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At least 289 records · Page 16

Revealing the Electrochemical Kinetics of Electrolytes in Nanosized LiFePO 4 Electrodes

Lithium-ion battery rate performance is ultimately limited by the electrolyte, yet the behaviors of electrolytes during high-rate (dis)charge remain elusive to electrochemical measurement. Herein, we develop and study a nanosized LiFePO 4 model system in which the electrolyte completely controls the electrochemical kinetics of the porous electrode. Impedance spectroscopy, cyclic voltammetry, and rate performance testing prove that ion transport in the electrolyte is the sole rate-limiting process, even in thin electrodes. A novel pseudo-steady-state extrapolation (S3E) method for Tafel analysis shows that LiFePO 4 obeys Butler-Volmer kinetics with a transfer coefficient of 3. The combination of these unexpectedly rapid interfacial kinetics and an activation barrier for phase transformation causes extreme reaction heterogeneity, which manifests as a moving reaction zone. Resistance versus capacity analysis enables direct measurement of electrolyte resistance growth during high-rate (dis)charge, revealing how the interaction between concentration polarization and a moving reaction zone controls electrolyte rate performance in LiFePO 4 electrodes. This work elucidates the profound impacts of the electrolyte on electrochemical measurements in porous battery electrodes: when the active material is not rate limiting, it is impossible to directly measure the intrinsic kinetics of the active material, but conversely, it becomes possible to directly measure the kinetics of the electrolyte.

Electrochemistry↗

High-Power Lithium Metal Batteries Enabled by High-Concentration Acetonitrile-Based Electrolytes with Vinylene Carbonate Additive

To enable next-generation high power, high-energy-density lithium (Li) metal batteries (LMBs), an electrolyte possessing both high Li Coulombic efficiency (CE) at high-rate and good anodic stability on cathodes is critical. Acetonitrile (AN) is a well-known organic solvent for high anodic stability and high ionic conductivity, yet its application in LMBs is limited due to its poor compatibility with Li metal anode even at high salt concentration conditions. Here, we developed a highly concentrated AN-based electrolyte with vinylene carbonate (VC) additive to suppress Li+ depletion at high current densities. Addition of VC in the AN-based electrolyte leads to the formation of a polycarbonate-based solid electrolyte interphase which minimizes Li corrosion and leads to very high Li CE of up to 99.1% at a current density of 0.2 mA cm-2. Using such an electrolyte, fast charging of Li||NMC333 cells has been realized at a high current density of 3.6 mA cm-2, and stable cycling of Li||NMC622 cells with a high cathode loading of 4 mAh cm-2 has also been demonstrated.

Peng, Zhe↗

High strain rate deformation of aged TRIP Ti-10V-2Fe-3Al (wt.%) examined by in-situ synchrotron X-ray diffraction

Transformation Induced Plasticity (TRIP) is a promising avenue for tailoring the work hardening response of metastable $β$ titanium (Ti) alloys. Here we show that aged TRIP Ti-10V-2Fe-3Al (wt.%) maintains higher elongations and flow stresses as strain rate increases, if phase stability and microstructural characteristics are tuned. Low temperature aging influences the matrix $β$ phase stability by $ω$ phase precipitation, which affords a promising way to impact the TRIP effect and obtain desirable mechanical properties, ranging from high damping capacity to good strength/ductility combinations. Although TRIP is active during quasi-static and dynamic testing up to 2000 s –1 , increasing aging time and/or strain rate reduces the overall propensity for the TRIP effect and extent of transformation, which occurs rapidly just at the onset of yielding. Importantly, TRIP with $ω$ phase precipitation provides interesting alloying, microstructure, and property design strategies for engineering applications like lightweight protective structures, where high strains and the need for energy absorption are encountered.

36 MATERIALS SCIENCE↗

High Dose Rate Irradiations of Enduray Vision System for Nuclear Inspections

Higher radiation-hardened video cameras are needed in the operation and remote handling of equipment in nuclear reactor inspection and refueling applications. Vega Wave Systems, Inc. has developed a radiation-hardened vision system for nuclear energy applications. This vision system has been developed under several small business innovative research programs (SBIRs) from the U.S. Department of Energy, and the previous GAIN voucher program at Argonne National Laboratory (ANL) was successful in demonstrating that a prototype of the camera is radiation-hard up to at least 525 kGy (5.25 × 106 rad, Si equivalent) at dose rates of 10 kGy/hr with no measurable degradation in image quality and no measurable radiation-induced noise (RIN). Vega Wave Systems has developed a new version of the camera with more than 3X the resolution using a new design and new components, and this new design requires radiation-hardness qualification for marketplace acceptance. The program described in this report provided high radiation-hardness testing of this redesigned high-resolution vision system using the Argonne Low-Energy Accelerator Facility (LEAF). This report presents the results of irradiation tests performed on Vega Wave System’s redesigned high resolution vision system at a dose rate of 9.3 kGy/hr and up to total doses of 1823 kGy. This was an accumulation of 197 hours of irradiation. The results were excellent, providing proof of the redesigned high-resolution vision system’s immunity to high levels of radiation.

