A new type of excitations by highly focused electron beams in scanning transmission electron microscopes is predicted for nanoparticles. The calculated electron energy loss spectra of metallic (silver) and insulating (SiO(sub2)) nanoplatelets reveal dramatic enhancement of radiative electromagnetic modes within the light cone, allowed by the breakdown of momentum conservation in the inelastic scattering event. These modes can be accessed with e-beams in the vacuum far-field zone, similarly to the recently developed far-field optics based on surface plasmon resonances.
A quantum mechanical scattering theory for relativistic, highly focused electron beams near nanoscopic platelets is presented, revealing a new excitation mechanism due to the electron wave scattering from the platelet edges. Radiative electromagnetic excitations within the light cone are shown to arise, allowed by the breakdown of momentum conservation along the beam axis in the inelastic scattering process. Calculated for metallic (silver and gold) and insulating (SiO2 and MgO) nanoplatelets, new radiative features are revealed above the main surface plasmon-polariton peak, and dramatic enhancements in the electron energy loss probability at gaps of the classical spectra, are found. The corresponding radiation should be detectable in the vacuum far-field zone, with e-beams exploited as sensitive tip-detectors of electronically excited nanostructures.
Results obtained from the optical absorption and photoluminescence (PL) spectroscopy experiments have shown the formation of excitons in the silver-exchanged glass samples. These findings are reported here for the first time. Further, we investigate the dramatic changes in the photoemission properties of the silver-exchanged glass samples as a function of postannealing temperature. Observed changes are thought to be due to the structural rearrangements of silver and oxygen bonding during the heat treatments of the glass matrix. In fact, photoelectron spectroscopy does reveal these chemical transformations of silver-exchanged soda glass samples caused by the thermal effects of annealing in a high vacuum atmosphere. An important correlation between temperature-induced changes of the PL intensity and thermal growth of the silver nanoparticles has been established in this Letter through precise spectroscopic studies.
Raman forbidden modes and surface defect related Raman features in SnO_2 nanostructures carry information about disorder and surface defects which strongly influence important technological applications like catalysis and sensing. Due to the weak intensities of these peaks, it is difficult to identify these features by using conventional Raman spectroscopy. Tip enhanced Raman spectroscopy (TERS) studies conducted on SnO_2 nanoparticles (NPs) of size 4 and 25 nm have offered significant insights of prevalent defects and disorders. Along with one order enhancement in symmetry allowed Raman modes, new peaks related to disorder and surface defects of SnO_2 NPs were found with significant intensity. Temperature dependent Raman studies were also carried out for these NPs and correlated with the TERS spectra. For quasi-quantum dot sized 4 nm NPs, the TERS study was found to be the best technique to probe the finite size related Raman forbidden modes.
Transmission electron microscopy, scanning transmission electron tomography, and electron energy loss spectroscopy were used to characterize three-dimensional artificial Si nanostructures called metalattices, focusing on Si metalattices synthesized by high-pressure confined chemical vapor deposition in 30-nm colloidal silica templates with ~7 and ~12 nm meta-atoms and ~2 nm meta-bonds. The meta-atoms closely replicate the shape of the tetrahedral and octahedral interstitial sites of the face-entered cubic colloidal silica template. Composed of either amorphous or nanocrystalline silicon, the metalattice exhibits long-range order and interconnectivity in two-dimensional micrographs and three-dimensional reconstructions. Electron energy loss spectroscopy provides information on local electronic structure. The Si L2,3 core-loss edge is blue-shifted compared to the onset for bulk Si, with the meta-bonds displaying a larger shift (0.55 eV) than the two types of meta-atoms (0.30 and 0.17 eV). Local density of state calculations using an empirical tight binding method are in reasonable agreement.