Ultra-high Energy Resolution Research Articles

The origin of the straight propagation of the σ phase in a Ni-based single crystal superalloy at elevated temperature

Topologically close-packed (TCP) phases, although inherently hard, are commonly perceived as detrimental in various alloys. In Ni-based single crystal superalloys (Ni-SXs), the primary adverse impact of TCP phases on material mechanical properties stems from their direct propagation, disrupting the original γ/γ′ dual-phase structure and leading to cleavage along the TCP phases under applied stress. Understanding the specific reasons for the straight propagation of TCP phases through the complex phase structure is essential for mitigating or potentially reversing their detrimental effects on material performance, a challenge that remains elusive. This study addressed this challenge by employing ultra-high spatial and energy resolution transmission electron microscopy (TEM) characterization, coupled with in situ scanning transmission electron microscopy (STEM) heating experiments in a fourth-generation Ni-based single crystal superalloy. Our research unveiled a significant phase-separation process during the incubation stage preceding σ phase formation at elevated temperatures, driven by the diffusion of atoms. Notably, domains of the γ′ phase, characterized by a scale of tens of nanometers, emerged within preexisting γ phases, and vice versa. This phenomenon reconstructed the original γ/γ′ dual-phase structure, leading to a finely refined dual-phase structure. The refined structure effectively reduced the diffusion distance of alloy elements necessary for forming σ phases. Consequently, the σ phases nucleated randomly and propagated directly through the newly refined γ/γ′ dual-phase structure. Throughout the thickening process, the notable difference in the diffusivity of alloying elements eventually resulted in the growth of a highly defective σ phase structure.

Magnetically propagating Hund’s exciton in van der Waals antiferromagnet NiPS3

Magnetic van der Waals (vdW) materials have opened new frontiers for realizing novel many-body phenomena. Recently NiPS3 has received intense interest since it hosts an excitonic quasiparticle whose properties appear to be intimately linked to the magnetic state of the lattice. Despite extensive studies, the electronic character, mobility, and magnetic interactions of the exciton remain unresolved. Here we address these issues by measuring NiPS3 with ultra-high energy resolution resonant inelastic x-ray scattering (RIXS). We find that Hund’s exchange interactions are primarily responsible for the energy of formation of the exciton. Measuring the dispersion of the Hund’s exciton reveals that it propagates in a way that is analogous to a double-magnon. We trace this unique behavior to fundamental similarities between the NiPS3 exciton hopping and spin exchange processes, underlining the unique magnetic characteristics of this novel quasiparticle.

Distinguishing Quasiparticle-Phonon Interactions by Ultrahigh-Resolution Lifetime Measurements.

We present a determination of quasiparticle-phonon interaction strengths at surfaces through measurements of phonon spectra with ultrahigh energy resolution. The lifetimes of low energy surface phonons on a pristine Ru(0001) surface were determined over a wide range of temperatures and an analysis of the temperature dependence enables us to attribute separate contributions from electron-phonon interactions, phonon-phonon interactions, and defect-phonon interactions. Strong electron-phonon interactions are evident at all temperatures and we show they dominate over phonon-phonon interactions below 400K.

Ultra-high Energy Resolution EELS and 4D STEM at Cryogenic Temperatures.

Ultra-high Energy Resolution EELS and 4D STEM at Cryogenic Temperatures.

Determination of absolute Np L x-ray emission intensities from 241Am decay using a metallic magnetic calorimeter

Photon emission intensities of radionuclides, i.e. the number of emitted photons per decay, are the single most important decay data when the photon spectrometry technique is employed in ionizing radiation metrology. However, their precise measurement is problematic because they are usually determined by photon spectrometry with spectrometers having a detection efficiency calibrated with x-ray and γ-ray emission intensities from other radionuclides. Therefore, these intensities are ultimately interdependent and correlated to some extent. A novel method was applied to determine the photon intensities of α-emitting radionuclides by measuring the ratio between the rate of photons in the full energy peaks and the rate of detected α-particles with the same detection set-up. Thus, there is no need to calibrate the detection efficiency and to standardize calibration sources by primary methods. The main condition to reach low uncertainties is to have a spectrometer with an intrinsic detection efficiency close to unity for the measured photons and α-particles. This condition was fulfilled by a metallic magnetic calorimeter (MMC) with an intrinsic efficiency of around 99% between 5 keV and 25 keV. In addition, the MMC provides an ultra-high energy resolution of 28 eV (full width at half maximum), facilitating the processing of the spectrum. The method was applied to determine L x-ray emission intensities from the decay of 241Am(α) → 237Np emitted between 11.9 keV and 22.4 keV. A total L x-ray emission intensity of 37.90 (12) per 100 disintegrations was obtained; the value agrees well with previous measurements and has a lower uncertainty. The uncertainties of the L x-ray groups Lα, Lηβ and Lγ were improved by a factor of two. Moreover, due to the high-energy resolution of 28 eV, a detailed set of 33 L x-ray emission intensities are provided.

