Search

Optical nanoantennas are well-known for the confinement of light into nanoscale hot spots, suitable for emission enhancement and sensing applications. Here, we show how control of the antenna dimensions allows tuning the local optical phase, hence turning a hot spot into a cold spot. We manipulate the local intensity exploiting the interference between driving and scattered field. Using single molecules as local detectors, we experimentally show the creation of subwavelength pockets with full suppression of the driving field. Remarkably, together with the cold excitation spots, we observe inhibition of emission by the phase-tuned nanoantenna. The fluorescence lifetime of a molecule scanned in such volumes becomes longer, showing slow down of spontaneous decay. In conclusion, the spatial phase of a nanoantenna is a powerful knob to tune between enhancement and inhibition in a 3-dimensional subwavelength volume.

Covalent organic frameworks (COFs) are molecule-based 2D and 3D materials that possess a wide range of mechanical and electronic properties. We have performed a joint experimental and theoretical study of the electronic structure of boroxine-linked COFs grown under ultrahigh vacuum conditions and characterized using scanning tunneling spectroscopy on Au(111) and hBN/Cu(111) substrates. Our results show that a single hBN layer electronically decouples the COF from the metallic substrate, thus suppressing substrate-induced broadening and revealing new features in the COF electronic local density of states (LDOS). The resulting sharpening of LDOS features allows us to experimentally determine the COF band gap, bandwidths, and the electronic hopping amplitude between adjacent COF bridge sites. These experimental parameters are consistent with the results of first-principles theoretical predictions.

Spontaneous light emission is known to be affected by the local density of states and enhanced when coupled to a resonant cavity. Here, we report on an experimental study of silicon-vacancy (SiV) color center fluorescence and spontaneous Raman scattering from subwavelength diamond particles supporting low-order Mie resonances in the visible range. For the first time to our knowledge, we have measured the size dependences of the SiV fluorescence emission rate and the Raman scattering intensity from individual diamond particles in the range from 200 to 450 nm. The obtained dependences reveal a sequence of peaks, which we explicitly associate with specific multipole resonances. The results are in agreement with our theoretical analysis and highlight the potential of intrinsic optical resonances for developing nanodiamond-based lasers and single-photon sources.

We investigate electronic states of Se-substituted 1T-TaS2 by scanning tunneling microscopy/spectroscopy (STM/STS), where superconductivity emerges from the unique Mott-charge-density-wave (Mott-CDW) state. Spatially resolved STS measurements reveal that a pseudogap replaces the Mott gap with the CDW gaps intact. The pseudogap has little correlation with the unit-cell-to-unit-cell variation in the local Se concentration but appears globally. The correlation length of the local density of states (LDOS) is substantially enhanced at the Fermi energy and decays rapidly at high energies. Furthermore, the statistical analysis of LDOS indicates the weak multifractal behavior of the wave functions. These findings suggest a correlated metallic state induced by disorder and provide a new insight into the emerging superconductivity in two-dimensional materials.

We propose a technique based on nonlocal resistance measurements for mapping transport in electron optics experiments. Utilizing tight-binding transport methods, we show how to use a four-terminal measurement to isolate the ballistic transport from a single lead of interest and reconstruct its contribution to the local density of states. This enables us to propose an experimentally tractable four-terminal device with via contacts for measuring Veselago lensing in a graphene p-n junction. Furthermore, we demonstrate how to extend this method as a scanning probe technique, implementing mapping of complex electron optics experiments including angled junctions, collimation optics, and beam steering. Our results highlight the fundamental importance of electron dephasing in ballistic transport and provide guidelines for isolating electron optics signals of interest. These findings unveil a fresh approach to performing electron optics experiments, with a plethora of two-dimensional material platforms to explore.

