Electron Energy Loss Spectroscopy Simulations Research Articles

Spectroscopic Observation and Modeling of Photonic Modes in CeO2 Nanostructures.

Photonic modes in dielectric nanostructures, e.g., wide gap semiconductor like CeO2 (ceria), have the potential for various applications such as information transmission and sensing technology. To fully understand the properties of such phenomenon at the nanoscale, electron energy-loss spectroscopy (EELS) in a scanning transmission electron microscope was employed to detect and explore photonic modes in well-defined ceria nanocubes. To facilitate the interpretation of the observations, EELS simulations were performed with finite-element methods. The simulations allow the electric and magnetic field distributions associated with different modes to be determined. A simple analytical eigenfunction model was also used to estimate the energy of the photonic modes. In addition, by comparing various spectra taken at different location relative to the cube, the effect of the surrounding environment on the modes could be sensed. This work gives a high-resolution description of the photonic modes' properties in nanostructures, while demonstrating the advantage of EELS in characterizing optical phenomena locally.

Simulating Electron Energy-Loss Spectroscopy and Cathodoluminescence for Particles in Arbitrary Host Medium Using the Discrete Dipole Approximation

Electron energy-loss spectroscopy (EELS) and cathodoluminescence (CL) are widely used experimental techniques for characterization of nanoparticles. The discrete dipole approximation (DDA) is a numerically exact method for simulating interaction of electromagnetic waves with particles of arbitrary shape and internal structure. In this work we extend the DDA to simulate EELS and CL for particles embedded into arbitrary (even absorbing) unbounded host medium. The latter includes the case of the dense medium, supporting the Cherenkov radiation of the electron, which has never been considered in EELS simulations before. We build a rigorous theoretical framework based on the volume-integral equation, final expressions from which are implemented in the open-source software package ADDA. This implementation agrees with both the Lorenz-Mie theory and the boundary-element method for spheres in vacuum and moderately dense host medium. And it successfully reproduces the published experiments for particles encapsulated in finite substrates. The latter is shown for both moderately dense and Cherenkov cases - a gold nanorod in $\text{SiO}_{\text{2}}$ and a silver sphere in $\text{SiN}_{\text{x}}$ respectively.

Several factors influencing energy-loss near-edge structure calculations using Wien2k.

Electron energy-loss spectroscopy (EELS) is widely applied combining with transmission electron microscopes with high spatial resolution, but its interpretation is a challenging task. One of the reasons is that the factors affecting EELS are very complicated. In this paper, we focus on the several factors involved in density functional theory (DFT) calculations. The sensitivity of calculated energy-loss near-edge structure (ELNES) to spin order, pressure and on-site Coulomb energy U has been discussed. Since EELS technique detects the local environment of atoms, the influence of spin order cannot be ignored. The chemical shifts and peak intensity of ELNES are also closely related to corresponding pressure. The correlation effects are very important for transition metal compounds and play a key role in EELS simulations. An overview of the effects of these factors on the ELNES is presented with the help of Wien2k code. The antiferromagnetic order results in the decreasing of intensities of related peaks and the moving of the peaks to high energy loss. The decreasing of lattice parameters causes the ELNES peaks to shift to high energy loss, and the peak shifts at the higher energy loss are more significant. The increase of correlation effect leads to the ELNES peaks to shift to high energy loss accompanied by the increase of the relative intensity of the peaks which locate at higher energy loss. Our work helps to understand how these factors affect EELS and to explain and predict the experimental EELS spectra. Through the discussion of these factors, we propose that some factors could not be ignored in EELS simulations.

Efficient and Versatile Model for Vibrational STEM-EELS.

We introduce a novel method for the simulation of the impact scattering in vibrational scanning transmission electron microscopy electron energy loss spectroscopy simulations. The phonon-loss process is modeled by a combination of molecular dynamics and elastic multislice calculations within a modified frozen phonon approximation. The key idea is thereby to use a so-called δ thermostat in the classical molecular dynamics simulation to generate frequency dependent configurations of the vibrating specimen's atomic structure. The method includes correlated motion of atoms and provides vibrational spectrum images at a cost comparable to standard frozen phonon calculations. We demonstrate good agreement of our method with simulations and experiments for a 15nm flake of hexagonal boron nitride.

Electron energy loss spectroscopy simulation by a frequency domain surface integral equation solver

Plasmonic nanoparticles have been mostly studied using conventional light sources. Recently, electron energy loss spectroscopy (EELS) has started to be used to analyze plasmonic nanoparticles where incident electromagnetic fields are created by swift electrons. To accurately simulate EELS experiments, several numerical methods have been adapted. In this paper, a frequency domain surface integral equation (FDSIE) solver is modified to simulate EELS for plasmonic nanoparticles of gold and silver. Accuracy and versatility of the proposed FDSIE solver are shown by several numerical examples and compared to existing numerical, analytical, and experimental results.

