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At least 325 records · Page 18

Experimental studies of crystal-melt differentiation in planetary basalt compositions

An important process that controls the evolution of magmas on and within planetary bodies is crystal-melt differentiation. Experimental studies of silicate melt solidification were performed on several planetary and terrestrial melt compositions, and experiments on one of these compositions in the microgravity environment of the space station would provide an opportunity to understand the factors that control crystal growth and crystal-melt exchange processes at crystal-melt interfaces during solidification. Experimental requirements are presented.

Grove, T. L.↗

Coarse-Grained Simulations of Polyrotaxane Hydrogels under Quiescent and Shear Conditions

Cyclodextrin-based polyrotaxanes (PR) form hydrogels in water through cyclodextrin (CD) aggregation and crystallization. These networks can break under shear flows, making them versatile platforms for extrusion-based 3D printing. To optimize the material properties of 3D-printed PR gels, a microscopic understanding of the structural evolution during 3D printing is necessary. Here, we employ coarse-grained (CG) simulations to reveal the PR assembly process at the molecular level. Our simulations reproduce the experimental crystal morphologies of PR at varying concentrations and chain lengths under quiescent conditions. Using nonequilibrium simulations, we show shear flow ruptures crystalline domain connectivity in PR gels and stacks the lamellae in the gradient direction, allowing the materials to flow during 3D printing. After the cessation of flow, the anisotropic crystal alignment and absence of available dangling PR diminish the intercrystal connectivity. The printed materials are therefore mechanically weaker than the pristine hydrogels, in agreement with experimental results. Nonetheless, by relating the microscopic structural evolution with viscoelastic properties of PR gels and solutions, we elucidate how flow conditions and sample composition affect the 3D printing performance of PR hydrogels.

Smith, Cameron D. [Dartmouth College, Hanover, NH ↗

Isothermal evaporation of a-pinene ozonolysis SOA: volatility, phase state, and oligomeric composition

We present measurements of the isothermal evaporation of a-pinene ozonolysis secondary organic aerosol (SOA). Using a novel, filter-based method, we replicate previous findings of the volume fraction remaining, presented here as carbon number weighted signal fraction remaining (SFR), as a function of evaporation time. We apply two detailed physical models to interpret the evaporative behavior of both the bulk SOA and individual components. Both models find that a combination of effectively non-volatile products, together with reversible oligomers (or otherwise reactive monomers) having a decomposition lifetime of 9 to 28 hours, best explains the evolution of composition and volatility as particles age in the absence of both organic vapors and oxidants, even under an assumption of relatively viscous (soft wax-like) particles. We find that the residence time in the SOA formation chamber, and time spent undergoing isothermal evaporation, both indicative of the physical age of the aerosol, are the most important experimental parameter determining the evaporation rate. The evolution of volatility observed in these experiments is compared to field measurements in a boreal forest site. The ambient monoterpene-dominated SOA volatility is only reproduced in the laboratory after 24 hours of extended aging in a dilute, dark, oxidant-free environment.

D'Ambro, Emma↗

Pinatubo Aerosol Evolution: Using Composite Data Sets to Build the Global- To Micro-Scale Picture and Assess Consistency of Different Measurements

This paper brings together experimental evidence required to build realistic models of the global evolution of physical, chemical, and optical properties of the aerosol resulting from the 1991 Pinatubo volcanic eruption. Such models are needed to compute the effects of the aerosol on atmospheric chemistry, dynamics, radiation, and temperature. Whereas there is now a large and crowing body of post-Pinatubo measurements by a variety of techniques, some results are in conflict, and a self-consistent, unified picture is needed, along with an assessment of remaining uncertainties. This paper examines, data from photometers, radiometers, impactors, optical counter/sizers, and lidars operated on the ground, aircraft, balloons, and spacecraft. Example data sources include: (1) Tracking sunphotometers and lidars at Mauna Loa Observatory (MLO) and on the DC-8. (2) Particle spectrometers and wire impactors on the ER-2 and DC-8. (3) Dustsondes (particle counter/sizers on balloons). and (3) SAGE II, SAM II, AVHRR, CLAES, and ISAMS sensors on a variety of satellites. We assess the mutual consistency of these disparate data sets and recommend 'consensus' properties and uncertainties in the process of developing a composite data set. Recommended properties include the spatial and temporal evolution of particle chemical composition, shape, wavelength-and temperature-dependent refractive index, size distribution, and optical depth spectra. Supporting references are cited and representative data shown.