High quality electrical contact to semiconducting transition metal dichalcogenides (TMDCs) such as $MoS_2$ is key to unlocking their unique electronic and optoelectronic properties for fundamental research and device applications. Despite extensive experimental and theoretical efforts reliable ohmic contact to doped TMDCs remains elusive and would benefit from a better understanding of the underlying physics of the metal-TMDC interface. Here we present measurements of the atomic-scale energy band diagram of junctions between various metals and heavily doped monolayer $MoS_2$ using ultra-high vacuum scanning tunneling microscopy (UHV-STM). Our measurements reveal that the electronic properties of these junctions are dominated by 2D metal induced gap states (MIGS). These MIGS are characterized by a spatially growing measured gap in the local density of states (L-DOS) of the $MoS_2$ within 2 nm of the metal-semiconductor interface. Their decay lengths extend from a minimum of ~0.55 nm near mid gap to as long as 2 nm near the band edges and are nearly identical for Au, Pd and graphite contacts, indicating that it is a universal property of the monolayer semiconductor. Our findings indicate that even in heavily doped semiconductors, the presence of MIGS sets the ultimate limit for electrical contact.

When coherent charge carriers cross micron-scale cavities, their dynamics can be governed by a few resonant states, also called “quantum scars”, determined by the cavity geometry. Quantum scars can be described using theoretical tools but have also been directly imaged in the case of high-quality semiconductor cavities as well as in disordered graphene devices, thanks to scanning gate microscopy (SGM). Here, we discuss spatially resolved SGM images of low-temperature charge transport through a mesoscopic ring fabricated from high-quality monolayer graphene lying on top of hexagonal boron nitride. SGM images are decorated with a pattern of radial scars in the ring area, which is found to evolve smoothly and reappear when varying the charge-carrier energy. The energies separating recurrent patterns are found to be directly related to geometric dimensions of the ring. Moreover, a recurrence is also observed in simulations of the local density of states of a model graphene quantum ring. The observed recurrences are discussed in the light of recent predictions of relativistic quantum scars in mesoscopic graphene cavities.

High-temperature thermal photonics presents unique challenges for engineers as the database of materials that can withstand extreme environments are limited. In particular, ceramics with high temperature stability that can support coupled light-matter excitations, that is, polaritons, open new avenues for engineering radiative heat transfer. Hexagonal boron nitride (hBN) is an emerging ceramic 2D material that possesses low-loss polaritons in two spectrally distinct mid-infrared frequency bands. The hyperbolic nature of these frequency bands leads to a large local density of states (LDOS). In 2D form, these polaritonic states are dark modes, bound to the material. In cylindrical form, boron nitride nanotubes (BNNTs) create subwavelength particles capable of coupling these dark modes to radiative ones. In this study, we leverage the high-frequency optical phonons present in BNNTs to create strong mid-IR thermal antenna emitters at high temperatures (938 K). Through direct measurement of thermal emission of a disordered system of BNNTs, we confirm their radiative polaritonic modes and show that the antenna behavior can be observed even in a disordered system. These are among the highest-frequency optical phonon polaritons that exist and could be used as high-temperature mid-IR thermal nanoantenna sources.

Chiral light-matter interactions as an emerging aspect of quantum optics enable exceptional physical phenomena and advanced applications in nanophotonics through the nanoscale exploitation of photon-emitter interactions. The chiral radiative properties of quantum emitters strongly depend on the photonic environment, which can be drastically altered by plasmonic nanostructures with a high local density of states (LDOS). Hence, precise knowledge of the chiral photonic environment is essential for manipulating the chirality of light-matter interactions, which requires high resolution chiral characterization techniques. In this work, chiral radiative LDOS distributions of single plasmonic nanostructures that directly govern the chiral radiative spontaneous decay of quantum emitters are imaged at the nanoscale by using cathodoluminescence nanoscopy, enabling precise and highly efficient control of chiral photon emission for chiroptical technologies. Radiative LDOS hot-spots with the chirality larger than 93% are obtained by properly designing chiral plasmonic modes of Au nanoantennas. After fabricating monolayered WSe

Lanthanoid series are unique in atomic elements. One reason is because they have 4f electronic states forbidding electric-dipole (ED) transitions in vacuum and another reason is because they are very useful in current-day optical technologies such as lasers and fiber-based telecommunications. Trivalent Er ions are well-known as a key atomic element supporting 1.5 μm band optical technologies and also as complex photoluminescence (PL) band deeply mixing ED and magnetic-dipole (MD) transitions. Here we show large and selective enhancement of ED and MD radiations up to 83- and 26-fold for a reference bulk state, respectively, in experiments employing plasmonic nanocavity arrays. We achieved the marked PL enhancement by use of an optimal design for electromagnetic (EM) local density of states (LDOS) and by Er-ion doping in deep subwavelength precision. We moreover clarify the quantitative contribution of ED and MD radiations to the PL band, and the magnetic Purcell effect in the PL-decay temporal measurement. This study experimentally demonstrates a new scheme of EM-LDOS engineering in plasmon-enhanced photonics, which will be a key technique to develop loss-compensated and active plasmonic devices.

