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At least 361 records · Page 20

Microstructure and electrochemical hydrogenation/dehydrogenation performance of melt-spun La-doped Mg{sub 2}Ni alloys

This work focuses on microstructure and electrochemical hydrogen storage properties of La-doped Mg{sub 2}Ni alloys. The alloys with nominal compositions of Mg{sub 2}Ni{sub 1−x}La{sub x} (x = 0, 0.1, 0.3, 0.5) were prepared via metallurgical smelting and melt-spun on a rotating copper wheel. The scanning electron microscope, X-ray diffraction, differential scanning calorimetry and transition electron microscope, galvanostatic charging/discharging and other electrochemical measurements were employed to investigate. The results show that the increasing of La content and melt-spinning speed favors the formation of Mg–Ni–La amorphous/nanocrystalline alloys. It is found that the melt-spun ribbons display increased discharge capacities and superior cycle stabilities compared to the as-cast alloys with and without La. The potentiodynamic polarization results indicate that melt-spun La-doped Mg{sub 2}Ni ribbons possess more positive corrosion potential E{sub corr} and exhibit relatively high corrosion resistance against the alkaline solution. The mechanism for electrochemical hydrogenation/dehydrogenation has been proposed based on the effect of microstructures on the mass/charge transfer process for electrode electrochemical reaction. - Highlights: • Nanocrystalline/amorphous Mg–Ni–La alloys are obtained by melt-spinning. • Microstructures of as-cast and rapid quenched Mg{sub 2}Ni{sub 1−x}La{sub x} alloys are investigated. • Electrochemical hydrogenation properties of experimental alloys are characterized. • Electrochemical hydrogen absorption/desorption mechanism is proposed.

36 MATERIALS SCIENCE↗

Ligand-Free Processable Perovskite Semiconductor Ink

We report traditional covalent semiconductors require complex processing methods for device fabrication due to their high cohesive energies. Here, we develop a stable, ligand-free perovskite semiconductor ink that can be used to make patterned semiconductor-based optoelectronics in one step. The perovskite ink is formed via the dissolution of crystals of vacancy-ordered double perovskite Cs 2 TeX 6 (X = Cl - , Br - , I - ) in polar aprotic solvents, leading to the stabilization of isolated [TeX 6 ] 2- octahedral anions and free Cs + cations without the presence of ligands. The stabilization of the fundamental perovskite ionic octahedral building blocks in solution creates multifunctional inks with the ability to reversibly transform between the liquid ink and the solid-state perovskite crystalline system in air within minutes. These easily processable inks can be patterned onto various materials via dropcasting, spraying or painting, and stamping, highlighting the crucial role of solvated octahedral complexes toward the rapid formation of phase-pure perovskite structures in ambient conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Intrinsic nonlocality of spin- and polarization-resolved probabilities in strong-field quantum electrodynamics

Spin and polarization are central to precision tests of fundamental physics and for interpreting radiation from astrophysical sources and ultraintense laser-matter experiments. Here, focusing on the fundamental process of nonlinear Compton scattering, we demonstrate that a key assumption underlying current strong-field quantum electrodynamics models, i.e., that emission can be treated as an instantaneous random event sampled from a local differential rate, is inconsistent once emission angles, electron spin, and/or photon polarization are resolved. Namely, even in strictly constant and uniform fields , the resulting fully differential distribution is sign indefinite, yielding negative inferred probabilities. The physical reason is that the photon emission probability builds up over a finite length of the electron trajectory, the formation region, during which the electron direction changes by roughly the same small angle that defines the radiation cone. Therefore, we put forward a new method where we integrate over this formation region analytically to obtain a physically consistent electron spin and photon polarization model. We show that the implementation of our model is compatible with existing Monte Carlo and particle-in-cell workflows. Simulations of a GeV-class electron-laser collision accessible at current petawatt facilities and of emission in a pulsarlike magnetic field are shown to reveal spin and polarization patterns that differ even qualitatively from state-of-the-art local models. In particular, our new model predicts substantial angle-dependent circular photon polarization where the well-known collinear-emission approach yields none, and a pronounced helicity bias in the recoiling electrons absent from current predictions. These findings have direct implications for upcoming strong-field QED experiments and for interpreting polarized radiation from extreme astrophysical environments.

