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At least 775 records · Page 43

Emergent Spin Dynamics Enabled by Lattice Interactions in a Bicomponent Artificial Spin Ice

Artificial spin ice (ASI) are arrays of nanoscaled magnets that can serve both as models for frustration in atomic spin ice as well as for exploring new spin-wave-based strategies to transmit, process, and store information. Here, we exploit the intricate interplay of the magnetization dynamics of two dissimilar ferromagnetic metals arranged on complimentary lattice sites in a square ASI to modulate the spin-wave properties effectively. We show that the interaction between the two sublattices results in unique spectra attributed to each sublattice, and we observe inter- and intra-lattice dynamics facilitated by the distinct magnetization properties of the two materials. The dynamic properties are systematically studied by angular-dependent broadband ferromagnetic resonance and confirmed by micromagnetic simulations. Here, we show that combining materials with dissimilar magnetic properties enables the realization of a wide range of two-dimensional structures, potentially opening the door to new concepts in nanomagnonics.

36 MATERIALS SCIENCE↗

Chemical Imaging of Atmospheric Biomass Burning Particles from North American Wildfires

The effects of biomass burning aerosols (BBA) on radiative forcing and cloud formation depend on chemical composition and the internal structures of individual particles within smoke plumes. To improve our understanding of the chemical and physical properties of BBA emitted at different times of the day and their evolution during atmospheric aging, we conducted a study as a part of the Fire Influence on Regional to Global Environments and Air Quality field campaign. Particle samples were collected onboard a research aircraft from smoke plumes from a wildfire in eastern Oregon during late afternoon and nighttime flights on August 28, 2019. A time-resolved aerosol collector was used to collect samples on substrates for offline spectromicroscopic imaging to investigate the single-particle characteristics of BBA particles. Approximately 20,400 individual particles from 10 selected samples were analyzed using computer-controlled scanning electron microscopy coupled with energy-dispersive X-ray microanalysis, revealing their elemental composition, morphology, and viscosity. Elemental microanalysis indicated that aged potassium is likely found in the form of K 2 SO 4 , KNO 3 , and possible K-organic salts. Further chemical speciation and carbon bonding mapping within individual particles were conducted using synchrotron-based scanning transmission X-ray microscopy (STXM) coupled with near edge X-ray absorption fine structure (NEXAFS) spectroscopy. Real-time, water-soluble light absorption measurements were acquired using a particle-into-liquid sampler instrument coupled to a liquid waveguide capillary cell and total organic analyzer. In the late afternoon samples, 65% of the total particle number population consisted entirely of organic components, compared to 46% in the nighttime particles. These differences were attributed to discrepancies in composition at the time of emission and to the daytime condensation and accumulation of photochemically formed secondary organic material on existing BBA particles, a process that halts at night. Microscopy images indicated that particle viscosity was lower in the nighttime particles (<10 1 Pa·s), likely due to increased relative humidity and a higher contribution from hygroscopic inorganic components. The chemical heterogeneity of individual particles was quantified using STXM-derived mixing state parameters. The nature of carbon bonding within individual particles was inferred from the extent of carbon sp 2 hybridization derived from NEXAFS spectra. Average percentages of sp 2 hybridization range between 40% and 60%, with no noticeable differences between late afternoon and nighttime flights. These findings were compared with the online optical properties of both late afternoon and nighttime smoke plumes, providing valuable insights into the complex relationship between chemical composition and optical properties of BBA particles at different times of the day.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Impact of Controlled Storage Conditions on the Hydrolysis and Surface Morphology of Amorphous-UO 3

