While plasmonic antennas composed of building blocks made of the same material have been thoroughly studied, recent investigations have highlighted the unique opportunities enabled by making compositionally asymmetric plasmonic systems. So far, mainly heterostructures composed of nanospheres and nanodiscs have been investigated, revealing opportunities for the design of Fano resonant nanostructures, directional scattering, sensing and catalytic applications. In this article, an improved fabrication method is reported that enables precise tuning of the heterodimer geometry, with interparticle distances made down to a few nanometers between Au−Ag and Au−Al nanoparticles. A wide range of mode energy detuning and coupling conditions are observed by near field hyperspectral imaging performed with electron energy loss spectroscopy, supported by full wave analysis numerical simulations. These results provide direct insights into the mode hybridization of plasmonic heterodimers, pointing out the influence of each dimer constituent in the overall electromagnetic response. By relating the coupling of nondipolar modes and plasmon−interband interaction with the dimer geometry, this work facilitates the development of plasmonic heterostructures with tailored responses, beyond the possibilities offered by homodimers. KEYWORDS: optical nanoantennas, plasmonic heterostructures, bimetallic antennas, electron energy loss spectroscopy, electron beam lithography, eigenmodes C ollective oscillations of the conduction electrons in metal nanostructures, known as localized surface plasmon resonances, 1 have been intensively studied and designed by manipulating both the nanostructures size and geometry, as well as their dielectric environment.2 These investigations, carried out over the entire visible light spectrum, including the near-UV and near-IR, have demonstrated the control of both nanoscale optical fields and far field radiation, 1 leading to the concept of optical nanoantennas.2,3 The electromagnetic properties of these structures are governed by their eigenmodes, ranging from dipoles to high order multipoles. 4,5 When the nanoparticles are arranged in pairs or multimers, these modes couple to each other and hybridize, producing further optical properties. 6−8 In the simplest and most common geometry, involving the coupling of two selfsimilar spherical nanoparticles separated by a nanogap, a wellknown dipole−dipole interaction along the dimer axis is produced. 6 This coupling generates an intense and confined near field in the gap region, which can enable large nanoscale fluorescence enhancement 9 and surface enhanced Raman scattering down to the single molecule level. 10,11 Thanks to a complete description of the plasmonic coupling for spherical self-similar nanoparticle dimers, Nordlander and coauthors 7 have shown that the gap dependent hybridization in such nanostructures stems from the interaction of the uncoupled eigenmodes. Specifically, the uncoupled modes hybridize with bonding and antibonding interactions a...