Simulating electron energy loss spectroscopy with the MNPBEM toolbox

Within the MNPBEM toolbox, we show how to simulate electron energy loss spectroscopy (EELS) of plasmonic nanoparticles using a boundary element method approach. The methodology underlying our approach closely follows the concepts developed by García de Abajo and coworkers (Garcia de Abajo, 2010). We introduce two classes eelsret and eelsstat that allow in combination with our recently developed MNPBEM toolbox for a simple, robust, and efficient computation of EEL spectra and maps. The classes are accompanied by a number of demo programs for EELS simulation of metallic nanospheres, nanodisks, and nanotriangles, and for electron trajectories passing by or penetrating through the metallic nanoparticles. We also discuss how to compute electric fields induced by the electron beam and cathodoluminescence. Program summaryProgram title:MNPBEM toolboxCatalogue identifier: AEKJ_v2_0Program summary URL:http://cpc.cs.qub.ac.uk/summaries/AEKJ_v2_0.htmlProgram obtainable from: CPC Program Library, Queen’s University, Belfast, N. IrelandLicensing provisions: Standard CPC licence, http://cpc.cs.qub.ac.uk/licence/licence.htmlNo. of lines in distributed program, including test data, etc.: 38886No. of bytes in distributed program, including test data, etc.: 1222650Distribution format: tar.gzProgramming language: Matlab 7.11.0 (R2010b).Computer: Any which supports Matlab 7.11.0 (R2010b).Operating system: Any which supports Matlab 7.11.0 (R2010b).RAM:≥1 GBClassification: 18.Catalogue identifier of previous version: AEKJ_v1_0Journal reference of previous version: Comput. Phys. Comm. 183 (2012) 370External routines: MESH2D available at www.mathworks.comDoes the new version supersede the previous version?: YesNature of problem:Simulation of electron energy loss spectroscopy (EELS) for plasmonic nanoparticles.Solution method:Boundary element method using electromagnetic potentials.Reasons for new version:The new version of the toolbox includes two additional classes for the simulation of electron energy loss spectroscopy (EELS) of plasmonic nanoparticles, and corrects a few minor bugs and inconsistencies.Summary of revisions:New classes “eelsstat” and “eelsret” for the simulation of electron energy loss spectroscopy (EELS) of plasmonic nanoparticles have been added. A few minor errors in the implementation of dipole excitation have been corrected.Running time:Depending on surface discretization between seconds and hours.

Seeing oxygen disorder in YSZ/SrTiO3colossal ionic conductor heterostructures using EELS

Colossal ionic conductivity was recently discovered in YSZ/SrTiO3 multilayers and was explained in terms of strain- and interface-enhanced disorder of the O sublattice. In the present paper we use a combination of scanning transmission electron microscopy and electron energy loss spectroscopy (EELS) and theoretical EELS simulations to confirm the presence of a disordered YSZ O sublattice in coherent YSZ/SrTiO3 multilayers. O K-edge fine structure simulated for the strained disordered O sublattice phase of YSZ possesses blurred-out features compared to that of ordered cubic bulk YSZ, and experimental EELS fine structure taken from the strained YSZ of coherent YSZ/SrTiO3 thin films is similarly blurred out. Elemental mapping is shown to be capable of resolving ordered YSZ O sublattices. Elemental mapping of O in the coherent YSZ/STO multilayers is presented in which the O sublattice is seen to be clearly resolved in the STO but blurred out in the YSZ, indicating it to be disordered. In addition, we present imaging and EELS results which show that strained regions exist at the incoherent interfaces of YSZ islands in STO with blurred out fine structure, suggesting these incoherent regions may also support high ionic conductivities. Recently, Cavallaro et al. reported electronic conductivities in samples of incoherent disconnected islands embedded in STO that are similar to the islands described herein. The presence of a region of O depleted STO at the interface with incoherent YSZ islands is revealed by EELS elemental mapping, implying the n-type doping of STO/YSZ nanocomposites with disconnected incoherent YSZ islands.

EELS and optical response of a noble metal nanoparticle in the frame of a discrete dipole approximation

Surface plasmons of noble metal nanoparticles have recently been studied by Electron Energy-Loss Spectroscopy (EELS) performed in an electron microscope. We present here the basic formalism for EELS simulations in a Discrete Dipole Approximation (DDA) framework for such surface excitations. We compare EELS data and optical properties of a silver triangular nanoprism and show that the spatial variation of surface plasmon excitation probabilities allows to discriminate modes of similar energies. We also emphasize the importance of the substrate polarization effect to reliably describe experimental data.