Energy-loss- and thickness-dependent contrast in atomic-scale electron energy-loss spectroscopy
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Tan, Haiyan↗
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Low-loss electron energy loss spectroscopy: An atomic-resolution complement to optical spectroscopies and application to graphene
Photon-based spectroscopies previously played a central role in exploring the electronic properties of crystalline solids and thin films. They are a powerful tool for probing the electronic properties of nanostructures, but they are limited by lack of spatial resolution. On the other hand, electron-based spectroscopies, e.g., electron energy loss spectroscopy (EELS), are now capable of subangstrom spatial resolution. Core-loss EELS, a spatially resolved analog of x-ray absorption, has been used extensively in the study of inhomogeneous complex systems. In this paper, we demonstrate that low-loss EELS in an aberration-corrected scanning transmission electron microscope, which probes low-energy excitations, combined with a theoretical framework for simulating and analyzing the spectra, is a powerful tool to probe low-energy electron excitations with atomic-scale resolution. The theoretical component of the method combines density functional theory–based calculations of the excitations with dynamical scattering theory for the electron beam. We apply the method to monolayer graphene in order to demonstrate that atomic-scale contrast is inherent in low-loss EELS even in a perfectly periodic structure. The method is a complement to optical spectroscopy as it probes transitions entailing momentum transfer. The theoretical analysis identifies the spatial and orbital origins of excitations, holding the promise of ultimately becoming a powerful probe of the structure and electronic properties of individual point and extended defects in both crystals and inhomogeneous complex nanostructures. The approach can be extended to probe magnetic and vibrational properties with atomic resolution.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Tau energy loss and ultrahigh energy skimming tau neutrinos
For this paper, we consider propagation of high-energy earth-skimming taus produced in interactions of astrophysical tau neutrinos. For astrophysical tau neutrinos, we take generic power-law flux, E -2 and the cosmogenic flux initiated by the protons. We calculate tau energy loss in several approaches, such as dipole models and the phenomenological approach in which parametrization of the F 2 is used. We evaluate the tau neutrino charged-current cross section using the same approaches for consistency. We find that uncertainty in the neutrino cross section and in the tau energy loss partially compensate giving very small theoretical uncertainty in the emerging tau flux for distances ranging from 2 to 100 km and for the energy range between 10 6 and 10 11 GeV , focusing on energies above 10 8 GeV . When we consider uncertainties in the neutrino cross section, inelasticity in neutrino interactions and the tau energy loss, which are not correlated, i.e. they are not all calculated in the same approach, theoretical uncertainty ranges from about 30% and 60% at 10 8 GeV to about factors of 3.3 and 3.8 at 10 11 GeV for the E -2 flux and the cosmogenic flux, respectively, for the distance of 10 km rock. The spread in predictions significantly increases for much larger distances, e.g., ~ 1,000 km . Most of the uncertainty comes from the treatment of photonuclear interactions of the tau in transit through large distances. We also consider Monte Carlo calculation of the tau propagation and we find that the result for the emerging tau flux is in agreement with the result obtained using analytic approach. Our results are relevant to several experiments that are looking for skimming astrophysical taus, such as the Pierre Auger Observatory, HAWC and Ashra. We evaluate the aperture for the Auger and discuss briefly application to the other two experiments.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Retrieving the energy-loss function from valence electron energy-loss spectrum: Separation of bulk-, surface-losses and Cherenkov radiation
With recent rapid advancement in electron microscopy instrumentation, in particular, bright electron sources and monochromators, valence electron energy-loss spectroscopy (VEELS) has become attractive for retrieving band structures, optical properties, dielectric functions and phonon information of materials. However, Cherenkov radiation and surface-loss contribution signi cantly alter ne structures of VEELS, even in simple semiconductors and insulators. This leads to the problem that dielectric function or bandgap structure of these materials cannot be determined correctly if these e ects are not removed. In this work we present a solution to this dilemma. We demonstrate that energy-loss function and real part of inverse complex dielectric function can be retrieved from raw data of VEELS. Based on the calculated example of Si, the limitation of our approach is discussed. We believe that our approach represents an improvement over previous procedures and has a broad prospect for applications.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Differentiating the bonding states in calcium carbonate polymorphs by low-loss electron-energy-loss spectroscopy
Calcium carbonate is one of the important building components in organisms, especially the two most common polymorphs, calcite and aragonite. Here, to understand the difference in bonding state, the two polymorphs are characterized by valence (low-loss) electron energy loss spectroscopy. It is found that the difference in Ca M 23 edge originating from 3p to 3d states is consistent with the change of Ca-O bonds in the two studied polymorphs. Surprisingly, the measured Ca M 23 edge is in qualitative agreement with the calculated partial density of states (PDOS) of Ca-d states in contrast to their L edges (from 2p to 3d states) which are strongly influenced by atomic multiplet effect (spin-orbit coupling). This is because the atomic multiplet effect is much reduced for the Ca 3p orbital, which permits the corresponding Ca M 23 edge to be compared with the PDOS results. Our findings show insights that PDOS can potentially be used to interpret the M 23 edge of lighter 3d transition metals such as scandium, titanium, vanadium and chromium when such interpretation may not be achieved for their L edges.