astrophysical electromagnetic fields↗

Mars - Chemical weathering as a massive volatile sink

The amounts of volatiles incorporated in the Martian regolith by photostimulated oxidation weathering of Fe(2+)-bearing minerals are estimated. The process of photostimulated oxidation weathering is described, and it is noted that all the necessary constituents for this process are present on Mars. The rates at which oxygen and hydrogen are irreversibly removed from the Martian atmosphere by the present process are determined, irreversible and reversible water losses are considered, and the loss of CO2 by carbonate formation is shown to be irreversible. The results suggest that photostimulated oxidation weathering has irreversibly consumed 100 to 100,000 g/sq cm of H2O and 10 to 10,000 g/sq cm of CO2, assuming a uniform rate over geologic time. It is concluded that if the amounts of H2O and CO2 actually removed by photostimulated oxidation are close to the upper limits of the present estimates, then that process may have had a major effect in limiting the amount of H2O and CO2 trapped in the regolith and polar caps.

Huguenin, R. L.↗

Ice Processes and Growth History on Arctic and Sub-Arctic Lakes Using ERS-1 SAR Data

A survey of ice growth and decay processes on a selection of shallow and deep sub-Arctic and Arctic lakes was conducted using radiometrically calibrated ERS-1 SAR images. Time series of radar backscatter data were compiled for selected sites on the lakes during the period ot ice cover (September to June) for the years 1991-1992 and 1992-1993. A variety of lake-ice processes could be observed, and significant changes in backscatter occurred from the time of initial ice formation in autumn until the onset of the spring thaw. Backscatter also varied according to the location and depth of the lakes. The spatial and temporal changes in backscatter were most constant and predictable at the shallow lakes on the North Slope of Alaska. As a consequence, they represent the most promising sites for long-term monitoring and the detection of changes related to global warming and its effects on the polar regions.

Morris, K.↗

Hidden domain boundary dynamics toward crystalline perfection

A central paradigm of nonequilibrium physics concerns the dynamics of heterogeneity and disorder, impacting processes ranging from the behavior of glasses to the emergent functionality of active matter. Understanding these complex mesoscopic systems requires probing the microscopic trajectories associated with irreversible processes, the role of fluctuations and entropy growth, and the timescales on which nonequilibrium responses are ultimately maintained. Approaches that illuminate these processes in model systems may enable a more general understanding of other heterogeneous nonequilibrium phenomena, and potentially define ultimate speed and energy cost limits for information processing technologies. Here, we apply ultrafast single-shot X-ray photon correlation spectroscopy to resolve the nonequilibrium, heterogeneous, and irreversible mesoscale dynamics during a light-induced phase transition in a (PbTiO 3 ) 16 /(SrTiO 3 ) 16 superlattice. Such ferroelectric superlattice systems are a useful platform to study phase transitions and topological dynamics due to their high degree of tunability. This provides an approach for capturing the nucleation of the light-induced phase, the formation of transient mesoscale defects at the boundaries of the nuclei, and the eventual annihilation of these defects, even in systems with complex polarization topologies. We identify a nonequilibrium correlation response spanning >10 orders of magnitude in timescales, with multistep behavior similar to the plateaus observed in supercooled liquids and glasses. We further show how the observed time-dependent long-time correlations can be understood in terms of stochastic and non-Markovian dynamics of domain walls, encoded in waiting-time distributions with power-law tails. This work defines possibilities for probing the nonequilibrium and correlated dynamics of disordered and heterogeneous media.

36 MATERIALS SCIENCE↗

Polarization signatures for abandoned agricultural fields in the Manix Basin area of the Mojave Desert

Polarimetric signatures from abandoned circular alfalfa fields in the Manix Basin area of the Mojave desert show systematic changes with length of abandonment. The obliteration of circular planting rows by surface processes could account for the disappearance of bright 'spokes', which seems to be reflection patterns from remnants of the planting rows, with increasing length of abandonment. An observed shift in the location of the maximum L-band copolarization return away from VV, as well as an increase in surface roughness, both occurring with increasing age of abandonment, seems to be attributable to the formation of wind ripple on the relatively vegetationless fields. A Late Pleistocene/Holocene sand bar deposit, which can be identified in the radar images, is probably responsible for the failure of three fields to match the age sequence patterns in roughness and peak shift.