Fate of charge order in overdoped La-based cuprates

In high-temperature cuprate superconductors, stripe order refers broadly to a coupled spin and charge modulation with a commensuration of eight and four lattice units, respectively. How this stripe order evolves across optimal doping remains a controversial question. Here we present a systematic resonant inelastic x-ray scattering study of weak charge correlations in La2−xSrxCuO4 and La1.8−xEu0.2SrxCuO4. Ultra high energy resolution experiments demonstrate the importance of the separation of inelastic and elastic scattering processes. Long-range temperature-dependent stripe order is only found below optimal doping. At higher doping, short-range temperature-independent correlations are present up to the highest doping measured. This transformation is distinct from and preempts the pseudogap critical doping. We argue that the doping and temperature-independent short-range correlations originate from unresolved electron–phonon coupling that broadly peaks at the stripe ordering vector. In La2−xSrxCuO4, long-range static stripe order vanishes around optimal doping and we discuss both quantum critical and crossover scenarios.

Experimental Evaluation of a 3-D CZT Imaging Spectrometer for Potential Use in Compton-Enhanced PET Imaging.

We constructed a prototype positron emission tomography (PET) system and experimentally evaluated large-volume 3-D cadmium zinc telluride (CZT) detectors for potential use in Compton-enhanced PET imaging. The CZT spectrometer offers sub-0.5-mm spatial resolution, an ultrahigh energy resolution (~1% @ 511 keV), and the capability of detecting multiple gamma-ray interactions that simultaneously occurred. The system consists of four CZT detector panels with a detection area of around 4.4 cm × 4.4 cm. The distance between the front surfaces of the two opposite CZT detector panels is ~80 mm. This system allows us to detect coincident annihilation photons and Compton interactions inside the detectors and then, exploit Compton kinematics to predict the first Compton interaction site and reject chance coincidences. We have developed a numerical integration technique to model the near-field Compton response that incorporates Doppler broadening, detector's finite resolutions, and the distance between the first and second interactions. This method was used to effectively reject random and scattered coincidence events. In the preliminary imaging studies, we have used point sources, line sources, a custom-designed resolution phantom, and a commercial image quality (IQ) phantom to demonstrate an imaging resolution of approximately 0.75 mm in PET images, and Compton-based enhancement.

Design of Ultrahigh Energy Resolution RIXS Beamline at NanoTerasu

The optical design of the ultrahigh-resolution RIXS beamline, which is currently developed at NanoTerasu in Japan, is described. The main goal of this beamline is to perform ultrahigh-resolution RIXS measurements with a total energy resolution of <10 meV at 250–1000 eV with E/ΔE>150,000 for both beamline and RIXS spectrometer. To achieve the ultra-high resolution, a 2D-RIXS spectrometer using energy-dispersive X-ray is employed to compensate for lower throughput at higher energy resolution, and the optics of the beamline is optimized for the 2D-RIXS spectrometer. A vertically dispersing in-focus variable-included-angle varied-line-spacing plane grating monochromator is employed for the beamline, with an entrance slit to ensure the ultrahigh resolution. First and second mirrors focus X-ray on entrance slits vertically and horizontally, respectively, and the divergent X-ray is irradiated onto the grating. For the 2D-RIXS spectrometer, there is no exit slit, and the vertically energy-dispersed X-ray is irradiated directly onto a sample. In front of the sample, X-ray is horizontally refocused by a Wolter type-I mirror. The expected horizontal focus size at the sample is ~0.7 μm. The expected photon flux is ~1×1011 photons/s at 500–1000 eV with a virtual slit width of 2 μm required for E/ΔE>150,000. The height of the dispersed X-ray available in the 2D-RIXS spectrometer is ~120 μm, which allows the use of a remarkably high flux of ~6×1012 photons/s, and the beamline will serve as an ultrahigh-resolution and high-efficiency RIXS facility.