36 MATERIALS SCIENCE↗
Nanoscale and Element-Specific Lattice Temperature Measurements Using Core-Loss Electron Energy-Loss Spectroscopy
Measuring nanoscale local temperatures, particularly in vertically integrated and multicomponent systems, remains challenging. Spectroscopic techniques like X-ray absorption and core-loss electron energy-loss spectroscopy (EELS) are sensitive to lattice temperature, but understanding thermal effects is nontrivial. This work explores the potential for nanoscale and element-specific core-loss thermometry by comparing the Si L2,3 edge’s temperature- dependent redshift against plasmon energy expansion thermometry (PEET) in a scanning TEM. Using density functional theory (DFT), time-dependent DFT, and the Bethe−Salpeter equation, we ab initio model both the Si L 2,3 and plasmon redshift. We find that the core-loss redshift occurs due to bandgap reduction from electron−phonon renormalization. Our results indicate that despite lower core-loss signal intensity compared to plasmon features, core-loss thermometry has key advantages and can be more accurate through standard spectral denoising. Specifically, we show that the Varshni equation easily interprets the core-loss redshift for semiconductors, which avoids plasmon spectral convolution for PEET in complex junctions and interfaces. We also find that core-loss thermometry is more accurate than PEET at modeling thermal lattice expansion in semiconductors, unless the specimen’s temperature-dependent dielectric properties are fully characterized. Furthermore, core-loss thermometry has the potential to measure nanoscale heating in multicomponent materials and stacked interfaces with elemental specificity at length scales smaller than the plasmon’s wave function.
Bethe–Salpeter equation↗
Competing effects of electronic and nuclear energy loss on microstructural evolution in ionic-covalent materials
Ever increasing energy needs have raised the demands for advanced fuels and cladding materials that withstand the extreme radiation environments with improved accident tolerance over a long period of time. Ceria (CeO2) is a well known ionic conductor that is isostructural with urania and plutonia-based nuclear fuels. In the context of nuclear fuels, immobilization and transmutation of actinides, CeO2 is a model system for radiation effect studies. Covalent silicon carbide (SiC) is a candidate for use as structural material in fusion, cladding material for fission reactors, and an inert matrix for the transmutation of plutonium and other radioactive actinides. Understanding microstructural change of these ionic-covalent materials to irradiation is important for advanced nuclear energy systems. While displacements from nuclear energy loss may be the primary contribution to damage accumulation in a crystalline matrix and a driving force for the grain boundary evolution in nanostructured materials, local non-equilibrium disorder and excitation through electronic energy loss may, however, produce additional damage or anneal pre-existing defects. At intermediate transit energies where electronic and nuclear energy losses are both significant, synergistic, additive or competitive processes may evolve that affect the dynamic response of materials to irradiation. The response of crystalline and nanostructured CeO2 and SiC to ion irradiation are studied under different nuclear and electronic stopping powers to describe some general material response in this transit energy regime. Although fast radiation-induced grain growth in CeO2 is evident with no phase transformation, different fluence and dose dependence on the growth rate is observed under Si and Au irradiations. While grain shrinkage and amorphization are observed in the nano-engineered 3C SiC with a high-density of stacking faults embedded in nanosize columnar grains, significantly enhanced radiation resistance is attributed to stacking faults that promote efficient point defect annihilation. Moreover, competing effects of electronic and nuclear energy loss on the damage accumulation and annihilation are observed in crystalline 4H-SiC. Systematic experiments and simulation effort are needed to understand the competitive or synergistic effects.
