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Register a new userFar-field interaction of focused relativistic electron beams in electron energy loss spectroscopy of nanoscopic platelets
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Added by
Itskovsky Matvey A.
Publication date
2008
fields
Physics
and research's language is
English
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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.
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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.
Recently it has been demonstrated that a careful treatment of both longitudinal and transverse matrix elements in electron energy loss spectra can explain the mystery of relativistic effects on the {it magic angle}. Here we show that there is an additional correction of order $(Zalpha)^2$ where $Z$ is the atomic number and $alpha$ the fine structure constant, which is not necessarily small for heavy elements. Moreover, we suggest that macroscopic electrodynamic effects can give further corrections which can break the sample-independence of the magic angle.
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.
The spatial distributions of anti-bonding $pi^ast$ and $sigma^ast$ states in epitaxial graphene multilayers are mapped using electron energy-loss spectroscopy in a scanning transmission electron microscope. Inelastic channeling simulations validate the interpretation of the spatially-resolved signals in terms of electronic orbitals, and demonstrate the crucial effect of the material thickness on the experimental capability to resolve the distribution of unoccupied states. This work illustrates the current potential of core-level electron energy-loss spectroscopy towards the direct visualization of electronic orbitals in a wide range of materials, of huge interest to better understand chemical bonding among many other properties at interfaces and defects in solids.
Exploiting the information provided by electron energy-loss spectroscopy (EELS) requires reliable access to the low-loss region where the zero-loss peak (ZLP) often overwhelms the contributions associated to inelastic scatterings off the specimen. Here we deploy machine learning techniques developed in particle physics to realise a model-independent, multidimensional determination of the ZLP with a faithful uncertainty estimate. This novel method is then applied to subtract the ZLP for EEL spectra acquired in flower-like WS$_2$ nanostructures characterised by a 2H/3R mixed polytypism. From the resulting subtracted spectra we determine the nature and value of the bandgap of polytypic WS$_2$, finding $E_{rm BG} = 1.6_{-0.2}^{+0.3},{rm eV}$ with a clear preference for an indirect bandgap. Further, we demonstrate how this method enables us to robustly identify excitonic transitions down to very small energy losses. Our approach has been implemented and made available in an open source Python package dubbed EELSfitter.
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