Spin Crossover and Exchange Effects on Oxygen Evolution Reaction Catalyzed by Bimetallic Metal Organic Frameworks
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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
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Delving into the depths of NGC 3783 with XRISM V. Broad-band modelling of ionized outflows
The Seyfert 1 galaxy NGC 3783 hosts a multi-phase warm absorber (WA) that has been extensively studied in the X-ray band. High-resolution spectra from 2000−2001 revealed a complex outflow with multiple ionization and velocity components. Two decades later, new XMM-Newton and XRISM observations allow us to investigate the long-term evolution of these outflows. We performed joint spectral modelling of the XMM-Newton /RGS and XRISM/Resolve time-averaged spectra using the pion photoionization code within SPEX. We derived the ionization parameter, column density, turbulent velocity, and outflow velocity for each absorption component, and investigated their thermal stability and absorption measure distribution (AMD) to characterize the physical and dynamical properties of the WA in NGC 3783 in 2024. We compared these results with the 2000−2001 epoch to assess long-term variability, stability, and possible changes in the absorber population. We identify eight WA components spanning log ξ = 1.08 − 3.38 and outflow velocities of 480−1230 km s −1 . The ranges of column densities and turbulent velocities remain broadly consistent with the WAs from 2000−2001, but the earlier data contained more low-ionization, high-velocity components. The total column density of all the outflows in 2024 is 1.5 times larger than in 2000−2001, which means that it has been replenished by fresh material. The dominant unresolved transition array (UTA) absorber (component B3) has increased its column density by a factor of three while maintaining a similar ionization parameter. The WAs in NGC 3783 have undergone significant structural and dynamical evolution over the past 24 years.
79 ASTRONOMY AND ASTROPHYSICS↗
Microstructural Evolution of Tantalum During Deformation and Subsequent Annealing
Microstructure-aware models are necessary to predict the behavior of material based on process knowledge or to extrapolate mechanical properties of materials to environmental conditions which are not easily reproduced in the laboratory, e.g., nuclear reactor environments. Elemental Ta provides a relatively simple BCC system in which to develop a microstructural understanding of deformation processes which can then be applied to more complicated BCC alloys. In situ neutron diffraction during compressive deformation and subsequent heat treatment have been used to monitor the evolution of microstructural features in Ta throughout simulated processing steps. Crystallographic texture and dislocation density are determined as a function of first plastic strain, then temperature. Lattice strains are determined and attributed to stresses at macroscopic, grain and dislocation length scales. The increase of the dislocation density through deformation and subsequent recovery during heat treatment is monitored through the changing diffraction line profile. Also, randomization of the texture is used as a signature of recrystallization. The recovery of dislocations through annihilation is not observed to depend on the initial dislocation density in the range studied here. In contrast, recrystallization is observed to depend strongly on the initially dislocation density.
36 MATERIALS SCIENCE↗
2D analysis of tokamak divertor-plasma detachment-bifurcation with operational parameters and geometries
UEDGE simulations with density scans for various input power, transport coefficients and outer poloidal leg length are performed to study the conditions for the existence of a bifurcation-like drop of T e at the outer strike point, commonly referred to as a detachment cliff, when transitioning to a detached plasma from an attached plasma in the outer divertor as the upstream density increases (McLean et al., 2015). The simulation results show that a detachment cliff tends to occur with a higher power input regardless of diffusivities and leg length. Further analysis of change of plasma profiles at a cliff indicate that, in addition to the sharp reduction of the E x B drift fluxes in the outer divertor studied in Jaervinen et al., (2018), the substantial change of the Mach number in the outer divertor and the decrease of the outer mid-plane T e due to the radiation front moving across the separatrix into the confinement region above the X-point consistently occur for all UEDGE density scans that have a detachment cliff. UEDGE time-dependent simulation of the evolution of a detachment cliff shows that the rapid increase of radiation above the X-point occurs in a time scale of ~0.3–0.5, which could possibly be the trigger for the formation of a detachment cliff, quicker than the Mach number change in a time scale of ~1 ms and the drop of T e in a time scale of ~2–3 ms in the outer divertor.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Electrical conductivities of (Mg,Fe)O at extreme pressures and implications for planetary magma oceans
During planet formation, planets undergo many impacts that can generate magma oceans. When these crystallize, part of the magma densifies via iron enrichment and migrates to the core–mantle boundary, forming an iron-rich basal magma ocean (BMO). The BMO could generate a dynamo in early Earth and super-Earths if the electrical conductivity of the BMO, which is thought to be sensitive to its Fe content, is sufficiently high. To test this hypothesis, here we conduct laser-driven shock experiments on ferropericlase (Mg x ,Fe 1−x )O (0.95 ≤ x ≤ 1) as an Fe-rich BMO analogue, perform density functional theory molecular dynamics simulations on MgO and calculate the long-term evolution of super-Earths. We find that the d.c. conductivities of MgO and (Mg,Fe)O are indistinguishable between 467 GPa and 1,400 GPa, despite previous predictions. Here, we predict that super-Earths larger than 3–6 Earth masses can produce BMO-driven dynamos that are almost one order of magnitude stronger than core-driven dynamos for several billion years.
