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At least 235 records · Page 13

Revealing the aging process of solid electrolyte interphase on SiOx anode

Abstract As one of the most promising alternatives to graphite negative electrodes, silicon oxide (SiO x ) has been hindered by its fast capacity fading. Solid electrolyte interphase (SEI) aging on silicon SiO x has been recognized as the most critical yet least understood facet. Herein, leveraging 3D focused ion beam-scanning electron microscopy (FIB-SEM) tomographic imaging, we reveal an exceptionally characteristic SEI microstructure with an incompact inner region and a dense outer region, which overturns the prevailing belief that SEIs are homogeneous structure and reveals the SEI evolution process. Through combining nanoprobe and electron energy loss spectroscopy (EELS), it is also discovered that the electronic conductivity of thick SEI relies on the percolation network within composed of conductive agents (e.g., carbon black particles), which are embedded into the SEI upon its growth. Therefore, the free growth of SEI will gradually attenuate this electron percolation network, thereby causing capacity decay of SiO x . Based on these findings, a proof-of-concept strategy is adopted to mechanically restrict the SEI growth via applying a confining layer on top of the electrode. Through shedding light on the fundamental understanding of SEI aging for SiO x anodes, this work could potentially inspire viable improving strategies in the future.

25 ENERGY STORAGE↗

Carrier-specific dynamics in 2H-MoTe2 observed by femtosecond soft x-ray absorption spectroscopy using an x-ray free-electron laser

Femtosecond carrier dynamics in layered 2H-MoTe2 semiconductor crystals have been investigated using soft x-ray transient absorption spectroscopy at the x-ray free-electron laser (XFEL) of the Pohang Accelerator Laboratory. Following above-bandgap optical excitation of 2H-MoTe2, the photoexcited hole distribution is directly probed via short-lived transitions from the Te 3d5/2 core level (M5-edge, 572–577 eV) to transiently unoccupied states in the valence band. The optically excited electrons are separately probed via the reduced absorption probability at the Te M5-edge involving partially occupied states of the conduction band. A 400 ± 110 fs delay is observed between this transient electron signal near the conduction band minimum compared to higher-lying states within the conduction band, which we assign to hot electron relaxation. Additionally, the transient absorption signals below and above the Te M5 edge, assigned to photoexcited holes and electrons, respectively, are observed to decay concomitantly on a 1–2 ps timescale, which is interpreted as electron–hole recombination. The present work provides a benchmark for applications of XFELs for soft x-ray absorption studies of carrier-specific dynamics in semiconductors, and future opportunities enabled by this method are discussed.

2D materials↗

The Dynamics of Ultrasonically Levitated Drops in an Electric Field

Ultrasonic and electrostatic levitation techniques have allowed the experimental investigation of the nonlinear oscillatory dynamics of free droplets with diameter between 0.1 and 0.4 cm. The measurement of the resonance frequencies of the first three normal modes of large amplitude shape oscillations in an electric field of varying magnitude has been carried out with and without surface charges for weakly conducting liquids in air. These oscillations of nonspherical levitated drops have been driven by either modulating the ultrasonic field or by using a time-varying electric field, and the free decay from the oscillatory state has been recorded. A decrease in the resonance frequency of the driven fundamental quadrupole mode has been measured for increasing oblate deformation in the absence of an electric field. Similarly, a decrease in this frequency has also been found for increasing DC electric field magnitude. A soft nonlinearity exists in the amplitude dependence of the resonant mode frequencies for freely decaying as well as ultrasonically and electrically driven uncharged drops. This decrease in resonance frequency is accentuated by the presence of free surface charge on the drop. Subharmonic resonance excitation has been observed for drops in a time-varying electric field, and hysteresis exists for resonant modes driven to large amplitude. Mode coupling from lower-order resonances to higher-order modes has been found to be very weak, even for fairly large amplitude shape oscillations. Most of these results are in general agreement with predictions from recent analytical and numerical investigations.