Many applications in (quantum) nanophotonics rely on controlling light-matter interaction through strong, nanoscale modification of the local density of states (LDOS). All-optical techniques probing emission dynamics in active media are commonly used to measure the LDOS and benchmark experimental performance against theoretical predictions. However, metal coatings needed to obtain strong LDOS modifications in, for instance, nanocavities, are incompatible with all-optical characterization. So far, no reliable method exists to validate theoretical predictions. Here, we use sub-nanosecond pulses of focused electrons to penetrate the metal and excite a buried active medium at precisely-defined locations inside sub-wavelength resonant nanocavities. We reveal the spatial layout of the spontaneous-emission decay dynamics inside the cavities with deep-subwavelength detail, directly mapping the LDOS. We show that emission enhancement converts to inhibition despite an increased number of modes, emphasizing the critical role of optimal emitter location. Our approach yields fundamental insight in dynamics at deep-subwavelength scales for a wide range of nano-optical systems.

One of the intriguing characteristics of honeycomb lattices is the appearance of a pseudo-magnetic field as a result of mechanical deformation. In the case of graphene, the Landau quantization resulting from this pseudo-magnetic field has been measured using scanning tunneling microscopy. Here we show that a signature of the pseudo-magnetic field is a local sublattice symmetry breaking observable as a redistribution of the local density of states. This can be interpreted as a polarization of graphene's pseudospin due to a strain induced pseudo-magnetic field, in analogy to the alignment of a real spin in a magnetic field. We reveal this sublattice symmetry breaking by tunably straining graphene using the tip of a scanning tunneling microscope. The tip locally lifts the graphene membrane from a SiO$_2$ support, as visible by an increased slope of the $I(z)$ curves. The amount of lifting is consistent with molecular dynamics calculations, which reveal a deformed graphene area under the tip in the shape of a Gaussian. The pseudo-magnetic field induced by the deformation becomes visible as a sublattice symmetry breaking which scales with the lifting height of the strained deformation and therefore with the pseudo-magnetic field strength. Its magnitude is quantitatively reproduced by analytic and tight-binding models, revealing fields of 1000 T. These results might be the starting point for an effective THz valley filter, as a basic element of valleytronics., Comment: Revised manuscript: streamlined the abstract and introduction, added methods to supplement, Nano Letters, 2017

Two-dimensional black phosphorus (BP) has sparked enormous research interest due to its high carrier mobility, layer-dependent direct bandgap and outstanding in-plane anisotropic properties. BP is one of the few two-dimensional materials where it is possible to tune the bandgap over a wide energy range from the visible up to the infrared. In this article, we report the observation of a giant Stark effect in electrostatically gated few-layer BP. Using low-temperature scanning tunnelling microscopy, we observed that in few-layer BP, when electrons are injected, a monotonic reduction of the bandgap occurs. The injected electrons compensate the existing defect-induced holes and achieve up to 35.5% bandgap modulation in the light-doping regime. When probed by tunnelling spectroscopy, the local density of states in few-layer BP shows characteristic resonance features arising from layer-dependent sub-band structures due to quantum confinement effects. The demonstration of an electrical gate-controlled giant Stark effect in BP paves the way to designing electro-optic modulators and photodetector devices that can be operated in a wide electromagnetic spectral range.

Solid-state quantum emitters, such as artificially engineered quantum dots or naturally occurring defects in solids, are being investigated for applications ranging from quantum information science and optoelectronics to biomedical imaging. Recently, these same systems have also been studied from the perspective of nanoscale metrology. In this letter, we study the near-field optical properties of a diamond nanocrystal hosting a single nitrogen vacancy center. We find that the nitrogen vacancy center is a sensitive probe of the surrounding electromagnetic mode structure. We exploit this sensitivity to demonstrate nanoscale fluorescence lifetime imaging microscopy (FLIM) with a single nitrogen vacancy center by imaging the local density of states of an optical antenna.