Exoplanets↗
Smoothing and flattening the universe through slow contraction versus inflation
In a systematic study, we use an equivalent pair of improved numerical relativity codes based on a tetrad-formulation of the classical Einstein-scalar field equations to examine whether slow contraction or inflation (or both) can resolve the homogeneity, isotropy and flatness problems. Our finding, based on a set of gauge/frame invariant diagnostics and the models considered, is that slow contraction robustly and rapidly smooths and flattens spacetime beginning from initial conditions that are outside the perturbative regime of the flat Friedmann-Robertson-Walker metric, whereas inflation fails these tests. We present new numerical evidence supporting the conjecture that the combination of ultralocal evolution and an effective equation-of-state with pressure much greater than energy density is the key to having robust and rapid smoothing. The opposite of ultralocality occurs in expanding spacetimes, which is the leading obstruction to smoothing following a big bang.
79 ASTRONOMY AND ASTROPHYSICS↗
Photoluminescence probing of light absorption centers at silica laser damage
We use photoluminescence (PL) imaging to study damage growth precursors within laser damage sites on the surface of silica. Damage site evolution is induced by multiple shots of UV nanosecond pulsed laser at various energy densities and monitored throughout the early stages of growth. Wide-field PL imaging rapidly locates microscopic light absorption centers within the silica damage site. Our quantitative analysis shows that damage sites with strong local PL intensity show a higher probability of growth upon subsequent laser pulses. Scanning electron microscopy (SEM) paired with a study of PL spectrum shows that the strong PL intensity appears from the subsurface fractures with high defect density, which provides a local light absorption center leading to significant damage growth. We believe that this result offers an efficient optical damage mitigation strategy by providing a rapid and non-destructive optical inspection approach.
36 MATERIALS SCIENCE↗
Precision Kinematic Sunyaev--Zel'dovich Measurements Across Halo Mass and Redshift with DESI DR2 and ACT DR6: Part I. Luminous Red Galaxies
We present the most precise measurements of the kinetic Sunyaev-Zel'dovich (kSZ) effect around luminous red galaxies to date, detecting the signal at $18σ$ significance in both harmonic and configuration space. Our analysis cross-correlates 2.4 million spectroscopic LRGs from the Dark Energy Spectroscopic Instrument (DESI) DR2 sample with Data Release 6 (DR6) of the Atacama Cosmology Telescope (ACT). We develop a novel harmonic-space cross-correlation approach using momentum-weighted kSZ templates, yielding nearly uncorrelated bandpowers within a framework consistent with other large-scale structure analyses. By incorporating the LRG halo occupation distribution (HOD) and its uncertainty, we convert measured galaxy gas profiles into halo gas profiles and provide generalized Navarro-Frenk-White (GNFW) fitting profiles, providing empirical targets for tuning feedback efficiency in hydrodynamical simulations and for baryonic modeling in large-scale structure analyses. We find strong evidence that gas profiles do not trace dark matter, providing direct evidence for gas redistribution beyond gravitational collapse. Comparing to hydrodynamical simulations, our measurements favor feedback efficiencies exceeding those in the Battaglia profile, suggesting more efficient gas ejection in group-scale halos than previously predicted. Splitting by redshift, we detect the kSZ signal at SNR $\approx 5$--$10$ in each of four bins and find amplitude evolution consistent with the expected decline in mean halo mass at fixed comoving number density. Splitting by stellar mass, we study the scaling of kSZ amplitude with galaxy properties. Together with BGS and ELG measurements in Paper II, these results span $0.1 \lesssim z \lesssim 1.6$ across three galaxy populations, demonstrating the potential of spectroscopic kSZ to map circumgalactic gas and constrain baryonic feedback.
