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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 361 records · Page 20

Modeling the contributions to acoustic nonlinearity from complex dislocation networks using 3D dislocation dynamics

Nonlinear ultrasonic parameters are highly sensitive to microstructural features that affect macroscale material behavior, providing a nondestructive means to characterize their evolution. Although dislocations are known to be a strong source of acoustic nonlinearity, establishing quantitative links between the acoustic nonlinearity parameter (β), measured via Second Harmonic Generation, and dislocation morphology—such as dislocation length and density—remains an open challenge. This work advances the numerical modeling of dislocation–β relationships using 3D dislocation dynamics (DD) simulations in two approaches: a “static” method computing strain and stress fields from dislocation configurations in the absence of external loading, and a “quasi-static” method to estimate β from the curvature of dislocation lines under applied load. First, the static method is combined with finite element analysis to investigate a recent assertion that heterogeneous initial strain fields can induce higher harmonic generation in a linear elastic medium; the present results do not corroborate this outcome. Then, the quasi-static method is applied to multiple-dislocation scenarios through parametric studies, revealing behaviors not predicted by analytical models, such as the competing interactions of edge and screw dislocations and the significant influence of applied stress on β. Finally, the simulations are used to model SHG experimental results and validate the hypothesis that β can decrease during plastic deformation, despite increasing dislocation density. As the DD code used here is open-source, it provides a practical platform for future investigation into microstructure–β relationships important to the interpretation of SHG results.

Materials science↗

In situ study of microstructure evolution and α → ω phase transition in annealed and pre-deformed Zr under hydrostatic loading

The detailed study of the effect of the initial microstructure on its evolution under hydrostatic compression before, during, and after the irreversible α → ω phase transformation and during pressure release in Zr using in situ x-ray diffraction is presented. Two samples were studied: one is plastically pre-deformed Zr with saturated hardness and the other is annealed. Phase transformation α → ω initiates at lower pressure for a pre-deformed sample but for a volume fraction of ω Zr, c > 0.7, a larger volume fraction is observed for the annealed sample. This implies that the proportionality between the athermal resistance to the transformation and the yield strength in the continuum phase transformation theory is invalid; an advanced version of the theory is outlined. Phenomenological plasticity theory under hydrostatic loading is outlined in terms of microstructural parameters, and plastic strain is estimated. During transformation, the first rule is suggested, i.e., the average domain size, microstrain, and dislocation density in ω Zr for c < 0.8 are functions of the volume fraction, c of ω Zr only, which are independent of the plastic strain tensor prior to transformation and pressure. The microstructure is not inherited during phase transformation. Surprisingly, for the annealed sample, the final dislocation density and the average microstrain after pressure release in the ω phase are larger than for the severely pre-deformed sample. The results suggest that an extended experimental basis is required for the predictive models for the combined pressure-induced phase transformations and microstructure evolutions.

36 MATERIALS SCIENCE↗

Minimization of Cathode|Solid-Electrolyte Interfacial Delamination through the Application of Interphase Layers

Next-generation lithium-ion batteries are expected to use solid electrolytes (SEs) to enable higher energy density and extreme fast-charge capabilities. One major mode of degradation at the cathode|SE interface is delamination between the cathode active materials and SEs, which leads to performance decay. Experimental observations indicate that implementation of interphase layers can minimize the cathode|SE delamination induced capacity fade. A multiscale computational methodology is developed here to investigate the applicability of boron substituted lithium carbonate (Li 2+x B x C 1–x O 3 , x = 0.5, or LBCO) to minimize the delamination at the cathode|SE interface. Atomistic simulations indicate that the fracture energies at both the cathode|LBCO and LBCO|SE interfaces are higher than those at the cathode|SE interface, which reduces the extent of delamination. Mesoscale simulations indicate that, apart from increasing the fracture energy, decreasing the evolution of strain energy by lowering the elastic modulus of the interphase layer can also minimize the extent of delamination at the cathode|SE interface. However, the adoption of an interphase layer with high ionic conductivity is necessary to minimize the ohmic losses during operation at higher current densities. This study provides guidance on selecting interphase layers with specific properties and thicknesses to minimize both interfacial delamination and impedance growth.