Scanning tunneling microscopy and local conductance mapping show spin-state coexistence in bilayer films of Fe[(H(2)Bpz(2))(2)bpy] on Au(111) that is independent of temperature between 131 and 300 K. This modification of bulk behavior is attributed in part to the unique packing constraints of the bilayer film that promote deviations from bulk behavior. The local density of states measured for different spin states shows that high-spin molecules have a smaller transport gap than low-spin molecules and are in agreement with density functional theory calculations.

We have fabricated single C(60) molecule transistors with ferromagnetic Ni leads (FM-SMTs) by using an electrical break junction method and investigated their magnetotransport. The FM-SMTs exhibited clear gate-dependent hysteretic tunnel magnetoresistance (TMR) and the TMR values reached as high as -80%. The polarity of the TMR was found to be always negative over the entire bias range studied here. Density functional theory calculations show that hybridization between the Ni substrate states and the C(60) molecular orbitals generates an antiferromagnetic configuration in the local density of states near the Fermi level, which gives a reasonable explanation for the observed negative TMR.

Single-emitter microscopy has emerged as a promising method of imaging nanostructures with nanoscale resolution. This technique uses the centroid position of an emitter's far-field radiation pattern to infer its position to a precision that is far below the diffraction limit. However, nanostructures composed of high-dielectric materials such as noble metals can distort the far-field radiation pattern. Previous work has shown that these distortions can significantly degrade the imaging of the local density of states in metallic nanowires using polarization-resolved imaging. But unlike nanowires, nanoparticles do not have a well-defined axis of symmetry, which makes polarization-resolved imaging difficult to apply. Nanoparticles also exhibit a more complex range of distortions, because in addition to introducing a high dielectric surface, they also act as efficient scatterers. Thus, the distortion effects of nanoparticles in single-emitter microscopy remains poorly understood. Here we demonstrate that metallic nanoparticles can significantly distort the accuracy of single-emitter imaging at distances exceeding 300 nm. We use a single quantum dot to probe both the magnitude and the direction of the metallic nanoparticle-induced imaging distortion and show that the diffraction spot of the quantum dot can shift by more than 35 nm. The centroid position of the emitter generally shifts away from the nanoparticle position, which is in contradiction to the conventional wisdom that the nanoparticle is a scattering object that will pull in the diffraction spot of the emitter toward its center. These results suggest that dielectric distortion of the emission pattern dominates over scattering. We also show that by monitoring the distortion of the quantum dot diffraction spot we can obtain high-resolution spatial images of the nanoparticle, providing a new method for performing highly precise, subdiffraction spatial imaging. These results provide a better understanding of the complex near-field coupling between emitters and nanostructures and open up new opportunities to perform super-resolution microscopy with higher accuracy.

We calculate the electronic local density of states (LDOS) of DNA nucleotide bases (A,C,G,T), deposited on graphene. We observe significant base-dependent features in the LDOS in an energy range within a few electronvolts of the Fermi level. These features can serve as electronic fingerprints for the identification of individual bases in scanning tunneling spectroscopy (STS) experiments that perform image and site dependent spectroscopy on biomolecules. Thus the fingerprints of DNA-graphene hybrid structures may provide an alternative route to DNA sequencing using STS.

We present an approach to predicting extrinsic electron resonance widths within quantum corral nanostructures based on analogies with acoustics. Established quantum mechanical methods for calculating resonance widths, such as multiple scattering theory, build up the scattering atom by atom, ignoring the structure formed by the atoms, such as walls or enclosures. Conversely, particle-in-a-box models, assuming continuous walls, have long been successful in predicting quantum corral energy levels, but not resonance widths. In acoustics, partial reflection from walls and various enclosures has long been incorporated for determining reverberation times. Pursuing an exact analogy between the local density of states of a quantum corral and the acoustic impedance of a concert hall, we show electron lifetimes in nanoscopic structures of arbitrary convex shape are well accounted for by the Sabine formula for acoustic reverberation times. This provides a particularly compact and intuitive prescription for extrinsic finite lifetimes in a particle-in-a-box with leaky walls, including quantum corral atomic walls, given single particle scattering properties.