Qu, F. J. [KIPAC, Menlo Park; Stanford U., HEPL; S↗
Spatially and temporally resolved plasma parameter estimations of laser heated MagLIF relevant gas pipes at NIF
The ability to control laser pre-heat is an integral part of the inertial confinement fusion concept known as Magnetized Liner Inertial Fusion. This process is studied at the National Ignition Facility (NIF) where 4 of the 192 laser beams are propagated through a 1-cm long gas cell where they deposit >20 kJ of energy into the gaseous fuel via inverse bremsstrahlung absorption. This process ionizes the gas, producing a plasma that follows behind the laser front and expands over the radius of the cell. Emission from this plasma, as viewed by a gated x-ray detector, can be used to build spatially and temporally resolved estimations of the pre-heat plasma's density and temperature profiles. This can then be used to estimate the plasma pressure, internal energy, and radiation losses. Estimations show the evolution of the plasma in magnetized and unmagnetized gas cells filled with ambient temperature neopentane (C5H12) +1% Ar, as well as unmagnetized cryogenically cooled (32 K) deuterium +1% Ne filled targets. This analysis shows the effects of initial gas-fill density, composition, and axial magnetization on the time-dependent plasma parameters. Previously, these parameters at the NIF had not been experimentally characterized, and these estimations provided a potential new means of testing radiation magneto-hydrodynamic predictive capability models. Results in unmagnetized targets have strong agreement with simulations. However, in targets with a 19 T applied axial magnetic field, this method yields electron temperatures up to 100% hotter than those predicted by HYDRA codes.
Bremsstrahlung↗
First Measurement of Z Opacity Sample Evolution near Solar Interior Conditions Using Time-Resolved Spectroscopy
Opacity model differences with Fe opacity measurements at high temperature (T>180 eV ) and high electron density (𝑛 𝑒 >3×10 22 cm −3 ) at nearly solar interior conditions have remained unresolved [Bailey et al., Nature 517, 56 (2015) and Nagayama et al., Phys. Rev. Lett. 122, 235001 (2019)]. Systematic errors from temporal gradients are one hypothesis for the discrepancy. Past data recorded on x-ray film provided spectral measurements over a time determined by the 2.8-ns backlighter duration. Here, we present the first measurements of opacity sample temporal evolution using novel hCMOS ultrafast x-ray camera technology. The measured conditions, measured backlighter time history, and modeled opacities are used to show that temporal gradients do not resolve the model-data discrepancy. The methods demonstrated provide potential advantages, including opacities at more extreme conditions, spectral line shift measurements, and improved measurements at other facilities.
atomic spectra↗
Operando X-ray imaging reveals size-dependent evolution of cobalt oxide thermochemical material during thermal redox cycles
Multivalent metal oxides are promising thermochemical materials (TCMs) for energy storage and conversion owing to their high energy density, air compatibility, and high-temperature stability. Co 3 O 4 serves as a model system for examining particle-size- and structure-dependent redox behavior. While particle size and porosity are known to affect performance, their interplay and the kinetics of pore formation during cycling remain unclear. Here we show the chemical and 3D morphological evolution of Co 3 O 4 micro- and nanoparticles during redox cycles at 800–900 °C using thermal analysis, in-situ synchrotron transmission X-ray microscopy (TXM), and scanning electron microscopy. Thermal analysis shows that nanoparticles re-oxidize more rapidly than microparticles at 800 °C. In-situ nanotomography and chemical imaging reveals that nanoparticles undergo redox conversion without forming internal pores, whereas microparticles develop isolated porosity during reduction. These pores persist through re-oxidation, correlating to a lower conversion rate in subsequent cycles. Our results demonstrate distinct degradation kinetics in Co 3 O 4 micro- and nanoparticles, underscoring the critical role of particle size and porosity in redox performance and informing strategies to enhance the long-term efficiency of metal oxide TCMs.