Russell, Philip B.↗

Pinatubo Aerosol Evolution: Using Composite Data Sets to Build the Global- to Micro-Scale Picture and Assess Consistency of Different Measurements

This paper brings together experimental evidence required to build realistic models of the global evolution of physical, chemical, and optical properties of the aerosol resulting from the 1991 Pinatubo volcanic eruption. Such models are needed to compute the effects of the aerosol on atmospheric chemistry, dynamics, radiation, and temperature. Whereas there is now a large and growing body of post-Pinatubo measurements by a variety of techniques, some results are in conflict, and a self-consistent, unified picture is needed, along with an assessment of remaining uncertainties. This paper examines data from photometers, radiometers, impactors, optical counters/sizers, and lidars operated on the ground, aircraft, balloons, and spacecraft. Example data sources include: - Tracking sunphotometers and lidars at Mauna Loa Observatory (MLO) and on the DC-8 - Particle spectrometers and wire impactors on the ER-2 and DC-8 - Dustsondes (particle counters/sizers on balloons) - SAGE II, SAM II, AVHRR, CLAES, and ISAMS sensors on a variety of satellites. We assess the mutual consistency of these disparate data sets and recommend 'consensus" properties and uncertainties in the process of developing a composite data set. Recommended properties include the spatial and temporal evolution of particle chemical composition, shape, wavelength and temperature-dependent refractive index, size distribution, and optical depth spectra. Supporting references are cited and representative data shown.

Russell, P. B.↗

Dichotomous Temperature Response in the Electronic Structure of Epitaxially Grown Altermagnet MnTe

The altermagnet candidate MnTe has recently gained significant interest due to its unconventional magnetic ordering. One of the key features of altermagnetism is the momentum-dependent spin-split band and its temperaturedependent evolution. Yet a fully momentum-resolved experimental investigation, including out-of-plane direction, is still lacking. Here, we systematically investigate the electronic structure of epitaxially grown MnTe by using angle-resolved photoemission spectroscopy (ARPES). Our photon-energy-dependent ARPES data reveal significant out-of-plane dispersions consistent with previous theoretical calculations. More interestingly, we identify two distinct temperature-dependent electronic band structure evolutions at different out-of-plane momentum positions: momentum-dependent energy shifts at the nodal plane and substantial spectral weight suppression at the off-nodal plane. These findings may suggest the importance of considering both the itinerant and localized nature of the magnetic ordering and momentum-dependent interactions. Our work provides crucial insights into the complex correlation between momentum, temperature, and electronic structure in MnTe, contributing to a deeper understanding of altermagnetism.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Iron isotope fractionation between solid and liquid metal in the Fe-P±Ni system: Experimental constraints and implications for meteorites

Iron meteorites record a range of Fe isotope compositions that hold valuable information regarding the evolution of their parent bodies. Interpreting this isotopic variability, however, requires experimental constraints on the equilibrium isotope fractionation between phases. It is thought that the cores of many iron meteorite parent bodies experienced fractional crystallization, during which crystallization of solid iron-nickel occurs from an increasingly non-metal-rich liquid alloy. Phosphorus is one component of this alloy, and this study provides the first constraints on Fe-isotope fractionation between solid and liquid alloys in the Fe-Ni-P system. Experiments comprising Fe and P show a clear enrichment in the light isotopes of Fe in the liquid phase, which increases with the amount of phosphorus. Nickel-bearing samples are offset from the trend defined by Ni-free experiments, which is accounted for by the change in the solid alloy phase from a body-centered cubic to face-centered cubic structure upon the addition of Ni. The increasing light isotope enrichment of the liquid with increasing P content suggests interstitial solution of P, which is known to lengthen Fe-Fe bonds in Fe-P liquids (Waseda and Shiraishi 1977). Results suggest a negligible effect of P on Fe isotope fractionation during planetesimal core crystallization. Iron isotopes may, however, prove useful for identifying the petrogenesis of schreibersite in pallasites and iron meteorites.