Ray, Terrill W.↗

Effect of Time and Deposition Method on Quality of Phosphonic Acid Modifier Self-Assembled Monolayers on Indium Zinc Oxide

Phosphonic acid (PA) self-assembled monolayers (SAMs) are utilized at critical interfaces between transparent conductive oxides (TCO) and organic active layers in organic photovoltaic devices (OPVs). The effects of PA deposition method and time on the formation of close-packed, high-quality monolayers is investigated here for SAMs fabricated by solution deposition, micro-contact printing, and spray coating. The solution deposition isotherm for pentafluorinated benzylphosphonic acid (F5BnPA) on indium-doped zinc oxide (IZO) is studied using polarization modulation-infrared reflection-absorption spectroscopy (PM-IRRAS) at room temperature as a model PA/IZO system. Fast surface adsorption occurs within the first min; however, well-oriented high-quality SAMs are reached only after -48 h, presumably through a continual process of molecular adsorption/desorption and monolayer filling accompanied by molecular reorientation. Two other rapid, soak-free deposition techniques, micro-contact printing and spray coating, are also explored. SAM quality is compared for deposition of phenyl phosphonic acid (PPA), F13-octylphosphonic acid (F13OPA), and pentafluorinated benzyl phosphonic acid (F5BnPA) by solution deposition, micro-contact printing and spray coating using PM-IRRAS. In contrast to micro-contact printing and spray coating techniques, 48-168 h solution deposition at both room temperature and 70 degrees C result in contamination- and surface etch-free close-packed monolayers with good reproducibility. SAMs fabricated by micro-contact printing and spray coating are much less well ordered.

14 SOLAR ENERGY↗

Anisotropic Excitons Reveal Local Spin Chain Directions in a van der Waals Antiferromagnet

A long‐standing pursuit in materials science is to identify suitable magnetic semiconductors for integrated information storage, processing, and transfer. Van der Waals magnets have brought forth new material candidates for this purpose. Recently, sharp exciton resonances in antiferromagnet NiPS 3 have been reported to correlate with magnetic order, that is, the exciton photoluminescence intensity diminishes above the Néel temperature. Here, it is found that the polarization of maximal exciton emission rotates locally, revealing three possible spin chain directions. This discovery establishes a new understanding of the antiferromagnet order hidden in previous neutron scattering and optical experiments. Furthermore, defect‐bound states are suggested as an alternative exciton formation mechanism that has yet to be explored in NiPS 3 . The supporting evidence includes chemical analysis, excitation power, and thickness dependent photoluminescence and first‐principles calculations. This mechanism for exciton formation is also consistent with the presence of strong phonon side bands. This study shows that anisotropic exciton photoluminescence can be used to read out local spin chain directions in antiferromagnets and realize multi‐functional devices via spin‐photon transduction.

36 MATERIALS SCIENCE↗

Thermodynamics of Light-Induced Nanoscale Polar Structures in Ferroelectric Superlattices

Here we study the thermodynamics of nanoscale polar structures in PbTiO 3 /SrTiO 3 ferroelectric superlattices induced by above-bandgap optical excitation using a phase-field model explicitly considering both structural and electronic processes. We demonstrate that the light-excited carriers provide the charge compensation of polarization bound charges and the lattice thermal energy, both of which are key to the thermodynamic stabilization of a previously observed supercrystal, a three dimensionally periodic nanostructure, within a window of substrate strains, while different mechanical and electrical boundary conditions can stabilize a number of other nanoscale polar structures by balancing the competing short-range exchange interactions responsible for the domain wall energy and longrange electrostatic and elastic interactions. The insights into the light-induced formation and richness of nanoscale structures from this work offer theoretical guidance for exploring and manipulating the thermodynamic stability of nanoscale polar structures employing a combination of thermal, mechanical, and electrical stimuli as well as light.

36 MATERIALS SCIENCE↗

Exploring the Impacts of Conditioning on Proton Exchange Membrane Electrolyzers by In Situ Visualization and Electrochemistry Characterization

For a proton exchange membrane electrolyzer cell (PEMEC), conditioning is an essential process to enhance its performance, reproducibility, and economic efficiency. To get more insights into conditioning, a PEMEC with Ir-coated gas diffusion electrode (IrGDE) was investigated by electrochemistry and in situ visualization characterization techniques. The changes of polarization curves, electrochemical impedance spectra (EIS), and bubble dynamics before and after conditioning are analyzed. The polarization curves show that the cell efficiency increased by 9.15% at 0.4 A/cm 2 , and the EIS and Tafel slope results indicate that both the ohmic and activation overpotential losses decrease after conditioning. The visualization of bubble formation unveils that the number of bubble sites increased greatly from 14 to 29 per pore after conditioning, at the same voltage of 1.6 V. Under the same current density of 0.2 A/cm 2 ; the average bubble detachment size decreased obviously from 35 to 25 µm. Furthermore, the electrochemistry and visualization characterization results jointly unveiled the increase of reaction sites and the surface oxidation on the IrGDE during conditioning, which provides more insights into the conditioning and benefits for the future GDE design and optimization.