LBCO↗

Understanding of Ag Nanocatalysts for Electrocatalytic CO2 Conversion: Effects of Particle Size and Carbon Support

In this talk, we combined ultrahigh vacuum (UHV) surface science techniques, electrochemical measurements, and computational modeling to investigate Ag based electrocatalysts for CO2 reduction reaction (CO2RR). Our goal is to understand the critical characteristics governing the activity and selectivity of Ag electrocatalysts. Ag electrocatalysts were grown on highly oriented pyrolytic graphite (HOPG) in the UHV chamber, characterized with X-ray photoelectron spectroscopy (XPS) and scanning tunneling microscopy (STM), and then tested in a custom-built gastight H-cell. Supported by computational modeling based on density functional theory (DFT) calculations and microkinetic modeling (MKM), our studies revealed a strong size-dependent electrocatalytic CO2-to-CO conversion of the Ag nanoparticle electrocatalysts with average particle diameter between 2 to 6 nm. Smaller diameter (< 3 nm) particles favored H2 evolution reaction (HER) due to a high population of Ag edge sites, whereas larger diameter particles favored CO2RR as the population of Ag(100) surface sites grew. We further discovered that electronic interactions between small diameter Ag particles and highly defective carbon supports could break the size-dependent CO2RR reactivity, resulting in highly selective (CO Faradaic Efficiency > 90%) and active Ag nanoparticle electrocatalysts with sizes < 2 nm diameter. This knowledge is key to understand electrocatalysts performance and to ultimately guide electrocatalyst design

Ag nanoparticles↗

Single-Shot Diagnosis of Electron Energy Evolution via Streaked Betatron X Rays in a Curved Laser Wakefield Accelerator

We report on an experimental observation of the streaking of betatron x rays in a curved laser wakefield accelerator. The streaking of the betatron x rays was realized by launching a laser pulse into a plasma with a transverse density gradient. By controlling the plasma density and the density gradient, we realized the steering of the laser driver, electron beam, and betatron x rays simultaneously. Furthermore, we observed an energy-angle correlation of the streaked betatron x rays and utilized it in diagnosing the electron acceleration process in a single-shot mode. Our work could also find applications in advanced control of laser beam and particle propagation. More importantly, the angular streaked betatron x ray has an intrinsic spatiotemporal correlation, which makes it a promising tool for single-shot pump-probe applications.

43 PARTICLE ACCELERATORS↗

Chemical state of nickel nanoparticles during the oxygen evolution reaction in a carbonate-bicarbonate buffer solution

The chemical state of nickel anodes during the oxygen evolution reaction can impact their electrocatalytic performance. Here, X-ray photoelectron and absorption spectroscopies reveal the chemical state of nickel nanoparticles under oxygen evolution reaction conditions in amildly alkaline carbonate-bicarbonate buffer solution. Ni 2+ and Ni 3+ species are observed at the reaction onset potential with a 7:4 ratio, with no remaining metallic nickel. These species include NiO, which increasingly converts to other Ni 2+ and Ni 3+ species once the potential is increased above the onset potential. Conversely, when a 20-nm-thick nickel film is used instead of nickel nanoparticles, a significant amount of metallic nickel remains in the inner layers. Nickel nanoparticles also undergo significant morphological and structural changes during the reaction, as evidenced by ex situ transmission electron microscopy. Amorphization of the nanoparticles is attributed to significant H 2 O incorporation, with the oxygen intensity increasing both in operando and ex situ measurements.

