the cathodoluminescence system used in this work.
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Atre, A., Brenny, B., Coenen, T. et al. Nanoscale optical tomography with cathodoluminescence spectroscopy. Nature Nanotech 10, 429–436 (2015). https://doi.org/10.1038/nnano.2015.39
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DOI: https://doi.org/10.1038/nnano.2015.39
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