Trinh, E. H.↗

The Dynamics of Ultrasonically Levitated Drops in an Electric Field

Ultrasonic and electrostatic leviation techniques have allowed the experimental investigation of the nonlinear oscillatory dynamics of free droplets with diameter between 0.1 and 0.4 cm. The measurement of the resonance frequencies of the first three normal modes of large amplitude shape oscillations in an electric field of varying magnitude has been carried out with and without surface charges for weakly conducting liquids in air. These oscillations of nonspherical levitated drops have been driven by either modulating the ultrasonic field or by using a time-varying electric field, and the free decay from the oscillatory state has been recorded. A decrease in the resonance frequency of the driven fundamental quadrupole mode has been measured for increasing oblate deformation in the absence of an electric field. Similarly, a decrease in this frequency has also been found for increasing DC electric field magnitude. A soft nonlinearity exists in the amplitude dependence of the resonant mode frequencies for freely decaying as well as ultrasonically and electrically driven uncharged drops. This decrease in resonance frequency is accentuated by the presence of free surface charge on the drop. Subharmonic resonance excitation has been observed for drops in a time-varying electric field, and hysteresis exists for resonant modes driven to large amplitude. Mode coupling from lower-order resonances to higher-order modes has been found to be very weak, even for fairly large amplitude shape oscillations. Most of these results are in general agreement with predictions from recent analytical and numerical investigations.

Ultrasonically↗

Modeling Molten Salt Spreading and Heat Transfer using MELTSPREAD – An Uncertainty Analysis

This report summarizes spreading and heat transfer results for molten salt pouring onto a flat stainless steel substrate that were calculated using MELTSPREAD to gain insight into bulk salt behavior during a molten salt spill accident. MELTSPREAD was developed at Argonne to model the one-dimensional flow and freezing behavior of molten corium and is being applied to model molten salts for the first time as part of this work. An uncertainty analysis of thermophysical properties and spill conditions was performed using MELTSPREAD to determine which properties and conditions have the greatest impact on model outcome. The model was run with and without the inclusion of decay heat. Eutectic FLiNaK was used as the salt composition because it is well-characterized and appropriate for model development. Small salt volumes were used for the initial model runs described in this report so that the model results can be compared to the results from ongoing experiments on molten salt spreading and heat transfer currently being conducted at Argonne at a benchtop scale. The spreading of a small volume of FLiNaK (50 mL) was found to be limited by the balance between the molten salt surface tension and gravity and not by freezing for the pour conditions and assumed mechanisms of heat transfer in the model. Heat transfer from the salt was highly inefficient to due to its low thermal conductivity, high heat capacity, and high heat of fusion and varying these properties had no effect on the spreading behavior. Changing the viscosity and density of the salt slightly affected the spreading behavior. Setting the salt surface tension to approximately zero to simulate the salt wetting the substrate had the greatest effect on the spreading behavior and this increased both the spreading velocity and overall spreading area. Including decay heat in the model had a significant effect on the long-term cooling behavior of the salt but had no effect on the overall spreading behavior. Future effort should involve modeling a larger volume of molten salt to represent a reactor case spill scenario because the spreading behavior of large volumes of salt may differ from the small volumes that were the focus of this document.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Radiochronometric discordance in cast uranium metal: a multi-laboratory intercomparison exercise

Here, the model age of a nuclear material is crucial in nuclear forensic analysis. Uranium metals with complex production histories often exhibit discordant model ages from the 230 Th– 234 U and 231 Pa– 235 U chronometers. Recent studies involving targeted uranium metal castings have enhanced our understanding of decay product behavior during casting, aiding nuclear forensic interpretation. Building on this prior work, forensics laboratories at Atomic Weapons Establishment (AWE), Lawrence Livermore National Laboratory (LLNL), and Los Alamos National Laboratory (LANL) conducted an interlaboratory comparison to investigate spatial heterogeneity in uranium metal cast under controlled conditions. Each laboratory measured samples of a mixed feedstock and its corresponding cast product. This work furthers our understanding of discordant model ages and the use of discordance as a signature to enhance confidence in interpretations of radiochronometric data for nuclear forensics.