08 HYDROGEN↗

Role of transients in the sustainability of solar coronal plumes

We report on the role of small-scale, transient magnetic activity in the formation and evolution of solar coronal plumes. Three plumes within equatorial coronal holes are analyzed over the span of several days based on the Solar Dynamic Observatory (SDO)/Atmospheric Imaging Assembly 171 Å and 193 Å images and SDO/Helioseismic and Magnetic Imager line-of-sight magnetograms. The focus is on the role of transient structures at the footpoints in sustaining coronal plumes for relatively long periods of time (i.e., several days). The appearance of plumes is a gradual and lengthy process. In some cases, the initial stages of plume formation are marked by the appearance of pillar-like structures whose footpoints are the sources of transient brightenings. In addition to nominal jets occurring prior to and during the development of plumes, the data show that a large number of small jets (i.e., {sup j}etlets{sup )} and plume transient bright points (PTBPs) occur on timescales of tens of seconds to a few minutes. These features are the result of quasi-random cancellations of fragmented and diffuse minority magnetic polarity with the dominant unipolar magnetic field concentration over an extended period of time. They unambiguously reflect a highly dynamical evolution at the footpoints and are seemingly the main energy source for plumes. This suggests a tendency for plumes to be dependent on the occurrence of transients (i.e., jetlets, and PTBPs) resulting from low-rate magnetic reconnection. The decay phase of plumes is characterized by gradual fainting and multiple rejuvenations as a result of the dispersal of the unipolar magnetic concentration and its precipitation into multiple magnetic centers.

79 ASTRONOMY AND ASTROPHYSICS↗

Exploring the Impact of Copper Oxide Substitution on Structure, Morphology, Bioactivity, and Electrical Properties of 45S5 Bioglass®

In recent decades, the requirements for implantable medical devices have increased, but the risks of implant rejection still exist. These issues are primarily associated with poor osseointegration, leading to biofilm formation on the implant surface. This study focuses on addressing these issues by developing a biomaterial for implant coatings. 45S5 bioglass® has been widely used in tissue engineering due to its ability to form a hydroxyapatite layer, ensuring a strong bond between the hard tissue and the bioglass. In this context, 45S5 bioglasses®, modified by the incorporation of different amounts of copper oxide, from 0 to 8 mol%, were synthesized by the melt–quenching technique. The incorporation of Cu ions did not show a significant change in the glass structure. Since the bioglass exhibited the capacity for being polarized, thereby promoting the osseointegration effectiveness, the electrical properties of the prepared samples were studied using the impedance spectroscopy method, in the frequency range of 102–106 Hz and temperature range of 200–400 K. The effects of CuO on charge transport mobility were investigated. Additionally, the bioactivity of the modified bioglasses was evaluated through immersion tests in simulated body fluid. The results revealed the initiation of a Ca–P-rich layer formation on the surface within 24 h, indicating the potential of the bioglasses to enhance the bone regeneration process.

Hammami, Imen (ORCID:0000000290072221)↗

Origin of the Anomalously Rocky Appearance of Tsiolkovskiy Crater

Rock abundance maps derived from the Diviner Lunar Radiometer instrument on the Lunar Reconnaissance Orbiter (LRO) show Tsiolkovskiy crater to have high surface rock abundance and relatively low regolith thickness. The location of the enhanced rock abundance to the southeast of the crater is consistent with a massive, well-preserved impact melt deposit apparent in LRO Miniature Radio Frequency instrument circular polarization ratio data. A new model crater age using LRO Lunar Reconnaissance Orbiter Camera imagery suggests that while it originated in the Late Imbrian, Tsiolkovskiy may be the youngest lunar crater of its size ( approximately 180 km diameter). Together these data show that Tsiolkovskiy has a unique surface rock population and regolith properties for a crater of its size and age. Explanation of these observations requires mechanisms that produce more large blocks, preserve boulders and large blocks from degradation to regolith, and/or uncover buried rocks. These processes have important implications for formation of regolith on the Moon.