Lack of inversion symmetry at a metallic surface can lead to an observable spin-orbit interaction. For certain metal surfaces, such as the Au(111) surface, the experimentally observed spin-orbit coupling results in spin rotation lengths on the order of tens of nanometers, which is the typical length scale associated with quantum corral structures formed on metal surfaces. In this work, multiple scattering theory is used to calculate the local density of states (LDOS) of quantum corral structures comprised of nonmagnetic adatoms in the presence of spin-orbit coupling. Contrary to previous theoretical predictions, spin-orbit coupling induced modulations are observed in the theoretical LDOS, which should be observable using scanning tunneling microscopy.

The Kondo effect, a widely studied phenomenon in which the scattering of conduction electrons by magnetic impurities increases as the temperature T is lowered, depends strongly on the density of states at the Fermi energy. It has been predicted by theory that magnetic impurities on free-standing monolayer graphene exhibit the Kondo effect and that control of the density of states at the Fermi level by external means can be used to switch the effect on and off. However, though transport data for Co adatoms on graphene monolayers on several substrates have been reported, there exists no evidence for a Kondo effect. Here we probe the role of the substrate on the Kondo effect of Co on graphene by combining low-temperature scanning tunneling microscopy and spectroscopy measurements with density functional theory calculations. We use a Ru(0001) substrate that is known to cause graphene to ripple, yielding a moire superlattice. The experimental data show a sharp Kondo resonance peak near the Fermi energy from only Co adatoms at the edge of atop regions of the moire pattern. The theoretical results show that the variation of the distance from the graphene to the Ru substrate, which controls the spin polarization and local density of states at the Fermi energy, is the key factor for the appearance of the Kondo resonance. The results suggest that rippling of graphene by suitable substrates is an additional lever for tuning and selectively switching the appearance of the Kondo effect.

The coupling of optical emitters with a nanostructured environment is at the heart of nano- and quantum optics. We control this coupling by the lithographic positioning of a few (1–3) quantum dots (QDs) along plasmonic silver nanowires with nanoscale resolution. The fluorescence emission from the QD-nanowire systems is probed spectroscopically, by microscopic imaging and decay time measurements. We find that the plasmonic modes can strongly modulate the fluorescence emission. For a given QD position, the local plasmon field dictates the coupling efficiency, and thus the relative weight of free space radiation and emission into plasmon modes. Simulations performed with a generic few-level model give very good agreement with experiment. Our data imply that the 2D degenerate emission dipole orientation of the QD can be forced to predominantly emit to one polarization component dictated by the nanowire modes.

Quantum dots (QDs) allow for manipulation of the position and energy levels of electrons at sub-10 nm length scales through control of material chemistry, size, and shape. It is known from optical studies that the bandgap of semiconductor QDs increases as their size decreases due to the narrowing of the quantum confinement potential. The mechanism of quantum confinement also indicates that the localized properties within individual QDs should depend on their shape in addition to their size, but direct observations of this effect have proven challenging due to the limited spatial resolution of measurement techniques at this scale and the ability to remove contributions from the surroundings. Here we present experimental evidence of spatial variations in the lowest available electron transition energy within a series of single electrically isolated QDs due to a dome-shaped geometry, measured using electron energy-loss spectroscopy in a (scanning) transmission electron microscope [(S)TEM-EELS]. We observe a consistent increase in the energy onset of electronic excitations from the lateral center of the dot toward the edges, which we attribute purely to shape. This trend is in qualitative agreement with a simple quantum simulation of the local density of states in a dome-shaped QD.

We perform spectrally resolved cathodoluminescence (CL) imaging nanoscopy using a 30 keV electron beam to identify the resonant modes of an ultrathin (20 nm), laterally tapered plasmonic Ag nanostrip antenna. We resolve with deep-subwavelength resolution four antenna resonances (resonance orders m = 2-5) that are ascribed to surface plasmon polariton standing waves that are confined on the strip. We map the local density of states on the strip surface and show that it has contributions from symmetric and antisymmetric surface plasmon polariton modes, each with a very different mode index. This work illustrates the power of CL experiments that can visualize hidden modes that for symmetry reasons have been elusive in optical light scattering experiments.