36 MATERIALS SCIENCE↗

Formation and Detriments of Residual Alkaline Compounds on High-Nickel Layered Oxide Cathodes

High-nickel layered oxides LiNi x M 1-x O 2 (x ≥ 0.9) have emerged as promising cathode materials for automotive batteries due to their high energy density and lower cost. However, the formation and accumulation of surface alkaline compounds during storage hinder their mass production and commercialization. Here, in this study, a validated chemical method is employed to deconvolute and quantify the evolution of each residual lithium compound in four representative cathodes during ambient-air storage, viz., LiNiO 2 (LNO), LiNi 0.95 Co 0.05 O 2 (NC), LiNi 0.95 Mn 0.05 O 2 (NM), and LiNi 0.95 Al 0.05 O 2 (NA). Furthermore, the activation energy of the reaction between water and the cathode is determined by measuring the leached LiOH concentration at various temperatures. While residual lithium and time-of-flight secondary-ion mass spectrometry measurements collectively reveal that the air stability overall follows the trend of NM > NA ≈ NC > LNO, the aged NM exhibits the highest charge-transfer resistance and the worst electrochemical performance among the cathodes. In situ, X-ray diffraction and scanning transmission electron microscopy unveil that the aged NM is plagued by a large area of resistive spinel-like M 3–x Li x O 4 phases, leading to aggravated particle reaction heterogeneity. Finally, a one-step recalcination method is demonstrated effective in fully restoring the degraded cathodes. This work provides insights into overcoming air sensitivity issues of high-Ni cathodes.

(S)TEM↗

Amphiphilic Baskets for Supramolecular Nanoarchitectures at Interfaces: Inverted Monolayer Formation on Water

Interfacial chemistry of molecular baskets remains poorly understood despite their promise for supramolecular applications of detection and sequestration of toxic molecules including those of illicit drugs, organophosphorus compounds, and anticancer agents. We present a fundamental investigation of the interfacial behavior of three amphiphilic supramolecular baskets (ASB 4, 8, and 12), having increasingly longer yet linear alkyl chains at the top of their bowl-shaped cavity. The studies were completed at the air−water interface to elucidate surface activity, interfacial stability, self-assembly, and monolayer organization that drive inverted monolayer formation, in which the molecular arms orient toward the aqueous phase in a configuration opposite to that typically observed for lipids. Herein, surface pressure−area isotherms of ASB 4, 8, 12, deposited on a water surface, were performed in tandem with nonequilibrium relaxation experiments to quantify surface activity, thermodynamic stability, and monolayer compressibility of the baskets’ monolayer assembly. Brewster angle microscopy enabled direct visualization of morphological evolution, aggregation, and packing at the interface. We show that systematic extension of the hydrocarbon arms, from four to 12 methylene groups, progressively modifies intermolecular packing, drives distinct two-dimensional aggregation pathways, and increases number densities at the air−water interface. Atomistic molecular dynamics simulations corroborate many of these experimentally observed trends and provide mechanistic detail on the cooperative roles of basket topology and interfacial concentration in regulating the hydration structure and dynamics within the cavities generated by surface-adsorbing baskets, consistent with observed variations in surface activity and packing. Our results establish how the topology of these unique supramolecules and their concentration govern interfacial organization and offer a rational framework for designing amphiphiles with predictable behavior at soft interfaces.

Hydrocarbons↗

Chromium versus Aluminum: Impact of Nickel Alloy Composition and Interfacial Kinetics on High-Temperature Passivating Oxide Formation

High-temperature corrosion resistance depends critically on the formation of a passivating surface oxide, which is highly sensitive to alloy composition and structure. Such details often elude experimental investigation, and simplified analytical models fail to provide a truly chemical view of passivating oxide evolution. Here, we explicitly compare the fundamental chemistry of Cr and Al as prototypical passivating elements in Ni alloys by directly simulating competing reaction and diffusion processes within the oxide film using kinetic Monte Carlo and density functional theory. We find that the origin and expression of passivating behavior during early-stage thermal oxidation are qualitatively different between the two alloy systems. Ni–Cr alloys feature a sudden onset of passivation associated with a sharp phase transition upon Cr enrichment that directly couples oxidation kinetics to phase transformation behavior. In contrast, Ni–Al alloys display more continuous oxide phase variation with Al enrichment, ultimately resulting in a lower composition threshold for passivation and a thinner passivating layer. In addition, we elucidate the nonobvious role of metal exchange within the alloy near the oxide boundary, which fundamentally alters film composition and passivating behavior. Furthermore, our results have key implications for engineering improved corrosion-resistant alloys, both in terms of compositional variation and processing.