58 GEOSCIENCES↗

Evolution of hairpin vortices in a shear flow

Recent experimental studies suggest that the hairpin vortex plays an important (and perhaps dominant) role in the dynamics of turbulent flows near walls. In this study a numerical procedure is developed to allow the accurate computation of the trajectory of a 3-D vortex having a small core radius. For hairpin vortices which are convected in a shear flow above a wall, the calculated results show that a 2-D vortex containing a small 3-D disturbance distorts into a complex shape with subsidiary hairpin vortices forming outboard of the original hairpin vortex. As the vortex moves above the wall, it induces unsteady motion in the viscous flow near the wall: numerical solutions suggest that the boundary-layer flow near the wall will ultimately erupt in response to the motion of the hairpin vortex and in the process a secondary hairpin vortex will be created. The computer results agree with recent experimental investigations.

Hon, T.-L.↗

Evolution of hairpin vortices in a shear flow

Recent experimental studies suggest that the hairpin vortex plays an important (and perhaps dominant) role in the dynamics of turbulent flows near walls. In this study, a numerical procedure is developed to allow the accurate computation of the trajectory of a 3D vortex having a small core radius. For hairpin vortices which are convected in a shear flow above a wall, the calculated results show that a 2D vortex containing a small 3D disturbance distorts into a complex shape with subsidiary hairpin vortices forming outboard of the original hairpin vortex. As the vortex moves above the wall, it induces unsteady motion in the viscous flow near the wall: numerical solutions suggest that the boundary-layer flow near the wall will ultimately erupt in response to the motion of the hairpin vortex and in the process a secondary hairpin vortex will be created. The computer results agree with recent experimental investigations.

Hon, T.-L.↗

Transition Metal Arsenide Catalysts for the Hydrogen Evolution Reaction

We report, to our knowledge for the first time, a combined experimental and density functional theory (DFT) investigation into the activity and stability of cobalt, molybdenum, and copper arsenides as catalysts for the hydrogen evolution reaction (HER). We find CoAs and MoAs to be the most active arsenide materials. We discuss the trends between calculated surface vacancy formation energies and catalyst stability. Using a simple thermodynamic model of HER activity, we find consistent trends between hydrogen binding free energy and the experimentally observed activity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Evolution of a localized thermal explosion in a reactive gas

Experimental observations of ignition in premixed gaseous reactants indicate that perfectly homogeneous initiation is practically unrealizable. Instead, combustion first sets in, as a rule, at small, discrete sites where inherent inhomogeneities cause chemical activity to proceed preferentially and lead to localized explosions. Combustion waves propagating away from these hot spots or reaction centers eventually envelop the remaining bulk. This study examines the spatial structure and temporal evolution of a hot spot for a model involving Arrhenius kinetics. The hot spot, characterized by peaks in pressure and temperature with little diminution in local density, is shown to have one of two possible self-similar structures. The analysis employs a combination of asymptotics and numerics, and terminates when pressure and temperature in the explosion have peaked.

Jackson, T. L.↗

Lifetimes of low-lying excited states in Kr 50 36 86

Background: The evolution of nuclear magic numbers at extremes of isospin is a topic at the forefront of contemporary nuclear physics. N = 50 is a prime example, with increasing experimental data coming to light on potentially doubly magic Sn 100 and Ni 78 at the proton-rich and proton-deficient extremes, respectively; however, experimental discrepancies exist in the data for less exotic systems. Purpose: In Kr 86 the B ( E 2 ; 2 1 + → 0 1 + ) value—a key indicator of shell evolution—has been experimentally determined by two different methodologies, with the results deviating by 3 σ . Here, we report on a new high-precision measurement of this value, as well as the first measured lifetimes and hence transition strengths for the 2 2 + and 3 ( 2 ) - states in the nucleus. Methods: The Doppler-shift attenuation method was implemented using the TRIUMF-ISAC γ -ray escape-suppressed spectrometer (TIGRESS) γ -ray spectrometer and the TIGRESS integrated plunger device. High-statistics Monte Carlo simulations were utilized to extract lifetimes in accordance with state-of-the-art methodologies. Results: Lifetimes of τ ( 2 1 + ) = 336 ± 4 (stat.) ± 20 (sys.) fs, τ ( 2 2 + ) = 263 ± 9 (stat.) ± 19 (sys.) fs, and τ ( 3 ( 2 ) - ) = 73 ± 6 (stat.) ± 32 (sys.) fs were extracted. This yields a transition strength for the first-excited state of B ( E 2 ; 2 1 + → 0 1 + ) = 259 ± 3 (stat.) ± 16 (sys.) e 2 fm 4 . Conclusions: Finally, the measured lifetime disagrees with the previous Doppler-shift attenuation method measurement by more than 3 σ , while agreeing well with a previous value extracted from Coulomb excitation. The newly extracted B ( E 2 ; 2 1 + → 0 1 + ) value indicates a more significant reduction in the N = 50 isotones approaching Z = 40 .

