Vanadium dioxide nanostructures represent a promising phase-changing platform for use in tunable plasmonic devices. However, localized surface plasmon resonances have been investigated in detail only in nanostructure arrays using optical techniques, which did not provide comprehensive information about individual plasmonic modes and their tunability. In this study, we present a comprehensive modal analysis of single-phase and multiphase vanadium dioxide nanoparticles. In situ high-resolution electron energy loss spectroscopy was utilized to resolve the dipole plasmon peak, higher-order and breathing plasmonic modes, and bulk losses as a function of nanoparticle size. Furthermore, the focus is directed toward capturing the dynamic nanoscale optical response throughout the metal-insulator transition. This system possesses the ability to be gradually switched on and off in terms of the emergence of near-infrared plasmonic absorption. The switching is accompanied by a gradual spectral shift of the absorption peak, which is essential for functional nanodevices based on vanadium dioxide.

We theoretically investigate the formation of electric and magnetic hot spots with reconfigurable plasmonic antennas. We consider three material systems offering different levels of reconfigurability: gold with the static response, vanadium dioxide which allows for ON/OFF switching, and composite gold-vanadium dioxide material platform which offers a possibility to switch between the electric and magnetic hot spot within a single antenna. Using bowtie and diabolo antennas as a case study, we evaluate optical response functions (scattering and absorption cross-sections, electric and magnetic field enhancement). We demonstrate that the composite material system brings, in addition to enhanced reconfigurability, also novel features of plasmonic antennas, such as strong optical absorption and a joint electric-magnetic hotspot.

Plasmonic antennas exploit localized surface plasmons to shape, confine, and enhance electromagnetic fields with subwavelength resolution. The field enhancement is contributed to by various effects, such as the inherent surface localization of plasmons or the plasmonic lightning-rod effect. Inspired by nanofocusing observed for propagating plasmons, we test the hypothesis that plasmonic antennas with a large cross-section represent a large charge reservoir, enabling large induced charge and field enhancement. Our study reveals that a large charge reservoir is accompanied by large radiative losses, which are the dominant factor, resulting in a low field enhancement.

We present ab initio theory for electron reflection spectroscopy of few-layer graphene for arbitrary angles of incidence. The inelastic effects are included in a consistent way using the optical potential retrieved from ab initio simulations of electron energy-loss spectra. We demonstrate a significant impact of inelastic effects even for single-layer graphene. Next, we address the ability of the electron reflection spectroscopy to determine specific parameters of graphene including not only the number of layers in the few-layer graphene but also the stacking type in the graphene multilayers, and to resolve moir & eacute; patterns in twisted graphene bilayers. We show that the predicted contrast, although significantly reduced by inelastic effects, is sufficient for the experimental detection of all considered parameters. Our findings are corroborated by a fair correspondence of our theoretical predictions with experimental data, both our own and recently published by other authors.

The plasmonic lightning-rod effect refers to the formation of a strong electric near field of localized surface plasmons at the sharp features of plasmonic antennas. While this effect is intuitively utilized in the design and optimization of plasmonic antennas, the relation between the magnitude of the electric field and the local curvature of the plasmonic antenna has not been yet rigorously established. Here, we provide such a study. We design sets of plasmonic antennas that allow to isolate the role of the local curvature from other effects influencing the field. The near electric field is inspected by electron energy loss spectroscopy and electrodynamic simulations. We demonstrate the existence of the plasmonic lightning-rod effect and establish its quantitative description, showing that its strength is comparable to the electrostatic lightning-rod effect. We also provide a simple phenomenological formula for the spatial dependence of the field. Finally, we introduce the effective radius of curvature related to the spatial distribution of induced charge in plasmonic antennas, significantly smaller than their geometrical radius.

Localized surface plasmon (LSP) resonances in plasmonic micro-/nanostructures such as metallic spheres and cylinders, exhibit sensitivity to nearby external changes, such as variations in the refractive index of a dielectric close to the structures. This useful characteristic can be exploited in multiple fields, including medicine, and chemistry. Here, we make use of Babinet’s principle of complementarity (a concept developed for low frequencies) to design plasmonic structures at optical frequencies. The structures consist of complementary metal-dielectric cylindrical dimers and apertures on a metal film. Their performance is evaluated both experimentally and numerically demonstrating their ability to be used for sensing applications.