Alloys↗

A Vibrational Probe of Electrical Doping in N2200 and Fermi-Level Alignment at Polymer Cathode/Metal Cocatalyst/Electrolyte Junctions

Hybrid (photo)­cathodes consisting of conjugated polymer and hydrogen evolution reaction (HER) cocatalysts are an emerging platform for low-cost solar fuel generation. Poly­{[N,N′-bis­(2-octyldodecyl)-naphthalene-1,4,5,8-bis­(dicarboximide)-2,6-diyl]-alt-5,5′-(2,2′-bithiophene)}, known as P­(NDI2OD-T2) or N2200, is a promising electron accepting material for bulk heterojunction photocathodes. Unlike inorganic (photo)­electrodes, much less is known about the energetic alignment of conjugated polymer electrode/metal/electrolyte junctions. Here, in this work, we investigate the electrical doping behavior in an N2200 cathode and its Fermi-level alignment with gold nanoparticles, which is used here as a model for the hydrogen evolution metal cocatalyst. Through UV/visible, Raman, and attenuated total-reflectance infrared spectroelectrochemistry, we observe the impact of electrical doping on the vibrational frequencies of neutral, anion, and dianion species in N2200, which suggests that electron density changes within the corresponding naphthalene-diimide (NDI) units. Upon one-electron reduction, the $C=O$ stretching frequency of the NDI anion unit (polaron) shows a red shift by ∼ 68 cm –1 . Additionally, the $C=O$ stretching frequency of neutral units in the doped N2200 shows a minor red shift of ∼ 5 cm –1 , suggesting charge transfer from neighboring polaron units. Surface-enhanced Raman spectroscopy measurements of a gold nanoparticle-functionalized N2200 electrode revealed that the Au Fermi level only shifts with that of N2200 upon polaron formation; thus, the formal potential of polymer polaron formation determines the behavior of the catalyst Fermi level, which we posit will modulate reaction capability. This mechanistic study provides a new approach for understanding the nanometer-scale energetics at the conjugated polymer/cocatalyst junction and provides critical insights for the future design of HER (photo)­cathodes.

charge transfer↗

The High Latitude Ionospheric Response to the Major May 2024 Geomagnetic Storm: A Synoptic View

Abstract The high latitude ionospheric evolution of the May 10‐11, 2024, geomagnetic storm is investigated in terms of Total Electron Content and contextualized with Incoherent Scatter Radar and ionosonde observations. Substantial plasma lifting is observed within the initial Storm Enhanced Density plume with ionospheric peak heights increasing by 150–300 km, reaching levels of up to 630 km. Scintillation is observed within the cusp during the initial expansion phase of the storm, spreading across the auroral oval thereafter. Patch transport into the polar cap produces broad regions of scintillation that are rapidly cleared from the region after a strong Interplanetary Magnetic Field reversal at 2230UT. Strong heating and composition changes result in the complete absence of the F2‐layer on the eleventh, suffocating high latitude convection from dense plasma necessary for Tongue of Ionization and patch formation, ultimately resulting in a suppression of polar cap scintillation on the eleventh.