42 ENGINEERING↗

Intelligent experiments through real-time AI: Fast Data Processing and Autonomous Detector Control for sPHENIX and future EIC detectors

This R&D project, initiated by the DOE Nuclear Physics AI-Machine Learning initiative in 2022, leverages AI to address data processing challenges in high-energy nuclear experiments (RHIC, LHC, and future EIC). Our focus is on developing a demonstrator for real-time processing of high-rate data streams from sPHENIX experiment tracking detectors. The limitations of a 15 kHz maximum trigger rate imposed by the calorimeters can be negated by intelligent use of streaming technology in the tracking system. The approach efficiently identifies low momentum rare heavy flavor events in high-rate p+p collisions (3MHz), using Graph Neural Network (GNN) and High Level Synthesis for Machine Learning (hls4ml). Success at sPHENIX promises immediate benefits, minimizing resources and accelerating the heavy-flavor measurements. The approach is transferable to other fields. For the EIC, we develop a DIS-electron tagger using Artificial Intelligence - Machine Learning (AI-ML) algorithms for real-time identification, showcasing the transformative potential of AI and FPGA technologies in high-energy nuclear and particle experiments real-time data processing pipelines.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Microstructure effects on high velocity microparticle impacts of copper

Constitutive models can fail to predict high-rate deformation behavior due to their inability to account for microstructural effects. In part, this is because of a dearth of experimental benchmarking data in the high strain-rate, low pressure regime, since many high-rate experiments also probe a region of strong shockwaves, at which point microstructure effects no longer play a primary role. This work uses laser-induced particle impact testing to quantitatively study high velocity impacts of small, rigid alumina microspheres on flat copper substrates with varying amounts of initial cold work in the weak shock regime, but at very high strain rates up to ~10 7 s –1 . Through paired experiments and numerical simulations, this work shows that the initial microstructure condition can have significant influence on dynamical mechanical properties in this range. Specifically, prior work hardening of the copper substrate leads to increased rebounding of the microparticles (i.e., less plastic dissipation in the impact) as well as smaller craters. Each of these experimental measurables can be converted into a strength measure, i.e., the dynamic yield strength or dynamic hardness, respectively, neither of which is well predicted consistently by existing constitutive laws. The general trend of hardening can be captured by such models by incorporating an existing “pre-strain,” suggesting that future calibration of the materials parameters may yield a good fit over a broader range of conditions. Our results emphasize the importance of reporting the microstructural condition in dynamic studies, as well as the necessity of accounting for these factors when formulating and optimizing constitutive models.

36 MATERIALS SCIENCE↗

A high-power, high-repetition-rate THz source for pump–probe experiments at Linac Coherent Light Source II

Experiments using a THz pump and an X-ray probe at an X-ray free-electron laser (XFEL) facility like the Linac Coherent Light Source II (LCLS II) require frequency-tunable (3 to 20 THz), narrow bandwidth (~10%), carrier-envelope-phase-stable THz pulses that produce high fields (>1 MV cm –1 ) at the repetition rate of the X-rays and are well synchronized with them. Herein, a two-bunch scheme to generate THz radiation at LCLS II is studied: the first bunch produces THz radiation in an electromagnet wiggler immediately following the LCLS II undulator that produces X-rays from the second bunch. The initial time delay between the two bunches is optimized to compensate for the path difference in THz transport. The two-bunch beam dynamics, the THz wiggler and radiation are described, as well as the transport system bringing the THz pulses from the wiggler to the experimental hall.

42 ENGINEERING↗

A layered Prussian blue analogue as fast-charging negative electrode material for lithium-ion batteries

The simultaneous achievement of fast-charging and high specific capacity remains a critical challenge for lithium-ion battery negative electrodes. Here we report a layered manganese-based Prussian blue analogue, synthesized through vacancy control and subsequent thermal transformation. As a conversion-type negative electrode, this material exhibits high-rate performance, delivering a specific capacity of 510 mAh g −1 at a specific current of 8 A g −1 , and operates at a moderate average voltage of approximately 1.2 V vs. Li/Li + , which mitigates lithium plating risks. This high-rate capability stems from the analogue’s specific linkage configurations, which facilitate a high content of active transition metal and strong Li+ adsorption at nitrogen sites. The high transition metal content enables a high reversible capacity, while strong Li + adsorption promotes an efficient initial crystalline-to-amorphous transformation. This process induces dynamically reversible component migration during subsequent cycling, thereby enhancing conversion reaction kinetics. Our findings provide insights into the application of Prussian blue analogues as fast-charging negative electrode materials. The development of fast-charging and high-capacity negative electrodes is critical for advanced lithium-ion batteries. Here, authors use a vacancy engineering strategy to develop a layered Prussian blue analogue with competitive rate capability, delivering a specific capacity of 510 mAh g −1 at a specific current of 8 A g −1 .