Multi-Sun EELS: Ultra-High Energy Resolution combined with High Spatial Resolution and High Beam Current

Multi-Sun EELS: Ultra-High Energy Resolution combined with High Spatial Resolution and High Beam Current

Unusual Band Splitting and Superconducting Gap Evolution with Sulfur Substitution in FeSe

High-resolution angle-resolved photoemission measurements were taken on FeSe1–x S x (x = 0, 0.04, and 0.08) superconductors. With an ultrahigh energy resolution of 0.4 meV, unusual two hole bands near the Brillouin-zone center, which was possibly a result of additional symmetry breaking, were identified in all the sulfur-substituted samples. In addition, in both of the hole bands highly anisotropic superconducting gaps with resolution limited nodes were evidenced. We find that the larger superconducting gap on the outer hole band is reduced linearly to the nematic transition temperature while the gap on the inner hole is nearly S-substitution independent. Our observations strongly suggest that the superconducting gap increases with enhanced nematicity although the superconducting transition temperature is not only governed by the pairing strength, demonstrating strong constraints on theories in the FeSe family.

Features and applications of the energy shift of the topological surface state

Contemporary studies of magnetic topological insulators (TIs) aimed at investigating Dirac point (DP) gaps by angle-resolved photoemission spectroscopy (ARPES) require ultrahigh energy, momentum, and spatial resolution. Despite satisfying all these conditions, accurate measurements can be spoiled by the well-known, but often neglected, effect of the energy shift of bands, in particular the topological surface state (TSS), due to sample contamination and irradiation. Thus, in this work we focus on the effect of TI irradiation with laser light ($h\ensuremath{\nu}=6.3$ eV) on the measurability of its electronic structure using the ARPES method. We find that the distribution of the shifted TSS is sufficiently localized and remains stable over time under constant conditions. Therefore, it can be used to store information. The TSS retains its spin pattern regardless of irradiation, as demonstrated by dichroic ARPES measurements. However, irradiation leads to a significant broadening of the TSS, accompanied by a drop in its intensity. All these factors complicate the analysis of the states near the DP and the DP gap size. Finally, using a simple model, we demonstrate the variability of the DP gap over time in the resulting ARPES image, caused by both shift and broadening effects. Thus, accurate values of the DP gap can be obtained by measuring over a relatively small period of time, which is determined by a certain time constant of the energy shift.

Advances in ultrahigh-energy resolution EELS: phonons, infrared plasmons and strongly coupled modes.

Nowadays, sub-50 meV atom-wide electron probes are routinely produced for electron energy loss spectroscopy in transmission electron microscopes due to monochromator technology advances. We review how gradual improvements in energy resolution enabled the study of very low-energy excitations such as lattice phonons, molecular vibrations, infrared plasmons and strongly coupled hybrid modes in nanomaterials. Starting with the theoretical framework needed to treat inelastic electron scattering from phonons in solids, we illustrate contributions in detecting optical surface phonons in photonic structures. We discuss phonon mapping capabilities in real and reciprocal space, and the localized phonon response near nano-/atomic-scale structural features. We also survey the progress of aloof spectroscopy in studying vibrations in organic materials and applications in measuring local temperature and photonic density of states in single nanostructures using phonon scattering. We then turn towards studies on infrared plasmons in metals and semiconductors. Spectroscopy analyses now extend towards probing extremely complex broadband platforms, the effects of defects and nanogaps, and some far-reaching investigations towards uncovering plasmon lifetime and 3D photonic density of states. In doped semiconductors, we review research on the use of the electron probe to correlate local doping concentration and atomic-scale defects with the plasmonic response. Finally, we discuss advances in studying strong coupling phenomena in plasmon-exciton and plasmon-phonon systems. Overall, the wealth of information gained extends our knowledge about nanomaterial properties and elementary excitations, illustrating the powerful capabilities of high-energy resolution scanning transmission electron microscopy-electron energy loss spectrometry.

Controlled Experiments and Optimized Theory of Absorption Spectra of Li Metal and Salts.