Themens, David R.↗

A self-healing plastic ceramic electrolyte by an aprotic dynamic polymer network for lithium metal batteries

Abstract Oxide ceramic electrolytes (OCEs) have great potential for solid-state lithium metal (Li 0 ) battery applications because, in theory, their high elastic modulus provides better resistance to Li 0 dendrite growth. However, in practice, OCEs can hardly survive critical current densities higher than 1 mA/cm 2 . Key issues that contribute to the breakdown of OCEs include Li 0 penetration promoted by grain boundaries (GBs), uncontrolled side reactions at electrode-OCE interfaces, and, equally importantly, defects evolution (e.g., void growth and crack propagation) that leads to local current concentration and mechanical failure inside and on OCEs. Here, taking advantage of a dynamically crosslinked aprotic polymer with non-covalent –CH 3 ⋯CF 3 bonds, we developed a plastic ceramic electrolyte (PCE) by hybridizing the polymer framework with ionically conductive ceramics. Using in-situ synchrotron X-ray technique and Cryogenic transmission electron microscopy (Cryo-TEM), we uncover that the PCE exhibits self-healing/repairing capability through a two-step dynamic defects removal mechanism. This significantly suppresses the generation of hotspots for Li 0 penetration and chemomechanical degradations, resulting in durability beyond 2000 hours in Li 0 -Li 0 cells at 1 mA/cm 2 . Furthermore, by introducing a polyacrylate buffer layer between PCE and Li 0 -anode, long cycle life >3600 cycles was achieved when paired with a 4.2 V zero-strain cathode, all under near-zero stack pressure.

36 MATERIALS SCIENCE↗

Core performance predictions in projected SPARC first-campaign plasmas with nonlinear CGYRO

This work characterizes the core transport physics of SPARC early-campaign plasmas using the PORTALS-CGYRO framework. Empirical modeling of SPARC plasmas with L-mode confinement indicates an ample window of breakeven (Q > 1) without the need of H-mode operation. Extensive modeling of multi-channel (electron energy, ion energy, and electron particle) flux-matched conditions with the nonlinear CGYRO code for turbulent transport coupled to the macroscopic plasma evolution using PORTALS reveals that the maximum fusion performance to be attained will be highly dependent on the near-edge pressure. Stiff core transport conditions are found, particularly when fusion gain approaches unity, and predicted density peaking is found to be in line with empirical databases of particle source-free H-modes. Impurity optimization is identified as a potential avenue to increase fusion performance while enabling core-edge integration. Extensive validation of the quasilinear TGLF model builds confidence in reduced-model predictions. The implications of projecting L-mode performance to high-performance and burning-plasma devices is discussed, together with the importance of predicting edge conditions.

Rodriguez-Fernandez, P. (ORCID:0000000273611131)↗

Mg and native defects in cubic silicon carbide from first principles

The diffusion of Mg defects in 3C-SiC is studied using the density functional theory. Mg has the highest burn-in rate as a transmutant in 3C-SiC when it is placed in high-energy neutron irradiation environment of a fusion reactor. The presence and evolution of transmutant defects impact thermal and mechanical properties of this important structural material. This study is focused on understanding the structure, stability, and evolution of Mg defects and the interaction of Mg with native defects in 3C-SiC. Our calculations of diffusion coefficients for different Mg defects suggest that Mg is likely to diffuse faster in pristine 3C-SiC than in the damaged one, in agreement with earlier experimental observations.

36 MATERIALS SCIENCE↗

Synchrotron self-Compton in a radiative-adiabatic fireball scenario: modelling the multiwavelength observations in some Fermi /LAT bursts

Energetic GeV photons expected from the closest and the most energetic Gamma-ray bursts (GRBs) provide a unique opportunity to study the very-high-energy emission as well as the possible correlations with lower energy bands in realistic GRB afterglow models. In the standard GRB afterglow model, the relativistic homogeneous shock is usually considered to be fully adiabatic, however, it could be partially radiative. Based on the external forward-shock scenario in both stellar wind and constant-density medium, we present a radiative-adiabatic analytical model of the synchrotron self-Compton (SSC) and synchrotron processes considering an electron energy distribution with a power-law index of $1\lt p\lt 2$ and $2\le p$. We show that the SSC scenario plays a relevant role in the radiative parameter $\epsilon$, leading to a prolonged evolution during the slow cooling regime. In a particular case, we derive the Fermi/LAT light curves together with the photons with energies $\ge 100$ MeV in a sample of nine bursts from the second Fermi/LAT GRB catalogue that exhibited temporal and spectral indices with $\gtrsim 1.5$ and $\approx 2$, respectively. These events can hardly be described with closure relations of the standard synchrotron afterglow model, and also exhibit energetic photons above the synchrotron limit. We have modelled the multiwavelength observations of our sample to constrain the microphysical parameters, the circumburst density, the bulk Lorentz factor, and the mechanism responsible for explaining the energetic GeV photons.