230Th/234U↗

Quantitative Specifications to Avoid Degradation during E-Beam and Induced Current Microscopy of Halide Perovskite Devices

Degradation due to electron beam exposure has posed a challenge in the use of electron microscopy to probe halide perovskite materials and devices. Herein, the interaction between the electron beam and the perovskite across acceleration voltages and at low probe currents is investigated in a scanning electron microscope (SEM) by monitoring the electron-beaminduced current (EBIC) response in perovskite solar cells in a planview configuration. SEM probe conditions are identified where dozens of repeated scans over a single region of the perovskite solar cell induce minimal electronic degradation. Overall, the induced current response of the perovskite device is found to strongly depend upon the beam condition: rapid decay occurs at high beam powers, the current activates at the lowest beam powers, and a newfound quasi-steady response is revealed at intermediate beam conditions. A quantitative window for the successful conduction of e-beam studies with minimal electronic degradation is revealed by evaluating induced current response over a wide range of perovskite devices, which invites broader use of SEM-based characterization techniques, including EBIC, as powerful techniques for correlative microscopy investigations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Coupling of Klein-Andreev resonant states in B⁢i 2 ⁢S⁢r 2 ⁢CaC⁢u 2 ⁢O 8+𝑥 -graphene-B⁢i 2⁢ S⁢r 2 ⁢CaC⁢u 2 ⁢O 8+𝑥 devices

Quantum devices require coherent coupling over macroscopic distances. Recently, resonances due to Klein tunneling and Andreev reflection states (KARS) have been observed in a naturally occurring p-n junction at the interface between B⁢i 2 ⁢S⁢r 2 ⁢CaC⁢u 2 ⁢O 8+𝑥 (BSCCO), a high−⁢𝑇 c superconductor (HTS), and graphene. The resonances appear as conductance oscillations with gating. Here, in this study, we show coupling between the KARS in BSCCO-graphene-BSCCO devices of varying separation (L). The coupling is evidenced by a power-law decay of resonance period as L increases from tens of nanometers to microns. These results demonstrate the long-distance coupling of KARS cavities in graphene-HTS junctions. The length dependence seen in experiments is supported by single-particle spectral functions which show KARS are coupled by transport modes in graphene. The strong coupling between KARS in BSCCO-graphene-BSCCO devices showcases the possibility of HTS-graphene junctions for quantum circuits and unconventional Josephson junctions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Rossi-alpha Analysis of CURIE Experiment

Critical assembly measurement and operations are crucial to the development of benchmark data to support research into criticality safety, radiation-detection development, and the overall application of nuclear technologies. Accurate nuclear data are needed for accurate predictive simulations, and validation using critical experiments is an important part of the nuclear data pipeline. The accuracy of nuclear data are improved using more robust and targeted measurements. In particular, the intermediate energy range of uranium is of great interest. LANL has successfully performed the Zeus series of experiments on the Comet assembly to investigate the intermediate energy range for HEU with various moderators. A successor to these experiments is the benchmark for the Critical Unresolved Region Integral Experiment (CURIE), designed to be sensitive to the unresolved resonance region (URR). This experiment is designed using polytetrafluoroethylene, more commonly known as Teflon, moderators. The CURIE experiment was successfully conducted at the National Criticality Experiments Research Center (NCERC). The Rossi-alpha method was used to evaluate the propensity of the CURIE configurations to sustain fission chains by estimating the prompt neutron decay constant α. This work evaluates the α at delayed critical using Rossi-alpha for different Teflon moderator thicknesses in the CURIE experiment. These results will help improve understanding of the CURIE benchmark experiments.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Extinct superheavy element in the Allende meteorite

Radiochemical neutron activation analysis of seven Allende samples for 26 trace elements were conducted. In addition, Cr and Fe were studied with the aid of instrumental neutron activation analysis. The investigation had the objective to identify the extinct superheavy element which was present in meteorites and decayed to Xe isotopes by spontaneous fission. The superheavy element was found to reside mainly in a rare mineral (probably a Fe, Ni, Cr, Al-sulfide), comprising only 0.04% of the meteorite. It is pointed out that of the nine volatile superheavy elements 111 to 119, only 115, 114, and 113 are expected to condense as sulfides in the temperature interval between 400 and 500 K corresponding to mineral formation conditions in the solar nebula.

Anders, E.↗

Evaluate Techniques for Penetrating a Shielded Enclosure Using Twisted Pair Wire

The aim of this project is to demonstrate techniques for effectively penetrating a radio shielded enclosure using Ethernet cable (CAT-6). This process requires that we measure the shielding performance by means of testing and data orchestration to collect and analyze our data to present observations with different test cases. Each test case would represent a different penetration strategy that utilizes distinctive wire coupling and characteristics (i.e. the type of bulkhead link, the twist of each CAT-6 cable, the shielding type of each CAT-6 cable, and the length of the cable). As the different cable setups are fabricated a prototype evaluation of setup is conducted to measure the signal integrity of our testing configuration. Our signal integrity is measured through the analysis of different parameters found in the prototype evaluation such as RF leakage, impedance mismatch, and decay rate. As each of these data values are effectively collected and analyzed the most effective cable setup is selected based upon its ability to penetrate the shielded enclosure. The testing data is compared in conjunction with the cost of the manufacturing of the prototype wire penetration.