Investigation of Li metal and ionic compounds through experimental and theoretical spectroscopy has been of tremendous interest due to their prospective applications in Li-metal and Li-ion batteries. Li K-edge soft X-ray absorption spectroscopy (sXAS) provides the most direct spectroscopic characterization; unfortunately, due to the low core-level energy and the highly reactive surface, Li-K sXAS of Li metal has been extremely challenging, as evidenced by many controversial reports. Here, through controlled and ultra-high energy resolution experiments of two kinds of in situ prepared samples, we report the intrinsic Li-K sXAS of Li-metal that displays a prominent leading peak that has not been revealed before. Furthermore, theoretical simulations show that, due to the low number of valence electrons in Li, the Li-K sXAS is strongly affected by the response of the valence electrons to the core hole. We successfully reproduce the Li-K sXAS by state-of-the-art calculations with considerations of a number of relevant parameters such as temperature, energy resolution, and, especially, contributions from transitions which are forbidden in the single-particle treatment. Such a comparative experimental and theoretical investigation is further extended to a series of Li ionic compounds, which highlight the importance of considering the total and single-particle energies for obtaining an accurate alignment of the spectra. Our work provides the first reliable Li-K sXAS of the Li metal surface with advanced theoretical calculations. The experimental and theoretical results provide a critical benchmark for studying Li chemistry in both metallic and ionic states.

Ultrafast extreme ultraviolet photoemission electron microscope.

Here, we report our newly built table-top ultrafast extreme ultraviolet (EUV) photoemission electron microscope. The coherent ultrafast EUV light is served by a single order harmonic, which is generated by the interaction between the intense 800-nm femtosecond laser and noble gases in the hollow core fiber. The required order of the harmonic is selected out by a single grating in the off-plane mount and focused on the sample in the ultrahigh vacuum chamber of the photoemission electron microscope. Using metal gold and copper samples, the spatial resolution is calibrated to be better than 50nm and the energy resolution is calibrated to be better than 300 meV. This microscope provides an advanced tool for studying electron dynamics covering the full Brillouin zone of solid materials with ultrahigh time, space, and energy resolution.

In-situ observation of trapped carriers in organic metal halide perovskite films with ultra-fast temporal and ultra-high energetic resolutions

We in-situ observe the ultrafast dynamics of trapped carriers in organic methyl ammonium lead halide perovskite thin films by ultrafast photocurrent spectroscopy with a sub-25 picosecond time resolution. Upon ultrafast laser excitation, trapped carriers follow a phonon assisted tunneling mechanism and a hopping transport mechanism along ultra-shallow to shallow trap states ranging from 1.72–11.51 millielectronvolts and is demonstrated by time-dependent and independent activation energies. Using temperature as an energetic ruler, we map trap states with ultra-high energy resolution down to < 0.01 millielectronvolt. In addition to carrier mobility of ~4 cm2V−1s−1 and lifetime of ~1 nanosecond, we validate the above transport mechanisms by highlighting trap state dynamics, including trapping rates, de-trapping rates and trap properties, such as trap density, trap levels, and capture-cross sections. In this work we establish a foundation for trap dynamics in high defect-tolerant perovskites with ultra-fast temporal and ultra-high energetic resolution.

Advanced Electron Microscopy of Multi-Valent Cathode Materials

Recent progress in the field of scanning/transmission electron microscopy (S/TEM) has resulted in intense electron probes providing an ultra-high spatial (e.g. sub-Å) and energy (3 meV) resolution, with a previously unattainable signal-to-noise ratio. Furthermore, the STEM-based methods: direct imaging of both heavy and light elements, and both the energy-dispersive X-ray (EDX) and electron energy loss (EEL) spectroscopies are becoming the most promising characterization tools for battery materials, providing an unprecedented opportunity to probe the evolution of structure and electronic state of the cathodes following their electrochemical activity. The current talk will focus on the electron microscopy characterization of various materials that are considered as potential cathodes for the multivalent batteries, including transition metal (TM) oxides and polyanionic compounds. Materials were characterized using aberration-corrected JEOL JEM-ARM200CF, equipped with a cold field emission and operated at 200 kV, in pristine, cycled, and in-situ irradiated phases exploring their structure, chemistry, and electronic states. The in-situ technique mimics the electrochemical cell and allows for single-particle tracking of the dynamic processes occurring upon oxygen loss from the material providing helpful knowledge to further strengthen the understanding of the electrochemical activity of the cathodes. Several imaging modes, including high/low angle annular dark field (H/LAADF) and annular bright field (ABF), in conjunction with EELS/EDX, were used extensively for the analysis. Various parameters such as TM valence, phase transition, oxygen deficiency, and multivalent ion intercalation will be discussed.