36 MATERIALS SCIENCE↗
Probing Battery Chemistry with Liquid Cell Electron Energy Loss Spectroscopy
We demonstrate the ability to apply electron energy loss spectroscopy (EELS) to follow the chemistry and oxidation states of LiMn 2 O 4 and Li 4 Ti 5 O1 2 battery electrodes within a battery solvent. The use and importance of in situ electrochemical cells coupled with a scanning/transmission electron microscope (S/TEM) has expanded and been applied to follow changes in battery chemistry during electrochemical cycling. Furthermore, we discuss experimental parameters that influence measurement sensitivity and provide a framework to apply this important analytical method to future in situ electrochemical studies.
25 ENERGY STORAGE↗
Nanostructural features degrading the performance of superconducting radio frequency niobium cavities revealed by transmission electron microscopy and electron energy loss spectroscopy
Nanoscale defect structure within the magnetic penetration depth of ∼100 nm is key to the performance limitations of niobium superconducting radio frequency cavities. Using a unique combination of advanced thermometry during cavity RF measurements, and TEM structural and compositional characterization of the samples extracted from cavity walls, we discover the existence of nanoscale hydrides in electropolished cavities limited by the high field Q slope, and show the decreased hydride formation in the electropolished cavity after 120 °C baking. Furthermore, we demonstrate that adding 800 °C hydrogen degassing followed by light buffered chemical polishing restores the hydride formation to the pre-120 °C bake level. We also show absence of niobium oxides along the grain boundaries and the modifications of the surface oxide upon 120 °C bake.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Effect of multipole excitations in electron energy-loss spectroscopy of surface plasmon modes in silver nanowires
We have characterized the surface plasmon resonance (SPR) in silver nanowires using spatially resolved electron energy loss spectroscopy (EELS) in the scanning transmission electron microscope. Non-symmetric EELS spectra due to high-k SPR propagation along the nanowire and spectral shifts due to higher-order mode excitation are observed when the beam is positioned near the tip of the nanowire. When the beam is far from the tip region and on the side of nanowire, no spectral shifts are observed as the beam is scanned in the radial direction of the nanowire. The experimental spectra are compared with three different theoretical approaches: direct numerical calculation of the energy loss, analytical models for energy loss, and numerical simulations using an optical model. All three models reproduce the spectral shifts as the electron beam approaches the cap of the nanowire. The analytical model reveals the origin of the shifts in high-order plasmon mode excitation.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Additive effects of electronic and nuclear energy loss in irradiation-induced amorphization of zircon
We used a combination of ion cascades and the unified thermal spike model to study the electronic effects from 800 keV Kr and Xe ion irradiation in zircon. We compared the damage production for four cases: (a) due to ion cascades alone, (b) due to ion cascades with the electronic energy loss activated as a friction term, (c) due to the thermal spike from the combined electronic and nuclear energy losses, and (d) due to ion cascades with electronic stopping and the electron-phonon interactions superimposed. As a result, we found that taking the electronic energy loss out as a friction term results in reduced damage, while the electronic electron-phonon interactions have additive impact on the final damage created per ion.
36 MATERIALS SCIENCE↗
Impact of inward turbulence spreading on energy loss of edge-localized modes
Nonlinear two-fluid and gyrofluid simulations show that an edge localized modes(ELM) crash has two phases: fast initial crash of ion temperature perturbation on the Alfvén time scale and slow turbulence spreading. The turbulencetransport phase is a slow encroachment of electron temperature perturbation due to the ELM event into pedestal region. Because of the inward turbulence spreading effect, the energy loss of an ELM decreases when density pedestal height increases. The Landau resonance yields the different cross phase-shift of ions and electrons. A 3 + 1 gyro-Landau-fluid model is implemented in BOUT++ framework. As a result, the gyrofluid simulations show that the kinetic effects have stabilizing effects on the ideal ballooning mode and the energy loss increases with the pedestal height.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Electron impact excitation of the electronic states of N2. III - Transitions in the 12.5-14.2-eV energy-loss region at incident energies of 40 and 60 eV
Analysis of electron energy-loss data at incident electron energies of 40 and 60 eV has led to the determination of normalized absolute differential cross sections for electron-impact excitation of five optically-allowed singlet states, two known triplet states, and two unknown triplet-like states of N2, lying in the energy-loss range 12.5-14.2 eV. The range of scattering angles was 5 to 138 deg. The optically allowed transitions and the known triplet excitations are identified. Cross sections for excitation to two unidentified triplet-like states at 13.155 and 13.395 eV were also obtained. The relationship of the generalized oscillator strength for the dipole-allowed states obtained from the described data to known optical oscillator strengths is discussed.