25 ENERGY STORAGE↗

Integration of multiple coinflip devices for high-quality random sampling

Artificial intelligence, scientific computing, and probabilistic computing use random sampling to approximate solutions to various problems, with larger models requiring a substantial quantity of random numbers. To generate the required vast quantity of random numbers at high rates, we explore so-called “coinflip” devices, which are stochastic microelectronic devices ideally capable of independently generating random bits with a tunable weight at a high rate. However, coinflip devices are inherently analog and demonstrate nonidealities, like temperature dependence and drift, that can introduce determinism into the outputs. We present important considerations for building systems of multiple coinflip devices to produce high-quality bitstreams with low error and little dependency on previous bits. Using tunnel diodes as coinflip devices, we implement a control loop to adapt to temperature dependence and generate fair bitstreams with each device. While this can lead to dependencies between bits in a single bitstream, we demonstrate that combining results generated in parallel with individual tunnel diodes can produce fair and unpredictable bitstreams. The suitability of these bitstreams for use in probabilistic computing is then demonstrated through a Monte Carlo approximation of π.

Taylor, Brady Garland [Sandia National Laboratorie↗

Metallicity, Atomic Disorder, and Li-Ion Storage in Fast-Charging Anodes

Oxides of Nb with Wadsley-Roth shear structures comprise a family of stable, high-rate anode materials for Li-ion batteries. A particular pair of them offers the unusual opportunity to test how important metallic conduction of the starting electrode is for electrode performance. The selected pair of compounds with similar 4 × 3 Wadsley-Roth block structures are insulating Ti 2 Nb 10 O 29 and metallic Nb 12 O 29 . A combination of diffraction, electrochemistry, magnetic measurements, and entropic potential measurements is employed to establish key findings for these two anode materials. We find that starting with a metallic oxide is not especially advantageous over a comparable material that readily transitions into a metallic state upon lithiation. Second, the rate performance appears to be dictated by ion mobility, and atomic Ti/Nb disorder in Ti 2 Nb 10 O 29 contributes to improved capacity retention at high rates by suppressing Li-ion ordering. However, subtle details in the nature of redox processes make Nb 12 O 29 a slightly better electrode material for long-term cycling at slower rates.

crystal structure↗

A novel method may reveal bulk metallic glass compressive ductility trends in high data rate nanoindentation

Recent methods allow novel amorphous alloy compositions to be rapidly manufactured at small scale; however, obtaining materials properties such as compressive ductility from these smaller specimens has remained a challenge. Here, we suggest a potential high-throughput nanoindentation method that may be able to rapidly characterize the relative compressive ductility between these alloys based on their serration characteristics. The properties of emergent serrations, when interpreted in a simple micromechanical stress relaxation model, may order these materials by their compressive plastic strain to failure. These results are consistent with the ordering obtained from compressed specimens as well as with model simulations, suggesting that this model may be broadly useful for interpreting compressive ductility from nanoindentation serrations. After it is validated on more materials, this new method will match the rapid pace of amorphous alloy development, thus allowing metallic glass properties to be fine-tuned for each application prior to scale prototyping.

36 MATERIALS SCIENCE↗

Miniature Beryllium Split-Hopkinson Pressure Bars for Extending the Range of Achievable Strain-Rates

Conventional Split Hopkinson Pressure Bars (SHPB) or “Kolsky” bars are often used for determining the high-rate compressive yield and failure strength of materials. However, for experiments generating very high strain-rates (>10 3 /s) miniaturization of the setup is often required for minimizing the effects of elastic wave dispersion in order to enable the inference of decreasingly short loading events from the data. Miniature aluminum and steel bars are often sufficient for meeting these requirements. However, for high enough strain-rates, miniaturization of steel or aluminum Kolsky bars may require prohibitively small diameter bars and test specimens that could become inappropriate for inferring representative properties of materials with large grain size relative to the test specimen size. The use of a beryllium Kolsky bar setup is expected to enable high rates to be accessible with larger diameter bars/specimen combinations due to the inherent physical properties of beryllium, which are expected to minimize the effects of elastic wave dispersion. For this reason, a series of beryllium Kolsky bars have been developed, and, in this paper, the dispersion characteristics of these bars are measured and compare the data with those of similarly sized 7075-T6 aluminum and C350 maraging steel. The results, which agree well with the theory, show no appreciable frequency dependence of the elastic wavespeed in the data from the beryllium bars, demonstrating its advantage over aluminum and steel in application to Kolsky bars.