We present annular dark field scanning transmission electron microscopy (ADF-STEM) as an efficient, fast, and non-destructive nanoscale tool for monitoring solid-state phase transition. Using metal-insulator transition in vanadium dioxide nanoparticles as an example, we characterize lattice and electronic signatures of the phase transition using analytical transmission electron microscopy including diffraction and electron energy-loss spectroscopy. We demonstrate that ADF-STEM shows a clear contrast across the transition, interpreted with the help of convergent electron beam diffraction as stemming from the crystal-lattice modification accompanying the transition. In addition, ADF-STEM utilizes 3–6 orders of magnitude lower electron dose when compared to electron microscopy techniques able to reveal the phase transition with the same spatial resolution and universality. The benefits of ADF-STEM are emphasized by recording a full hysteresis loop for the metal-insulator transition of a single vanadium dioxide nanoparticle. Our study opens the prospect for fast, non-destructive, large-area and nanoscale characterization of solid-state phase transitions.

Vanadium dioxide (VO2) is a strongly correlated material that exhibits the insulator-to-metal transition (IMT) near room temperature, which makes it a promising candidate for applications in nanophotonics or optoelectronics. However, creating VO2 nanostructures with the desired functionality can be challenging due to microscopic inhomogeneities that can significantly impact the local optical and electronic properties. Thin lamellas, produced by focused ion beam milling from a homogeneous layer, provide a useful prototype for studying VO2 at the truly microscopic level using a scanning transmission electron microscope (STEM). High-resolution imaging is used to identify structural inhomogeneities while electron energy-loss spectroscopy (EELS) supported by statistical analysis helps to detect V x O y stoichiometries with a reduced oxidation number of vanadium at the areas of thickness below 70 nm. On the other hand, the thicker areas are dominated by vanadium dioxide, where the signatures of the IMT are detected in both core-loss and low-loss EELS experiments with in situ heating. The experimental results are interpreted with ab initio and semi-classical calculations. This work shows that structural inhomogeneities such as pores and cracks present no harm to the desired optical properties of VO2 samples.

A detailed analysis of the optical response of a system accommodating several coupled modes is needed for the complete understanding of the strong coupling effect. In this paper, we report on the analysis of scattering cross section spectra of Au antennas on a SiO$_{2}$ layer on a Si substrate in the IR region. A classical model of coupled oscillators is used for determining the resonant energies, damping rates and coupling strengths of four phonon polariton modes in the SiO$_{2}$ layer coupled to a localized surface plasmon mode in a Au antenna. The calculated Hopfield mixing coefficients then show the contribution of the individual uncoupled modes to the hybrid modes of the coupled system.

We report on the optical properties of a CsPbBr3 polycrystalline thin film on a single grain level. A sample composed of isolated nanocrystals (NCs) mimicking the properties of the polycrystalline thin film grains that can be individually probed by photoluminescence spectroscopy was prepared. These NCs were analyzed using correlative microscopy allowing the examination of structural, chemical, and optical properties from identical sites. Our results show that the stoichiometry of the CsPbBr3 NCs is uniform and independent of the NCs' morphology. The photoluminescence (PL) peak emission wavelength is slightly dependent on the dimensions of NCs, with a blue shift up to 9 nm for the smallest analyzed NCs. The magnitude of the blueshift is smaller than the emission line width, thus detectable only by high-resolution PL mapping. By comparing the emission energies obtained from the experiment and a rigorous effective mass model, we can fully attribute the observed variations to the size-dependent quantum confinement effect.

The engineering of localized surface plasmon (LSP) resonances in plasmonic structures has led to advances in fields such as chemistry, medicine, and sensing. For the latter case, LSP resonances in metallic micro-/nano structures are particularly important due to these resonances being sensitive to external changes in their near-field, such as the presence of nearby dielectrics. In this communication, complementary metal-dielectric plasmonic structures designed by exploiting Babinet’s principle are studied and designed to act as plasmonic sensors of thin film dielectrics. We make use of metallic plasmonic dimers and their complementary structures (holes on a thin metallic screen) and provide an in-depth study of their performance in terms of their field distribution and sensitivity.