St. Julian, Christopher↗

Meteor Shower Forecast Improvements from a Survey of All-Sky Network Observations

Meteoroid impacts are capable of damaging spacecraft and potentially ending missions. In order to help spacecraft programs mitigate these risks, NASA's Meteoroid Environment Office (MEO) monitors and predicts meteoroid activity. Temporal variations in near-Earth space are described by the MEO's annual meteor shower forecast, which is based on both past shower activity and model predictions. The MEO and the University of Western Ontario operate sister networks of all-sky meteor cameras. These networks have been in operation for more than 7 years and have computed more than 20,000 meteor orbits. Using these data, we conduct a survey of meteor shower activity in the "fireball" size regime using DBSCAN. For each shower detected in our survey, we compute the date of peak activity and characterize the growth and decay of the shower's activity before and after the peak. These parameters are then incorporated into the annual forecast for an improved treatment of annual activity.

Moorhead, Althea V.↗

Characterization of Naturally-Occurring Particles in the Nasa Langley 0.3-m Transonic Cryogenic Tunnel Using PTV

Naturally-occurring particles within the NASA Langley 0.3-m Transonic Cryogenic Tunnel are characterized for their aerodynamic performance using particle tracking velocimetry. Two sets of experiments were conducted to observe different behaviors of the particles. The normal shockwave emanating from the top surface of a supercritical airfoil was used to induce velocity lag in the particles, and the subsequent spatial decay of the velocity was used to estimate the effective diameter of the particles. Mean particle diameters between 1.6 and 1.9 𝝁m were measured, with sizes ranging from 0.2 to 3.5 𝝁m over the entire ensemble. The response of particles to separated flow was investigated. By operating in “high-lift” (low Mach number, high angle of attack) conditions with a semi-span airfoil, the ability of particles to detect separated flow on the upper surface of the airfoil was assessed. Transition from fully attached flow to fully separated flow was observed on the top surface of the airfoil accompanying a variation of angle of attack from 8° to 12°. Examination of velocity distributions indicates less than 10 percent of particle trajectories did not respond to the regions of separated flow. These results are promising, but further facility-specific work is needed to answer the broader question of particle tracking reliability.

Transonic↗

Characterization of Naturally-Occurring Particles in the NASA Langley 0.3-m Transonic Cryogenic Tunnel Using PTV

Naturally-occurring particles within the NASA Langley 0.3-m Transonic Cryogenic Tunnel are characterized for their aerodynamic performance using particle tracking velocimetry. Two sets of experiments were conducted to observe different behaviors of the particles. The normal shockwave emanating from the top surface of a supercritical airfoil was used to induce velocity lag in the particles, and the subsequent spatial decay of the velocity was used to estimate the effective diameter of the particles. Mean particle diameters between 1.6 and 1.9 𝝁m were measured, with sizes ranging from 0.2 to 3.5 𝝁m over the entire ensemble. The response of particles to separated flow was investigated. By operating in “high-lift” (low Mach number, high angle of attack) conditions with a semi-span airfoil, the ability of particles to detect separated flow on the upper surface of the airfoil was assessed. Transition from fully attached flow to fully separated flow was observed on the top surface of the airfoil accompanying a variation of angle of attack from 8° to 12°. Examination of velocity distributions indicates less than 10 percent of particle trajectories did not respond to the regions of separated flow. These results are promising, but further facility-specific work is needed to answer the broader question of particle tracking reliability.

Transonic↗

On the physics of a long decay X-ray event

The paper discusses the long decay X-ray event which appeared as an expanding loop system on the solar limb on 13-14 Aug. 1973 which was also observed temporally and spectrally. A one-dimensional hydrodynamic study was undertaken to investigate increasing and decreasing phases of the event; it was shown that the inferred temperature gradients along the loops during the heating phase are consistent with unrestricted dynamic and conductive flows along the magnetic field lines. It was concluded that it cannot be definitely stated that enhanced emission at the tops of the loops is due to pressure gradients along the field lines; also, the large emission measure variations in the 10 to the 5th to 10 to the 6th K plasma during the event's decline may be due to the temperature dependence of radiative decay within a multiloop configuration.