36 MATERIALS SCIENCE↗

Search for a Narrow Resonance Lighter than 200 GeV Decaying to a Pair of Muons in Proton-Proton Collisions at $\sqrt{s} =$ TeV

A search is presented for a narrow resonance decaying to a pair of oppositely charged muons using s=13 TeV proton-proton collision data recorded at the LHC. In the 45–75 and 110–200 GeV resonance mass ranges, the search is based on conventional triggering and event reconstruction techniques. In the 11.5–45 GeV mass range, the search uses data collected with dimuon triggers with low transverse momentum thresholds, recorded at high rate by storing a reduced amount of trigger-level information. The data correspond to integrated luminosities of 137 and 96.6 fb-1 for conventional and high-rate triggering, respectively. No significant resonant peaks are observed in the probed mass ranges. The search sets the most stringent constraints to date on a dark photon in the ∼30–75 and 110–200 GeV mass ranges.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

High Data Rate Detector for Neutron Reflectometer

Neutron reflectometers are a class of instruments that employ neutron diffraction for measuring the structure of thin films. The technique provides valuable information over a wide variety of scientific and technological applications including chemical aggregation, polymer and surfactant adsorption, structure of thin film magnetic systems, biological membranes, etc. Such instruments are considered to be one of the most important in the neutron science field. Newer facilities place growing demands on the count rate capability of the specialized neutron detectors required. Proportional Technologies completed the Phase I effort successfully with a fully operational prototype detector built at PTI and tested at the CG1A neutron beam of the High Flux Isotope Reactor (HFIR, Oak Ridge, TN). The prototype incorporated 3 panels of 14 copper-walled cells each (total of 42 cells), each lined with 1.3 μm of 10B4C. The detector was tested for efficiency, spatial resolution, count rate linearity, uniformity, overlap and scatter. Testing revealed stable operation, uniform response across cells, and successful resolution of individual cells. The maximum count rate tested in the 3 panels combined was 590 kHz, limited by a deadtime of about 1 μs in the digital electronics. The local rate measured in a single cell showed no deadtime losses up to 810 cps/mm2, indicating that a rate of 20 Mhz can be supported in the 308-cell detector planned for Phase II.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Towards a numu CC exclusive cross section measurement with one proton and one muon in the final state at the NOvA near detector

NOvA is a long-baseline neutrino experiment at Fermilab that studies neutrino oscillations via electron neutrino appearance and muon neutrino disappearance. The NOvA Near Detector, located 1 km from the NuMI target, records a high rate of neutrino interactions in the energy range of 1-5 GeV. One of the limitations in precise extraction of oscillations is the large systematic uncertainty on neutrino-nucleus interactions. The high rate of neutrino interactions in the NOvA Near Detector provides the opportunity to probe various neutrino interaction processes and nuclear models, via the extraction of cross sections of particular final states. Nuclear models can be improved by measuring neutrino-nucleus cross sections with respect to kinematic variables which are known to be more sensitive to nuclear effects, such as transverse kinematic imbalance (TKI) variables. Usage of TKI variables allows for more direct constraints on models of neutrino scattering, as these variables can more directly investigate, for instance, effects of Fermi motion and final state interactions. In this work, we describe progress towards a method of identifying and reconstructing protons in the NOvA near detector to enable the cross section measurement of charged current neutrino interactions with a visible muon and a proton in the final state, reported in TKI variables.

Weber, Colin [Minnesota U.] (ORCID:000000031117067↗

EdgeAI: Machine learning via direct attached accelerator for streaming data processing at high shot rate x-ray free-electron lasers

We present a case for low batch-size inference with the potential for adaptive training of a lean encoder model. We do so in the context of a paradigmatic example of machine learning as applied in data acquisition at high data velocity scientific user facilities such as the Linac Coherent Light Source-II x-ray Free-Electron Laser. We discuss how a low-latency inference model operating at the data acquisition edge can capitalize on the naturally stochastic nature of such sources. We simulate the method of attosecond angular streaking to produce representative results whereby simulated input data reproduce high-resolution ground truth probability distributions. By minimizing the mean-squared error between the decoded output of the latent representation and the ground truth distributions, we ensure that the encoding layers and resulting latent representation maintains full fidelity for any downstream task, be it classification or regression. We present throughput results for data-parallel inference of various batch sizes, some with throughput exceeding 100 k images per second. We also show in situ training below 10 s per epoch for the full encoder–decoder model as would be relevant for streaming and adaptive real-time data production at our nation’s scientific light sources.

97 MATHEMATICS AND COMPUTING↗