Correlated 3D Nanoscale Mapping and Simulation of Coupled Plasmonic Nanoparticles

[Image: see text] Electron tomography in combination with electron energy-loss spectroscopy (EELS) experiments and simulations was used to unravel the interplay between structure and plasmonic properties of a silver nanocuboid dimer. The precise 3D geometry of the particles fabricated by means of electron beam lithography was reconstructed through electron tomography, and the full three-dimensional information was used as an input for simulations of energy-loss spectra and plasmon resonance maps. Excellent agreement between experiment and theory was found throughout, bringing the comparison between EELS imaging and simulations to a quantitative and correlative level. In addition, interface mode patterns, normally masked by the projection nature of a transmission microscopy investigation, could be unambiguously identified through tomographic reconstruction. This work overcomes the need for geometrical assumptions or symmetry restrictions of the sample in simulations and paves the way for detailed investigations of realistic and complex plasmonic nanostructures.