The hydration and morphological effects of amorphous (A)-UO 3 following storage under varying temperature and relative humidity have been investigated. This study provides valuable insight into U-oxide speciation following aging, the U-oxide quantitative morphological data set, and, overall, the characterization of nuclear material provenance. A-UO 3 was synthesized via the washed uranyl peroxide synthetic route and aged based on a 3-factor circumscribed central composite design of experiment. Target aging times include 2.57, 7.00, 14.0, 21.0, and 25.4 days, temperatures of 5.51, 15.0, 30.0, 45.0, and 54.5 °C, and relative humidities of 14.2, 30.0, 55.0, 80.0, and 95.8% were examined. Following aging, crystallographic changes were quantified via powder X-ray diffraction and an internal standard Rietveld refinement method was used to confirm the hydration of A-UO 3 to crystalline schoepite phases. The particle morphology from scanning electron microscopy images was quantified using both the Morphological Analysis of MAterials software and machine learning. Results from the machine learning were processed via agglomerative hierarchical clustering analysis to distinguish trends in morphological attributes from the aging study. Significantly hydrated samples were found to have a much larger, plate-like morphology in comparison to the unaged controls. Predictive modeling via a response surface methodology determined that while aging time, temperature, and relative humidity all have a quantifiable effect on A-UO 3 crystallographic and morphological changes, relative humidity has the most significant impact.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Low Repetition-Rate, High-Resolution Femtosecond Transmission Electron Microscopy

Spatial and energy resolutions of state-of-the-art transmission electron microscopes (TEMs) have surpassed 50 pm and 5 meV. However, with respect to the time domain, even the fastest detectors combined with the brightest sources may only be able to reach the microsecond timescale. Thus, conventional methods are incapable of resolving myriad fundamental ultrafast (i.e., attosecond to picosecond) atomic-scale dynamics. The successful demonstration of femtosecond (fs) laser-based (LB) ultrafast transmission electron microscopy (UEM) nearly 20 years ago provided a means to span this nearly 10-order-of-magnitude temporal gap. While nanometer-picosecond UEM studies of dynamics are now well established, ultrafast Å-scale imaging has gone largely unrealized. Further, while instrument development has rightly been an emphasis, and while new modalities and uses of pulsed-beam TEM continue to emerge, the overall chemical and materials application space has been only modestly explored to date. In this Perspectives article, we argue that these apparent shortfalls can be attributed to a simple lack of data and detail. We speculate that present work and continued growth of the field will ultimately lead to the realization that Å-scale fs dynamics can indeed be imaged with minimally modified UEM instrumentation and with repetition rates (f rep ) below - and perhaps even well below - 1 MHz. We further argue that use of low f rep , whether for LB UEM or for chopped/bunched beams, significantly expands the accessible application space. Furthermore, this calls for systematically establishing modality-specific limits so that especially promising technologies can be pursued, thus ultimately facilitating broader adoption as individual instrument capabilities expand.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Depth-Resolved Lithiated Gradients in Pristine and Laser-Ablated Anodes During Fast Charging

Laser ablating 3D electrode microstructures is a technique to improve Li-ion battery fast-charge performance. This technique has been theoretically proposed and electrochemically validated previously in the literature. The fundamental principle underlying laser ablation is that the ablated features reduce Li-ion transport pathways, improving access to the electrode active material near the current collector. This, in turn, promotes more homogeneous electrode utilization. The present study seeks to directly affirm the physics attributed to laser ablation using operando high-speed synchrotron X-ray diffraction. In this study, depth-resolved graphite lithiation gradients are measured operando during high-rate (15 min) charging. The depth-resolved lithiation dynamics of both ablated and non-ablated anodes are compared. The results highlight that the laser-ablated graphite electrode has notably more homogeneous utilization as compared to the non-ablated electrode. Additionally, the ablated electrode has a significant delay in reaching the maximum graphite lithiation at the separator, indicating less propensity for lithium plating. During low rate delithiation/discharge (2 hr), the two cells' lithiation gradients converge. Notably, a calibrated physics-based electrochemical model accurately reflects experimental findings, suggesting the potential to use pseudo-4D models not only to optimize laser ablation parameters in fast-charge capable electrodes but also to guide fast charging protocols that avoid lithium plating.

25 ENERGY STORAGE↗

The creep properties of dispersion-strengthened silver-gallium oxide alloys.