acceleration of particles↗

Microscopy X-ray imaging enriched with small angle X-ray scattering for few nanometer resolution reveals shock waves and compression in intense short pulse laser irradiation of solids

Understanding how laser pulses compress solids into high-energy-density states requires diagnostics that simultaneously resolve macroscopic geometry and nanometer-scale structure. Here we present a combined X-ray imaging (XRM) and small-angle X-ray scattering (SAXS) approach that bridges this diagnostic gap. Using the Matter in Extreme Conditions end station at LCLS, we irradiated 25 μm copper wires with 45 fs, 0.9 J, 800 nm pulses at 3.5 × 10 19 W/cm 2 while probing with 8.2 keV XFEL pulses. XRM visualizes the evolution of ablation, compression, and inward-propagating fronts with ∼ 200 nm resolution, while SAXS quantifies their nanometer-scale sharpness via the time-resolved evolution of scattering streaks. The joint analysis reveals that an initially smooth compression steepens into a nanometer-sharp shock front after t sh ≈ (18 ± 3) ps, consistent with an analytical steepening model and hydrodynamic simulations. The front reaches a velocity of c sh ≈ 25 k m / s and a lateral width of several tens of microns, demonstrating direct observation of shock formation and decay at solid density for the first time with few-nanometer precision. This integrated XRM–SAXS method establishes a quantitative, multi-scale diagnostic of laser-driven shocks in dense plasmas relevant to inertial confinement fusion, warm dense matter, and planetary physics.

Kluge, Thomas [Helmholtz-Zentrum Dresden-Rossendor↗

The classical equations of motion of quantized gauge theories, Part 2: Electromagnetism

In this and companion papers, we show that quantum field theories with gauge symmetries permit a broader class of classical dynamics than typically assumed. In this article, we show that the quantization of electromagnetism permits the existence of classical electric field states that do not obey Gauss’s law. These states are gauge invariant and their time evolution can be consistently described using the Schrödinger equation. The time evolution of these states is such that at the classical level, the full set of Maxwell’s equations would appear to hold, with the physical effects of these states being attributable to an auxiliary, static “shadow” charge density with no internal degrees of freedom. This density could affect the dynamics of charged particles in our universe and it may thus be of observational interest.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Magnetization orientation-dependent Shubnikov-de Haas oscillations in ferromagnetic Weyl semimetal Co 3 Sn 2 S 2

We report a study of Shubnikov–de Haas oscillations in high-quality single crystals of ferromagnetic Weyl semimetal Co 3 Sn 2 S 2 . The Fermi surfaces resolved in our experiments are three-dimensional and reflect an underlying trigonal crystallographic symmetry. Combined with density functional calculations, we identify that multiple Fermi surfaces in the system—of both electron and hole nature—arise from the energy dispersion of the (spin-orbit gapped) mirror-protected nodal rings. We observe an evolution of the Fermi surfaces with in-plane magnetic fields, in contrast to field perpendicular to the kagome lattice planes, which has little effect. Viewed alongside the easy-axis anisotropy of the system, our observation reveals an evolution of the electronic structure of Co 3 Sn 2 S 2 —including the Weyl points—with the ferromagnetic moment orientation. Through the case study of Co 3 Sn 2 S 2 , our results provide concrete experimental evidence of an anisotropic interplay via spin-orbit coupling between the magnetic degrees of freedom and electronic band singularities, which has long been expected in semimetallic and metallic magnetic systems.

36 MATERIALS SCIENCE↗