3D Imaging of Gap Plasmons in Vertically Coupled Nanoparticles by EELS Tomography.

Plasmonic gap modes provide the ultimate confinement of optical fields. Demanding high spatial resolution, the direct imaging of these modes was only recently achieved by electron energy loss spectroscopy (EELS) in a scanning transmission electron microscope (STEM). However, conventional 2D STEM-EELS is only sensitive to components of the photonic local density of states (LDOS) parallel to the electron trajectory. It is thus insensitive to specific gap modes, a restriction that was lifted with the introduction of tomographic 3D EELS imaging. Here, we show that by 3D EELS tomography the gap mode LDOS of a vertically stacked nanotriangle dimer can be fully imaged. Besides probing the complete mode spectrum, we demonstrate that the tomographic approach allows disentangling the signal contributions from the two nanotriangles that superimpose in a single measurement with a fixed electron trajectory. Generally, vertically coupled nanoparticles enable the tailoring of 3D plasmonic fields, and their full characterization will thus aid the development of complex nanophotonic devices.

Tomographic imaging of the photonic environment of plasmonic nanoparticles.

The photonic local density of states (LDOS) governs the enhancement of light-matter interaction at the nanoscale, but despite its importance for nanophotonics and plasmonics experimental local density of states imaging remains extremely challenging. Here we introduce a tomography scheme based on electron microscopy that allows retrieval of the three-dimensional local density of states of plasmonic nanoparticles with nanometre spatial and sub-eV energy resolution. From conventional electron tomography experiments we obtain the three-dimensional morphology of the nanostructure, and use this information to compute an expansion basis for the photonic environment. The expansion coefficients are obtained through solution of an inverse problem using as input electron-energy loss spectroscopy images. We demonstrate the applicability of our scheme for silver nanocuboids and coupled nanodisks, and resolve local density of states enhancements with extreme sub-wavelength dimensions in hot spots located at roughness features or in gaps of coupled nanoparticles.Imaging the photonic local density of states of plasmonic nanoparticles remains extremely challenging. Here, the authors introduce a tomography scheme based on electron microscopy that allows retrieval of the three-dimensional local density of states with nanometre spatial and sub-eV energy resolution.

Full Three-Dimensonal Reconstruction of the Dyadic Green Tensor from Electron Energy Loss Spectroscopy of Plasmonic Nanoparticles.

Electron energy loss spectroscopy (EELS) has emerged as a powerful tool for the investigation of plasmonic nanoparticles, but the interpretation of EELS results in terms of optical quantities, such as the photonic local density of states, remains challenging. Recent work has demonstrated that, under restrictive assumptions, including the applicability of the quasistatic approximation and a plasmonic response governed by a single mode, one can rephrase EELS as a tomography scheme for the reconstruction of plasmonic eigenmodes. In this paper we lift these restrictions by formulating EELS as an inverse problem and show that the complete dyadic Green tensor can be reconstructed for plasmonic particles of arbitrary shape. The key steps underlying our approach are a generic singular value decomposition of the dyadic Green tensor and a compressed sensing optimization for the determination of the expansion coefficients. We demonstrate the applicability of our scheme for prototypical nanorod, bowtie, and cube geometries.

Correlated 3D Nanoscale Mapping and Simulation of Coupled Plasmonic Nanoparticles.

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.

Tomography of particle plasmon fields from electron energy loss spectroscopy.

We theoretically investigate electron energy loss spectroscopy (EELS) of metallic nanoparticles in the optical frequency domain. Using a quasistatic approximation scheme together with a plasmon eigenmode expansion, we show that EELS can be rephrased in terms of a tomography problem. For selected single and coupled nanoparticles we extract the three-dimensional plasmon fields from a collection of rotated EELS maps. Our results pave the way for a fully three-dimensional plasmon-field tomography and establish EELS as a quantitative measurement device for plasmonics.

Ultrafast strong-field photoemission from plasmonic nanoparticles.

We demonstrate the ultrafast generation of electrons from tailored metallic nanoparticles and unravel the role of plasmonic field enhancement in this process by comparing resonant and off-resonant particles, as well as different particle geometries. We find that electrons become strongly accelerated within the evanescent fields of the plasmonic nanoparticles and escape along straight trajectories with orientations governed by the particle geometry. These results establish plasmonic nanoparticles as versatile ultrafast, nanoscopic sources of electrons.