Steady-state creep rates were measured for two preparations of a dispersion-strengthened alloy of silver with 1 mol % gallium oxide. One preparation, an internally-oxidized type, had a grain size 40 times that of the other preparation, which was a consolidated-powder type of alloy. The temperature and stress dependence of the steady-state creep rate differs widely for the two alloys and must be attributed to the difference in grain size. The activation energy for steady-state creep of the internally-oxidized coarse grained material is near that for self-diffusion of silver, which strongly indicates a creep process controlled by dislocation climb.

Lenel, F. V.↗

Aspects of the mechanisms of smoke generation by burning materials

An investigation of smoke generation during the burning of natural and synthetic solid materials (relevant to fire safety problems), under simulated fire conditions, is presented. Smoke formation mechanisms, including flaming and nonflaming combustion, are reviewed, and the complex physical, chemical, and electrical processes, important in smoke particulate production, are identified. With reference to the smoke formation mechanisms, measured experimental data are discussed, and include effects of ventilation gas temperature, dependence on material composition, and chemical analysis of smoke particulates. Significant differences in smoke characteristics are observed between flaming and nonflaming conditions, which is attributed to specific differences in controlling mechanisms and resultant ways leading to particulate formation. The effects of polymer substrate properties and effects of additives for a given substrate on smoke properties are also discussed in terms of basic processes. It is shown that many of the measured trends can be interpreted by considering postulated mechanisms of particulate formation.

Bankston, C. P.↗

The Apollo 16 regolith - Comparative petrology of the greater than 20 micron and 20-10 micron soil fractions, lateral transport and differential volatilization

The present investigation is concerned with questions regarding a preferential transport of finer-grained material on the lunar surface. Attention is also given to a possible appearance of volatization effects in the case of fine-grained glass beads. It is found that preferential lateral transport of fine-grained material is not efficient over the distances required to introduce mare material into the Apollo-16 (A-16) lunar highlands. The presence of granitic glasses found in the 20-10 micron fractions is attributed to comminution of mesostasis. The composition of mesostasis and the silica-rich phases contained within it reported by other investigators supports this conclusion. No evidence could be found of increased volatilization in the finer grained samples.

Kempa, M. J.↗

Volcanism, global catastrophe and mass mortality

The effects of very large volcanic eruptions are well documented in many studies, mostly based on observations made on three historic eruptions, Laki 1783; Tambora 1815 and Krakatau 1883. Such eruptions have effects that are catastrophic locally and measurable globally, but it is not clear that even the largest volcanic eruptions have had global catastrophic effects, nor caused mass extinctions. Two different types of volcanic eruption were considered as likely to have the most serious widespread effects: large silicic explosive eruptions producing hundreds or thousands of cubic kilometers of pyroclastic materials, and effusive basaltic eruptions producing of approximately 100 cubic kilometers of lava. In both cases, the global effects are climatic, and attributable to production of stratospheric aerosols. Other possibilities need to be explored. Recent research on global change has emphasized the extreme sensitivity of the links between oceanic circulation, atmospheric circulation and climate. In particular, it was argued that the pattern of ocean current circulation (which strongly influences climate) is unstable; it may rapidly flip from one pattern to a different one, with global climatic consequences. If volcanism has been a factor in global environmental change and a cause of mass extinctions, it seems most likely that it has done so by providing a trigger to other processes, for example by driving oceanic circulation from one mode to another.

Francis, P. W.↗

More shock recovery experiments on mesosiderite analogs

Mesosiderites, a small but unique group of stony-iron meteorites with affinities to howardites, eucrites, and pallasites, remain enigmatic in terms of their petrogenesis. They are composed of approximately equal weight proportions of Fe-Ni metal plus troilite and gabbroic, basaltic, and orthopyroxenitic materials. The metal and silicates, which display variable grain sizes and shapes, are delicately intermingled, forming irregular grain boundaries that have been attributed to a wide range of origins from subsolidus metamorphism to supersolidus igneous processes. Perhaps the most relevant question regarding the petrogenesis of mesosiderites is: what is the source and duration of heating that could produce the unequilibrated textures and chemistry of these meteorites? A leading candidate appears to be impacts of metallic core fragments with a differentiated asteroidal surface. This provides not only a suitable source of heat, but also the metal component uniquely required by mesosiderites. A series of shock recovery experiments on mesosiderite analogs has been continued. Textural and chemical similarities have been found that support an impact-derived origin for these unusual meteorites.