25 ENERGY STORAGE↗
Facile One-Pot Block Copolymer-Mediated Solvothermal Approach for Synthesis of High-Entropy Alloy with Enhanced OER Activity
Herein, we introduce a straightforward synthesis approach for highly active dendritic multimetallic high-entropy alloy (DMHEA@PtIrPdAgRu) nanoparticles with sufficient entropic mixing, featuring uniform distribution of five noble group metals (Pt, Ir, Pd, Ag, and Ru) via a block copolymer-mediated one-pot solvothermal reduction method for oxygen evolution reaction (OER). In this synthesis, N,N -dimethylformamide (DMF) is used as a reductant as well as solvent and core–shell-corona-type (poly(styrene)- block -poly(vinylpyridine)- block -poly(ethylene oxide)) (PS-PVP-PEO) block copolymer as a structure directing agent. The cooperative effect between the copolymer architecture and the reducing environment of DMF promoted a confined nucleation mechanism for forming a single-phase dendritic structure HEA with high compositional uniformity, thereby mitigating phase segregation, a common challenge in the synthesis of multimetallic nanoparticles. This prepared DMHEA@PtIrPdAgRu catalyst exhibits a low overpotential of 490 mV to attain a high current density of 100 mA cm –2 with a Tafel slope of 442 mV dec –1 for oxygen evolution. The superior OER performance is attributed to the synergistic cooperation among its active and coordinated metal centers as well as the incorporation of corrosion-resistant metal like platinum.
block copolymer↗
The cosmology of ultralight scalar dark matter coupled to right-handed neutrinos
We consider ultralight scalar dark matter that couples to right-handed neutrinos. Due to the high density of neutrinos in the early universe, the background neutrino density dominates the dynamics of the scalar field, and qualitatively alters the field’s cosmological evolution. This effect has not been included in previous literature, and changes the interpretation of cosmological data and its interplay with laboratory experiments. To illustrate these points a simplified model of a 1 + 1 setup with a single scalar field is analyzed.
Cosmology of Theories BSM↗
The porosity surrounding carbides and second phase stringers in monolithic U-10Mo fuel plate after irradiation
Post-irradiation microstructure characterization plays an important role in qualifying the low-enriched uranium (LEU) monolithic U-10 wt%Mo plate-type fuel for United States high-performance research reactors (USHPRRs) program. Inhomogeneous features resulting from manufacturing and irradiation processes, including carbides, second phase stringers, and extensive void spaces caused by the combining of small porosities, may increase the risk of heat concentration in local regions of the fuel plate over the operating conditions. In this study, characteristics of carbides, stringers, and porosity after multiple levels of irradiation at varying fission densities were studied by electron microscopes to decipher the morphology of pores and the porosity evolution in U-10 wt%Mo. For carbides, the result shows that porosities start forming on UMo grain boundaries, then on UMo/carbides interfaces as the burn-up going higher. However, the porosities surrounding carbides grow larger than the ones on UMo grain boundaries. The porosities around the uranium carbides could interconnect to form larger void space. The study revealed that the void spaces larger than 5 µm were found around uranium carbides after high burnup, while no evidence was observed to support the similar voids formed near second phase stringers even though the size of the stringers (> 50 µm) was much larger than uranium carbides (< 20 µm). The evolution of porosities suggests that the formation of second phase stringers may not create more significant porosities compared to regular uranium carbides regions during fuel operating conditions.
11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
Probing the atomic dynamics of ultrafast melting with femtosecond electron diffraction
Melting is an every-day phase transition that is determined by thermodynamic parameters like temperature and pressure. In contrast, ultra-fast melting is governed by the microscopic response to a rapid energy input and, thus, can reveal the strength and dynamics of atomic bonds as well as the energy flow rate to the lattice. Accurately describing these processes remains challenging and requires detailed insights into transient states encountered. Here, we present data from femtosecond electron diffraction measurements that capture the structural evolution of copper during the ultrafast solid-to-liquid phase transformations. At absorbed energy densities 2-4 times the melting threshold, melting begins at the surface slightly below the nominal melting point followed by rapid homogeneous melting throughout the volume. Molecular dynamics simulations reproduce these observations and reveal a weak electron-lattice energy transfer rate for the given experimental conditions. Both simulations and experiments show no indications of rapid lattice collapse when its temperature surpasses proposed limits of superheating, providing evidence that the inherent dynamics limits the speed of disordering in ultrafast melting of metals.
