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↗
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↗
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↗
Structural Characterization of Loblolly Pine Derived Biochar by X-ray Diffraction and Electron Energy Loss Spectroscopy
Biochar from lignocellulosic biomass is emerging as a sustainable material with versatile applications, but its detailed properties are poorly understood because of its structural complexity. We propose a biochar structural development model based on experimental results including composition analysis, surface area and pore analysis, X-ray diffraction analysis, electron microscopy imaging, and electron energy loss spectroscopy. Loblolly pine derived biochars were produced at different carbonization temperatures between 300 to 1000 °C. Fixed carbon, sp 2 content, and number of graphene layers increased with increased carbonization temperature. Alternating average C–C bond length, interlayer spacing distance, and layer coherence length were observed. Bulk plasmon excitation energy was correlated to the average C–C bond length, and it serves as a good indicator of the carbon structure development when compared to the perfect graphitic carbon structure. On the basis of the experimental results, four different structural development phases are identified, which provide a comprehensive understanding of biochar nanocarbon crystallite development. Unlike previous biochar structure models, which proposed radially growing polyaromatic carbon crystallite, we propose a lengthwise growing polyaromatic carbon crystallite model. Furthermore, this experiment-based biochar model should be helpful when determining the structure of unknown biomass-derived carbon materials and disordered pyrolytic carbon materials.
Biomass carbonization↗
Direct Nanoscale Characterization of Deep Levels in AgCuInGaSe 2 Using Electron Energy–Loss Spectroscopy in the Scanning Transmission Electron Microscope
A new experimental framework for the characterization of defects in semiconductors is demonstrated. Through the direct, energy-resolved correlation of three analytical techniques spanning six orders of magnitude in spatial resolution, a critical mid-bandgap electronic trap level (E V + 0.56 eV) within Ag 0.2 Cu 0.8 In 1–x Ga x Se 2 is traced to its nanoscale physical location and chemical source. This is achieved through a stepwise, site-specific correlated characterization workflow consisting of device-scale (≈1 mm 2 ) deep level transient spectroscopy (DLTS) to survey the traps present, scanning probe–based DLTS (scanning-DLTS) for mesoscale-resolved (hundreds of nanometers) mapping of the target trap state’s spatial distribution, and scanning transmission electron microscope based electron energy-loss spectroscopy (STEM-EELS) and X-ray energy-dispersive spectroscopy for nanoscale energy-, structure, and chemical-resolved investigation of the defect source. Furthermore, this first demonstration of the direct observation of sub-bandgap defect levels via STEM-EELS, combined with the DLTS methods, provides strong evidence that the longsuspected Cu In/Ga substitutional defects are indeed the most likely source of the E V + 0.56 eV trap state and serves as a key example of this approach for the fundamental identification of defects within semiconductors, in general.
14 SOLAR ENERGY↗
High resolution electron energy loss spectroscopy with two-dimensional energy and momentum mapping
High resolution electron energy loss spectroscopy (HREELS) is a powerful technique to probe vibrational and electronic excitations at surfaces. The dispersion relation of surface excitations, i.e., energy as a function of momentum, has in the past, been obtained by measuring the energy loss at a fixed angle (momentum) and then rotating sample, monochromator, or analyzer. Here, we introduce a new strategy for HREELS, utilizing a specially designed lens system with a double-cylindrical Ibach-type monochromator combined with a commercial VG Scienta hemispherical electron energy analyzer, which can simultaneously measure the energy and momentum of the scattered electrons. The new system possesses high angular resolution (<0.1°), detecting efficiency and sampling density. The capabilities of this system are demonstrated using Bi{sub 2}Sr{sub 2}CaCu{sub 2}O{sub 8+δ}. The time required to obtain a complete dispersion spectrum is at least one order of magnitude shorter than conventional spectrometers, with improved momentum resolution and no loss in energy resolution.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