Chutjian, A.↗
Differential Measurements of Jet Substructure and Partonic Energy Loss in Au+Au Collisions at √ sNN = 200 GeV
The STAR collaboration presents jet substructure measurements related to both the momentum fraction and the opening angle within jets in p+p and Au+Au collisions at √sNN =200GeV. The substructure observables include SoftDrop groomed momentum fraction (zg), groomed jet radius (Rg), and subjet momentum fraction (zSJ) and opening angle (θSJ). The latter observable is introduced for the first time. Fully corrected subjet measurements are presented for p+p collisions and are compared to leading-order Monte Carlo models. The subjet θSJ distributions reflect the jets leading opening angle and are utilized as a proxy for the resolution scale of the medium in Au+Au collisions. We compare data from Au+Au collisions to those from p+p which are embedded in minimum-bias Au+Au events in order to include the effects of detector smearing and the heavy-ion collision underlying event. The subjet observables are shown to be more robust to the background than zg and Rg. We observe no significant modifications of the subjet observables within the two highest-energy, back-to-back jets, resulting in a distribution of opening angles and the splittings that are vacuumlike. We also report measurements of the differential dijet momentum imbalance (AJ) for jets of varying θSJ. We find no qualitative differences in energy loss signatures for varying angular scales in the range 0.1< θSJ<0.3, leading to the possible interpretation that energy loss in this population of high-momentum dijet pairs, is due to soft medium-induced gluon radiation from a single color charge as it traverses the medium.
Abdallah, M. S.↗
Impact of the pedestal plasma density on dynamics of edge localized mode crashes and energy loss scaling
The latest BOUT++ studies show an emerging understanding of dynamics of edge localized mode(ELM) crashes and the consistent collisionality scaling of ELMenergy losses with the world multi-tokamak database. A series of BOUT++ simulations are conducted to investigate the scaling characteristics of the ELMenergy losses vs collisionality via a density scan. Moreover, the linear results demonstrate that as the pedestal collisionality decreases, the growth rate of the peeling-ballooning modes decreases for high n but increases for low n (1 < n < 5), therefore the width of the growth rate spectrum γ(n) becomes narrower and the peak growth shifts to lower n. For nonlinear BOUT++ simulations show a two-stage process of ELM crash evolution of (i) initial bursts of pressure blob and void creation and (ii) inward void propagation. The inward void propagation stirs the top of pedestal plasma and yields an increasing ELM size with decreasing collisionality after a series of micro-bursts. The pedestal plasma density plays a major role in determining the ELMenergy loss through its effect on the edge bootstrap current and ion diamagnetic stabilization. Finally, the critical trend emerges as a transition (1) linearly from ballooning-dominated states at high collisionality to peeling-dominated states at low collisionality with decreasing density and (2) nonlinearly from turbulence spreading dynamics at high collisionality into avalanche-like dynamics at low collisionality.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Neutron Time-of-Flight Measurements of Charged-Particle Energy Loss in Inertial Confinement Fusion Plasmas
Neutron spectra from secondary 3 H(d,n)α reactions produced by an implosion of a deuterium-gas capsule at the National Ignition Facility have been measured with order-of-magnitude improvements in statistics and resolution over past experiments. Furthermore, these new data and their sensitivity to the energy loss of fast tritons emitted from thermal 2 H(d,p) 3 H reactions enable the first statistically significant investigation of charged-particle stopping via the emitted neutron spectrum. Radiation-hydrodynamic simulations, constrained to match a number of observables from the implosion, were used to predict the neutron spectra while employing two different energy loss models. This analysis represents the first test of stopping models under inertial confinement fusion conditions, covering plasma temperatures of k B T ≈ 1–4 keV and particle densities of n ≈ (12–2) × 10 24 cm –3 . Under these conditions, we find significant deviations of our data from a theory employing classical collisions whereas the theory including quantum diffraction agrees with our data.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Energy loss of high-energy cosmic rays in pair- producing collisions with ambient photons
Energy loss of high energy cosmic rays traversing isotropic radiation field of arbitrary energy spectrum in pair producing collisions with ambient photons
Blumenthal, G. R.↗