Rowan, L. R.↗

Mapping target signatures via partial unmixing of AVIRIS data

A complete spectral unmixing of a complicated AVIRIS scene may not always be possible or even desired. High quality data of spectrally complex areas are very high dimensional and are consequently difficult to fully unravel. Partial unmixing provides a method of solving only that fraction of the data inversion problem that directly relates to the specific goals of the investigation. Many applications of imaging spectrometry can be cast in the form of the following question: 'Are my target signatures present in the scene, and if so, how much of each target material is present in each pixel?' This is a partial unmixing problem. The number of unmixing endmembers is one greater than the number of spectrally defined target materials. The one additional endmember can be thought of as the composite of all the other scene materials, or 'everything else'. Several workers have proposed partial unmixing schemes for imaging spectrometry data, but each has significant limitations for operational application. The low probability detection methods described by Farrand and Harsanyi and the foreground-background method of Smith et al are both examples of such partial unmixing strategies. The new method presented here builds on these innovative analysis concepts, combining their different positive attributes while attempting to circumvent their limitations. This new method partially unmixes AVIRIS data, mapping apparent target abundances, in the presence of an arbitrary and unknown spectrally mixed background. It permits the target materials to be present in abundances that drive significant portions of the scene covariance. Furthermore it does not require a priori knowledge of the background material spectral signatures. The challenge is to find the proper projection of the data that hides the background variance while simultaneously maximizing the variance amongst the targets.

Boardman, Joseph W.↗

Progress In Magnetized Target Fusion Driven by Plasma Liners

Magnetized target fusion (MTF) attempts to combine the favorable attributes of magnetic confinement fusion (MCF) for energy confinement with the attributes of inertial confinement fusion (ICF) for efficient compression heating and wall-free containment of the fusing plasma. It uses a material liner to compress and contain a magnetized plasma. For practical applications, standoff drivers to deliver the imploding momentum flux to the target plasma remotely are required. Spherically converging plasma jets have been proposed as standoff drivers for this purpose. The concept involves the dynamic formation of a spherical plasma liner by the merging of plasma jets, and the use of the liner so formed to compress a spheromak or a field reversed configuration (FRC).

Thio, Francis Y. C.↗

Magnetized Target Fusion Driven by Plasma Liners

Magnetized target fusion (MTF) attempts to combine the favorable attributes of magnetic confinement fusion (MCF) for energy confinement with the attributes of inertial confinement fusion (ICF) for efficient compression heating and wall-free containment of the fusing plasma. It uses a material liner to compress and contain a magnetized plasma. For practical applications, standoff drivers to deliver the imploding momentum flux to the target plasma remotely are required. Spherically converging plasma jets have been proposed as standoff drivers for this purpose. The concept involves the dynamic formation of a spherical plasma liner by the merging of plasma jets, and the use of the liner so formed to compress a spheromak or a field reversed configuration (FRC). For the successful implementation of the scheme, plasma jets of the requisite momentum flux density need to be produced. Their transport over sufficiently large distances (a few meters) needs to be assured. When they collide and merge into a liner, relative differences in velocity, density and temperature of the jets could give rise to instabilities in the development of the liner. Variation in the jet properties must be controlled to ensure that the growth rate of the instabilities are not significant over the time scale of the liner formation before engaging with the target plasma. On impact with the target plasma, some plasma interpenetration might occur between the liner and the target. The operating parameter space needs to be identified to ensure that a reasonably robust and conducting contact surface is formed between the liner and the target. A mismatch in the "impedance" between the liner and the target plasma could give rise to undesirable shock heating of the liner leading to increased entropy (thermal losses) in the liner. Any irregularities in the liner will accentuate the Rayleigh-Taylor instabilities during the compression of the target plasma by the liner.