We have demonstrated the reversible and local modification of the electronic properties of graphene by hydrogen passivation and subsequent electron-stimulated hydrogen desorption with an scanning tunneling microscope tip. In addition to changing the morphology, we show that the hydrogen passivation is stable at room temperature and modifies the electronic properties of graphene, opening a gap in the local density of states. This insulating state is reversed by local desorption of the hydrogen, and the unaltered electronic properties of graphene are recovered. Using this mechanism, we have "written" graphene patterns on nanometer length scales. For patterned regions that are roughly 20 nm or greater, the inherent electronic properties of graphene are completely recovered. Below 20 nm we observe dramatic variations in the electronic properties of the graphene as a function of pattern size. This reversible and local mechanism for modifying the electronic properties of graphene has far-reaching implications for nanoscale circuitry fabricated from this revolutionary material.

cited By 21; International audience; Evidence for modified electronic structure in double-walled carbon nanotubes with respect to their individual inner and outer constituent single-walled nanotubes is provided by scanning tunneling microscopy and spectroscopy experiments. The contribution originating from the inner tube to the local density of states of the double-walled system was identified in agreement with previous theoretical calculations. Consequently, the chiral index for the inner tube was extracted based on the additional van Hove singularities present in the experimental tunneling spectra. © 2007 American Chemical Society.

Field emission properties of B-doped carbon nanotubes are investigated from both theoretical and experimental standpoints. Using tight-binding and ab initio calculations, it is observed that B-saturating tip edges of carbon nanotubes induce the presence of large peaks within the local density of states (LDOS) located in an energy region close to the Fermi level (Ef). These localized states suggest a field emission enhancement for the B-doped tubes. In addition, ab initio theoretical results indicate that the work function for B-doped tubes is 1.7 eV lower when compared to pure carbon-terminated nanotubes. Experimentally, it is found that B-doped tubes, which are produced by arc discharge techniques and contain B mainly at the tips, exhibit stable electron field emission at lower turn-on voltages (1.4 V/mum) when compared to pure single- and multiwalled carbon nanotubes (2.8 and 3.0 V/mum, respectively) measured under the same conditions. We strongly believe our results will bring new insights in the fabrication of stable field emission sources.

Plasmonic nanostructures dramatically alter the radiative and nonradiative properties of single molecules in their vicinity. This coupling-induced change in decay channels selectively enhances specific vibronic transitions, which can enable plasmonic control of molecular reactivity. Here, we report coupling-dependent spectral emission shaping of single Rhodamine 800 molecules in the vicinity of plasmonic gold nanorods. We show that the relative vibronic transition rates of the first two vibronic transitions of the spontaneous emission spectrum can be tuned in the weak coupling regime, by approximately 25-fold, on the single molecule level.

The coupling of optical emitters with a nanostructured environment is at the heart of nano- and quantum optics. We control this coupling by the lithographic positioning of a few (1–3) quantum dots (QDs) along plasmonic silver nanowires with nanoscale resolution. The fluorescence emission from the QD-nanowire systems is probed spectroscopically, by microscopic imaging and decay time measurements. We find that the plasmonic modes can strongly modulate the fluorescence emission. For a given QD position, the local plasmon field dictates the coupling efficiency, and thus the relative weight of free space radiation and emission into plasmon modes. Simulations performed with a generic few-level model give very good agreement with experiment. Our data imply that the 2D degenerate emission dipole orientation of the QD can be forced to predominantly emit to one polarization component dictated by the nanowire modes.

Monolayer hexagonal boron nitride (hBN) tunnel barriers investigated using conductive atomic force microscopy reveal moire patterns in the spatial maps of their tunnel conductance consistent with the formation of a moire superlattice between the hBN and an underlying highly ordered pyrolytic graphite (HOPG) substrate. This variation is attributed to a periodc modulation of the local density of states and occurs for both exfoliated hBN barriers and epitaxially grown layers. The epitaxial barriers also exhibit enhanced conductance at localized subnanometer regions which are attributed to exposure of the substrate to a nitrogen plasma source during the high temperature growth process. Our results show clearly a spatial periodicity of tunnel current due to the formation of a moire superlattice and we argue that this can provide a mechanism for elastic scattering of charge carriers for similar interfaces embedded in graphene/hBN resonant tunnel diodes.

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 characte...