Localised surface plasmons excited on nano-/microstructures acting as plasmonic nanoantennas [1]–[3] have attracted increased attention in recent years with their ability to strongly confine incident electromagnetic (EM) fields in the visible and near-infrared regime. LSP resonances excited on plasmonic structures have been shown to strongly enhance incident fields with subwavelength spatial resolutions close to their surface (the near field) [4]–[10]. Sensors have also benefited from research and innovation in plasmonics. This is due to the spectral position of LSP resonances being sensitive in plasmonic nanostructures to external changes such as variations in the thickness and refractive index of a nearby dielectric.

Gallium is a plasmonic material offering ultraviolet to near-infrared tunability, facile and scalable preparation, and good stability of nanoparticles. In this work, we experimentally demonstrate the link between the shape and size of individual gallium nanoparticles and their optical properties. To this end, we utilize scanning transmission electron microscopy combined with electron energy loss spectroscopy. Lens-shaped gallium nanoparticles with a diameter between 10 and 200 nm were grown directly on a silicon nitride membrane using an effusion cell developed in house that was operated under ultra-high-vacuum conditions. We have experimentally proven that they support localized surface plasmon resonances and their dipole mode can be tuned through their size from the ultraviolet to near-infrared spectral region. The measurements are supported by numerical simulations using realistic particle shapes and sizes. Our results pave the way for future applications of gallium nanoparticles such as hyperspectral absorption of sunlight in energy harvesting or plasmon-enhanced luminescence of ultraviolet emitters.

Plasmonic structures that exhibit localized surface plasmon (LSP) resonances have been exploited in multiple applications including sensing, medicine, and chemistry. LSPs resonances appearing in, for instance, periodic/aperiodic rods or spheres have been recently used for sensing due to the fact that such resonances are sensitive to local external variations such as changes in the refractive index of a dielectric placed on top of them. In this communication, we make use of complementary plasmonic structures (exploiting the Babinet’s principle) consisting of metal-dielectric cylindrical components to study their performance as dielectric film sensors. An in-depth comparison of the complementary structures with the original plasmonic configurations is carried out demonstrating the advantages/disadvantages of each design.

Developing methods to sense local variations in nearby materials, such as their refractive index and thickness, is important in different fields including chemistry and biomedical applications, among others. Localized surface plasmons (LSPs) excited in plasmonic nanostructures have demonstrated to be useful in this context due to the spectral location of their associated resonances being sensitive to changes near the plasmonic structures. In this manuscript, Babinet's principle is explored by exploiting LSP resonances excited in complementary metal-dielectric cylindrical plasmonic structures (plasmonic particle-dimers and aperture-dimers in our case). Both plasmonic structures are evaluated numerically and experimentally using Electron Energy Loss Spectroscopy (EELS), providing a full physical understanding of the complementary nature of the excited LSP resonances. The studied plasmonic structures are then exploited for dielectric sensing under two configurations: when a thin dielectric film is positioned atop the plasmonic structures and when the analyte surrounds/fills the plasmonic particles/apertures. The complementary sensing performance of both proposed structures is also evaluated, showing the approximate validity of the Babinet principle with sensitivities values of up to 700 nm/RIU for thin dielectric sensing.

Electron energy loss spectroscopy (EELS) is often utilized to characterize localized surface plasmon modes supported by plasmonic antennas. However, the spectral resolution of this technique is only mediocre, and it can be rather difficult to resolve modes close in the energy, such as coupled modes of dimer antennas. Here, we address this issue for a case study of the dimer plasmonic antenna composed of two gold discs. We analyze four nearly degenerate coupled plasmon modes of the dimer: longitudinal and transverse bonding and antibonding dipole modes. With a traditional approach, which takes into account the spectral response of the antennas recorded at specific points, the modes cannot be experimentally identified with EELS. Therefore, we employ the spectral and spatial sensitivity of EELS simultaneously. We propose several metrics that can be utilized to resolve the modes. First, we utilize electrodynamic simulations to verify that the metrics indeed represent the spectral positions of the plasmon modes. Next, we apply the metrics to experimental data, demonstrating their ability to resolve three of the above-mentioned modes (with transverse bonding and antibonding modes still unresolved), identify them unequivocally, and determine their energies. In this respect, the spatio-spectral metrics increase the information extracted from electron energy loss spectroscopy applied to plasmonic antennas.