Thio, Y. C. Francis↗

Stardust Abundance Variations among Interplanetary Dust Particles

Presolar grain abundances reflect the degree of processing primitive materials have experienced. This is evidenced by the wide range of silicate stardust abundances among primitive meteorites (~10 to 300 ppm) [1], attributable to parent body hydrothermal processing. Stardust abundance variations are also pronounced in anhydrous interplanetary dust particles (CPIDPs), that have not experienced parent body processing (300 to > 10,000 ppm) [2-4]. The large range in stardust abundances among CP IDPs thus reflect nebular processing. Here we present results of a systematic search for stardust among cluster CP IDPs. Our goals are to establish mineralogical trends among IDPs with different stardust abundances. This may shed light into the nature of isotopically normal presolar grains (GEMS grains?; 5) if their abundances vary similarly to that of isotopically exotic stardust grains.

Messenger, S.↗

Enabling high areal capacity for Co-free high voltage spinel materials in next-generation Li-ion batteries

The rapidly growing technological demand for lithium-ion batteries has prompted the development of novel cathode materials with high energy density, low cost, and improved safety. High voltage spinel, LiNi 0.5 Mn 1.5 O 4 (LNMO), is one of the most promising candidates yet to be commercialized. The two primary obstacles for this material are the inferior electronic conductivity and fast capacity degradation in full cells due to the high operating voltage. By systematically addressing these limitations, we successfully develop a thick LNMO electrode with areal capacity loadings up to 3 mAh·cm –2 . The optimized thick electrode is paired with a commercial graphite anode at both the coin cell and pouch cell level, achieving a full cell capacity retention as high as 72% and 78%, respectively, after 300 cycles. We attribute this superior cycling stability to careful optimizations of cell components and testing conditions, with a specific focus improving electronic conductivity and high voltage compatibility. These results suggest precise control of materials quality, electrode architecture and electrolyte optimization can soon support the development of a cobalt-free battery system based on a thick LNMO cathode (>4 mAh·cm 2 ), which will eventually meet the needs of next-generation Li-ion batteries with reduced cost, improved safety, and assured sustainability.

25 ENERGY STORAGE↗

Multiband Fermi surface in $1T–$$\mathrm{VSe_2}$ and its implication for the charge density wave phase

Angle-resolved photoemission spectroscopy experiments reveal a surprisingly richer surface electronic structure in $1T–$$\mathrm{VSe_2}$ than previously predicted or probed. Earlier claims supporting a charge density wave phase in this material are reexamined in terms of these findings and are found to be untenable. Here, the Fermi surface is found to be gapless, while band warping effects, currently attributed to three-dimensional lattice distortion, result from the simultaneous dispersion of the closely lying multiple bands. Based on these findings, a charge density wave scenario in $1T–$$\mathrm{VSe_2}$ is unlikely. On the other side, the presence of multiple states crossing the Fermi level should constitute relevant constraints for any viable microscopic model of the structural phase transition of $\mathrm{VSe_2}$.

36 MATERIALS SCIENCE↗

SQMS Nanofabrication Taskforce: Towards Fabrication of High Coherence Superconducting Qubits

SQMS Nanofabrication Taskforce, which brings together experts in nanofabrication and materials science at the SQMS Center, has been launched to implement novel materials, substrates, and fabrication techniques for high coherence superconducting quantum devices. In a first coordinated effort, the Nanofabrication Taskforce developed fabrication processes to eliminate the lossy materials at surfaces and interfaces of superconducting qubits to enhance qubit coherence. The initial results of this study demonstrated T1 enhancement by almost an order of magnitude with best T1 s reaching ~ 600 $\mu$s. [1] We attribute this improvement to the replacement of lossy native Nb oxide layer with native Ta oxide, which is thinner and less disordered. we are now currently working on strategies with an aim towards moving qubit coherence times to millisecond timescales and beyond. The results of a systematic study will be presented to address substrate preparation, alternative materials as low loss platforms (Nb, Ta, and Re), novel non-oxide forming low loss capping layers such as proximitized Au, optimized qubit designs, and optimized Josephson junction materials, processing, and design.

Bal, Mustafa↗