Greenhagen, Benjamin T.↗

Investigation of Mixed-Type Craters and the Role of Bifluoride Additives to Produce Zirconia-Toughened Alumina-Based PEO Coating

Al{sub 2}O{sub 3}-ZrO{sub 2} composite ceramic coatings were prepared on Al6061 aluminum alloy by plasma electrolytic oxidation in Na{sub 3}PO{sub 4}-K{sub 2}ZrF{sub 6}-Na{sub 2}SiF{sub 6}-based alkaline electrolyte. Optimum processing time for the coating formation was found to be ~ 50 min. Cross section and surface morphology of the coatings were analyzed using scanning electron microscope. From the phase and elemental composition analysis, the presence of m-ZrO{sub 2} and t-ZrO{sub 2} phases was confirmed. It was further observed that the peak intensities of t-ZrO{sub 2} and α-Al{sub 2}O{sub 3} phases increased with processing time, which was attributed to the enhanced crystallinity caused by the efficient sintering conditions. Corrosion properties were investigated by potentiodynamic polarization test in 3.5 wt.% NaCl solution. The results showed high improvement in corrosion rate with minimum recorded value ~ 0.25 mmy (mm/year) and corrosion current ~ 0.15 × 10{sup −6} A/cm{sup 2}.

36 MATERIALS SCIENCE↗

Optimization of La 2 NiO 4+δ Electrolysis Cell Oxygen Electrode through Surfactant-Enabled LaCoO 3±δ Nanocatalyst Deposition

Lanthanum nickelate (LNO) has shown promise as a Cr-resistant air electrode material for SOECs but has suboptimal surface oxygen exchange properties. Nanocoating of the LNO surface with lanthanum cobaltite (LCO) was chosen to improve cell performance as a surface oxygen conductor. The work focused on the implementation of a two-step nano-LCO film deposition utilizing catechol molecules in a porous LNO electrode. The subgoals of the work were to maintain nanosized LCO particles/ grains to increase active surface area and to control the regularity/ homogeneity of the coating across the microstructure. To achieve these goals, a novel surfactant-enhanced liquid infiltration method was utilized, where nucleation sites were spread across the electrode structure to control the location and size of LCO particles. Various catechol surfactant compositions were evaluated for their ability to control the kinetics of nanoparticle deposition and the homogeneity of the coating. Chelated LCO was characterized by X-ray diffraction (XRD), which found a substantial improvement in LCO formation with surfactant addition and determined polymerized norepinephrine to be the best-performing surfactant, with 88.4% pure LCO formed at low temperature. X-ray photoelectron spectroscopy (XPS) confirmed LCO nanostructures formed by the two-step infiltration process, showing no impurities and a stable perovskite structure. Deposition kinetics were analyzed using atomic force microscopy (AFM), correlating infiltration times and solution molarity to nanoparticle size and distribution, the results of which were confirmed in symmetrical cell samples by scanning electron microscopy (SEM). Electrochemical impedance spectroscopy (EIS) testing demonstrated substantial improvements in polarization resistance, where the nanocoating reduced the resistance by ∼55% to 0.152 Ω·cm 2 at 700 °C and 0.039 Ω·cm 2 at 800 °C. Electrical conductivity relaxation (ECR) at this temperature confirmed an improved surface oxygen exchange coefficient of the LCO + LNO heterostructure predicted by the Bode data from EIS, alongside a reduction in activation energy by about 30%.

Deposition↗

An Overview of the SOLVE-THESEO 2000 Campaign

Between November 1999 and April 2000, two major field experiments, the SAGE III Ozone Loss and Validation Experiment (SOLVE) and the Third European Stratospheric Experiment on Ozone (THESEO 2000), collaborated to form the largest field campaign yet mounted to study Arctic ozone loss. This international campaign involved more than 500 scientists from over 20 countries spread across the high and mid-latitudes of the northern hemisphere. The main scientific aims of SOLVE-THESEO 2000 were to study (a) the processes leading to ozone loss in the Arctic vortex and (b) the effect on ozone amounts over northern mid-latitudes. The campaign included satellites, heavy lift balloon launches, 6 different aircraft, ground stations, and scores of ozone-sonde. Campaign activities were principally conducted in 3 intensive measurement phases centered on early December 1999, late January 2000, and early March 2000. Observations made during the campaign showed that temperatures were unusually cold in the polar lower stratosphere over the course of the 1999-2000 winter. These cold temperatures resulted in the formation of extensive polar stratospheric clouds (PSCs) across the Arctic. Heterogeneous chemical reactions on the surfaces of the PSC particles produced high levels of reactive chlorine within the polar vortex by early January. This reactive chlorine catalytically destroyed about 60% of the ozone in a layer near 20 km between late January and mid-March 2000.

Newman, Paul A.↗