Krall, K. R.↗

Lowering the Energy Threshold of the CUORE Experiment: Benefits in the Surface Alpha Events Reconstruction

CUORE is a tonne-scale cryogenic experiment located at the Laboratori Nazionali del Gran Sasso that exploits bolometric technique to search for neutrinoless double beta decay of 130 Te. Thanks to its very low background and large mass, CUORE is also a powerful tool to study a broad class of phenomena, such as solar axions and WIMP scattering. The ability to conduct such sensitive searches crucially depends on the energy threshold, which has to be kept as low as possible. Here, we show how the trigger algorithm affects the sensitivity to low-energy phenomena and the interpretation of the energy spectrum. In particular, we focus on the impact that the trigger algorithm has on the identification of the coincidence events among different crystals and, consequently, on the reconstruction of the background.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Electron-nuclear decoupling at a spin clock transition

The ability to design quantum systems that decouple from environmental noise sources is highly desirable for development of quantum technologies with optimal coherence. The chemical tunability of electronic states in magnetic molecules combined with advanced electron spin resonance techniques provides excellent opportunities to address this problem. Indeed, so-called clock transitions have been shown to protect molecular spin qubits from magnetic noise, giving rise to significantly enhanced coherence. Here we conduct a spectroscopic and computational investigation of this physics, focusing on the role of the nuclear bath. Away from the clock transition, linear coupling to the nuclear degrees of freedom causes a modulation and decay of electronic coherence, as quantified via electron spin echo signals generated experimentally and in silico. Meanwhile, the effective hyperfine interaction vanishes at the clock transition, resulting in electron-nuclear decoupling and an absence of quantum information leakage to the nuclear bath, providing opportunities to characterize other decoherence sources.

74 ATOMIC AND MOLECULAR PHYSICS↗

A Measurement of the Eta Meson Radiative Decay Width via the Primakoff Effect

The ? meson is an interesting tool to study fundamental symmetries in Quantum Chromodynamics (QCD). In particular, its radiative decay width, ? p? Ñ ??q, is an important quantity that can be predicted in the framework of Chiral Perturbation Theory. A precision measurement of this quantity would provide critical inputs to understanding the mixing of the ? and ?1 mesons and extracting constants with wide-ranging applications in low-energy QCD. This decay width has been measured in the past using two different experimental techniques. The more popular technique utilized e`e´ collisions to produce ? mesons through electromagnetic interactions. Today, the Particle Data Group (PDG) averages the results of five such experiments to obtain their currently-accepted value of the decay width as: 0.515?0.018 keV. However the first measurement of this quantity was obtained from a fixed-target experiment that measured the cross section for photoproduction of ? mesons on a nuclear target via the Primakoff effect. Their result of 0.324?0.046 keV shows strong tension with the average of the collider measurements, motivating a new, high precision measurement using the Primakoff method. For this purpose, the PrimEx-eta experiment was conducted in Hall D of the Thomas Jefferson National Accelerator Facility (Jefferson Lab or JLab). The data is currently being analyzed to measure the differential cross section for the photoproduction of ? mesons on a liquid, 4He target. Preliminary results obtained from the analysis of the first phase of the PrimEx-eta experiment show reasonable agreement with the currently-accepted PDG value of the radiative decay width. However, as will be discussed, there are many challenges to this precision measurement which must be studied before any results can be finalized and compared with previous measurements. In parallel to the ? decay width measurement, the PrimEx-eta experiment measured the total cross section for the fundamental, Quantum Electrodynamics (QED) process of Compton scattering from the atomic electrons inside the target. The results obtained from this measurement are in strong agreement with the next-to-leading order QED calculations, and the total combined uncertainties are below 3% for incident photon energies between 7-10 GeV. In addition to providing the first precision measurement of the total Compton scattering cross section within this beam energy range, this measurement verifies the capability of the PrimEx-eta experimental setup to perform absolute cross section measurements at forward angles, and serves as a reference process for the calibration of systematic uncertainties.

Smith, Andrew↗