Lattice resolution of vibrational modes in the electron microscope

The combination of aberration correction and ultra high energy resolution with monochromators has made it possible to record images showing lattice resolution in phonon modes, both with a displaced collection aperture and more recently with an on –axis collection aperture. In practice the objective aperture has to include Bragg reflections that correspond to the observed lattice image spacings, and the specimen has to be sufficiently thick for adequate phonon scattered intensity. There has been controversy as to whether the images with the on axis detector are really a consequence of lattice resolution in a phonon mode or just a transfer of information from an image that was formed by elastically scattered electrons. We present results of calculations based on a theory that includes the possibility of dynamical electron diffraction for both incident and scattered electrons and the full phonon dispersion relation. We show that Umklapp scattering from the second Brillouin Zone back to the first Brillouin Zone is necessary for lattice resolution with the on axis detector and that it is therefore reasonable to attribute the lattice resolution to the phonon scattering.

Development of a multi-detector readout circuitry for ultrahigh energy resolution single-photon imaging applications

In this paper, we present the design and preliminary performance evaluation of a novel external multi-channel readout circuitry for small-pixel room-temperature semiconductor detectors, namely CdZnTe (CZT) and CdTe, that provide an excellent intrinsic spatial (250 and 500μm pixel size) and an ultrahigh energy resolution (∼1% at 122 keV) for X-ray and gamma-ray imaging applications. An analog front-end printed circuit board (PCB) was designed and developed for data digitization, data transfer and ASIC control of pixelated CZT or CdTe detectors. Each detector unit is 2 cm × 2 cm in size and 1 or 2 mm in thickness, being bump-bonded onto a HEXITEC ASIC, and wire-bonded to a readout detector module PCB. The detectors’ front-end is then connected, through flexible cables of up to 10 m in length, to a remote data acquisition system that interfaces with a PC through USB3.0 connection.We present the design and performance of a prototype multi-channel readout system that can read out up to 24 detector modules synchronously. Our experimental results demonstrated that the readout circuitry offers an ultrahigh spectral resolution (0.8 keV at 60 keV and 1.05 keV at 122 keV) with the Cd(Zn)Te/HEXITEC ASIC modules tested. This architecture was designed to allow easy expansion to accommodate a larger number of detector modules, and the flexibility of arranging the detector modules in a large and deformable detector array without degrading the excellent energy resolution.

Ultra-high Energy Resolution EELS

Ultra-high Energy Resolution EELS

Simulations of Electron Flux Oscillations as Observed by MagEIS in Response to Broadband ULF Waves

AbstractCoherent electron flux oscillations of hundreds of keV are often observed by the Van Allen Probes in the magnetosphere during quiet times in association with ultralow frequency (ULF) waves. They are observed in the form of periodic flux fluctuations, with a drift frequency that is energy dependent, but are not associated with drift echoes following storm‐ or substorm‐related energetic particle injections. Instead, they are associated with the resonant interaction of electrons with ULF waves and are an indication of ongoing electron radial diffusion. To investigate details of such flux oscillations, particle‐tracing simulations are conducted under the effect of realistic, broadband ULF electric and consistent magnetic fluctuations. Virtual detectors are simulated along spacecraft orbits and the results are compared to measurements. Through a parametric study, it is found that the width of electron energy channels is a critical parameter affecting the observed amplitude of flux oscillations, with narrower energy channel widths enabling the observation of higher‐amplitude flux oscillations; this potentially explains why such features were not observed regularly before the Van Allen Probes era, as previous spacecraft generally had lower energy resolution, which only enabled the observation of large‐amplitude drift echoes following a storm or substorm. Results are confirmed using the Magnetic Electron Ion Spectrometer (MagEIS) ultrahigh energy resolution data. Energy width effects are quantified through a parametric simulation study that matches flux oscillation observations during a period that is characterized by extremely quiet conditions, where the Van Allen Probes observed flux oscillations over multiple days.