FOS: Physical sciences↗
Constraints on Large-Scale White Noise in the Cosmic Density Field
We present observational constraints on large-scale white noise (LSWN) in the cosmic density field, a phenomenon predicted to arise from non-linear mode coupling during cosmological evolution. Building on the theoretical framework of Paper I, where we demonstrated that non-linearities inevitably redistribute power from small to large scales through mode mixing, we confront these predictions with current cosmological data. We modify the CLASS Boltzmann code to incorporate a white noise component $k_\mathrm{BH}/k$ in the primordial power spectrum and perform parameter estimation using current cosmological data. The non-detection of excess power on the largest observable scales places stringent upper bounds: $k_\mathrm{BH} \leq 1.80 \times 10^{-13}~\mathrm{Mpc}^{-1}$ at 99% confidence. These constraints imply the primordial power spectrum must deviate from perfect scale invariance on small scales, either through a cutoff at $k_{\mathrm{cut}} \lesssim 3~\mathrm{pc}^{-1}$ or through running of the spectral index with $α_s \lesssim -0.015$. Our results demonstrate that LSWN provides a powerful probe of the primordial spectrum at scales orders of magnitude smaller than directly observable, offering unique constraints on early-universe physics.
Barenboim, Gabriela [Valencia U., IFIC; Valencia U↗
Neural network denoising of x-ray images from high-energy-density experiments
Noise is a consistent problem for x-ray transmission images of High-Energy-Density (HED) experiments because it can significantly affect the accuracy of inferring quantitative physical properties from these images. We consider experiments that use x-ray area backlighting to image a thin layer of opaque material within a physics package to observe its hydrodynamic evolution. The spatial variance of the x-ray transmission across the system due to changing opacity serves as an analog for measuring density in this evolving layer. The noise in these images adds nonphysical variations in measured intensity, which can significantly reduce the accuracy of our inferred densities, particularly at small spatial scales. Denoising these images is thus necessary to improve our quantitative analysis, but any denoising method also affects the underlying information in the image. In this paper, we present a method for denoising HED x-ray images via a deep convolutional neural network model with a modified DenseNet architecture. In our denoising framework, we estimate the noise present in the real (data) images of interest and apply the inferred noise distribution to a set of natural images. These synthetic noisy images are then used to train a neural network model to recognize and remove noise of that character. We show that our trained denoiser network significantly reduces the noise in our experimental images while retaining important physical features.
47 OTHER INSTRUMENTATION↗
The ionomer as an oxygen evolution reaction promoter: piperidinium’s impact on mechanistic pathways on NiO, IrO 2 , and Fe–NiO
The commercial viability of anion exchange membrane (AEM) electrolysis requires optimization of various stack components, with specific catalyst-ionomer combinations often yielding higher current densities, lowered Tafel slopes, and improved mass activity. In this joint theoretical-experimental study, theoretical calculations detail the impact of Versogen’s piperidinium functional group on the complex, kinetically limiting oxygen evolution reaction, finding that the functional group can act as a promoter of specific steps (O*/O 2 * formation; H 2 O/O 2 desorption with reaction enthalpies ranging between 0.2–0.6 eV at higher coverages of O x H y intermediates) on NiO and NiFeO x catalysts. In particular, Fe sites on the NiFeO x catalyst facilitate concerted mechanisms of O*/O 2 * formation and H 2 O desorption with a low enthalpy of 0.5 eV; O 2 desorption alone requires only 0.3 eV. In contrast, Versogen-IrO 2 results in stronger Ir–O bonds, where the enthalpies for bond breaking (Ir–OH 2 and Ir–O 2 ) are considerably higher (1.4 eV and 1.6 eV, respectively). Rotating disk electrode studies utilized commercially available NiO and IrO 2 and synthesized 7.5 wt % Fe in NiFeO x catalysts in combination with Versogen, a common AEM ionomer, and Nafion, an alternative binder. Electrochemical testing validated the impact of these mechanistic changes on ionomer-catalyst combinations, finding that Versogen particularly activates NiO and NiFeO x compared to IrO 2 . Following a 13.5 h hold at 1.8 V, mass activities and Tafel slopes improved to 34 ± 13 A g −1 and 79 ± 2 mV dec −1 (NiO) and 82 ± 4.9 A g −1 and 72 ± 2 mV dec −1 (NiFeO x ). In contrast, Versogen-IrO 2 only reached 17 ± 2.9 A g −1 and 81 ± 3 mV dec −1 . Optimization of the ionomer-catalyst can yield significant increases in performance from initial activity and after an electrochemical conditioning procedure: this enhancement to the mass activity resulted in a 200.9 ± 106.1% improvement for Versogen-NiFeO x and 1284.2 ± 260.5% for Versogen-NiO. In contrast, Nafion-NiFeO x and -NiO offered moderate improvements of 39.1 ± 30.5% and 120.9 ± 59.1%, respectively.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