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Experimental Insights into the Geochemistry of Mercury

With the recent estimate of Mercury's surface composition from the X-Ray Spectrometer and Gamma-Ray Spectrometer that were onboard NASA's MErcury Surface, Space ENvironment, Geochemistry and Ranging (MESSENGER) spacecraft, we now have our first opportunity to directly investigate the compositions of lavas from the planet Mercury and indirectly investigate the chemical make-up of its interior. Results from MESSENGER showed exotic surface compositions with more than 3 wt% sulfur in some lavas and relatively low amounts of iron (less than 3 wt%) across the surface. These striking features are consistent with magmatism occurring under highly reducing conditions which has an impact on the thermal and chemical evolution of a planetary body. Here we'll explore the geochemical evolution of Mercury through a series of experimental studies and discuss the implications of low oxygen fugacity on elemental behavior and magmatic processes.

Vander Kaaden, Kathleen E.↗

Time-dependent experimental identification of inter-ELM microtearing modes in the tokamak edge on DIII-D

In a series of discharges on the DIII-D tokamak, fast vertical plasma jogs are used to induce current perturbations in the steep gradient region of the H-mode edge. These current perturbations directly influence the edge q profile, decoupling the resonant location and instability drive of pedestal-localized microtearing modes (MTMs.) By exploiting this effect, we develop and apply a new experimental technique to track the dynamical frequency evolution of MTMs in the pedestal region, providing a compelling validation of the MTM model. The frequency of potential MTMs is calculated as the Doppler-shifted electron diamagnetic frequency at rational q=m/n surfaces, showing remarkable agreement with chirped frequency behavior of n=3, 4 and 5 modes detected with fast magnetics. Data is collected throughout multiple ELM cycles in order to build robust statistics describing the time-dependent frequency evolution of MTMs, which can be explained by examining the recovery of pedestal gradients after an ELM event. MTMs have a dominant transport contribution in the electron thermal channel, so the presented results indicate that reduced models of pedestal transport must be electromagnetic in nature and constructed with accurate calculations of MTM stability; inclusion of this physics is essential for accurate predictions of the electron temperature pedestal profile. Supporting measurements of mode saturation, propagation direction and transport fingerprints are made to support the dynamic frequency determination, unambiguously and experimentally identifying MTMs in the pedestal region of DIII-D.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

A parameterized model for the evolution of isotopic heterogeneities in a convecting system

It is experimentally shown that, although steady convective flows are efficient means to heterogeneity within a single cell, they do not produce a dispersal of heterogeneous material over scales that are large by comparison to their depth, which requires that the flow be time-dependent on a time scale comparable to the overturn time. Convection in an internally heated layer does possess this property, and numerical solutions are presently used to study the way in which it disperses a set of neutrally bouyant particles initially confined to a small space. The derived concept of effective diffusivity is applied to the isotopic evolution of the Sm-Nd and Rb-Sr systems, with spatial variations generated by horizontal variations in degree of melting 1.8 billion years ago.

Richter, F. M.↗

Edge reactivity and water-assisted dissociation on cobalt oxide nanoislands

Here, transition metal oxides show great promise as Earth-abundant catalysts for the oxygen evolution reaction in electrochemical water splitting. However, progress in the development of highly active oxide nanostructures is hampered by a lack of knowledge of the location and nature of the active sites. Here we show, through atom-resolved scanning tunnelling microscopy, X-ray spectroscopy and computational modelling, how hydroxyls form from water dissociation at under coordinated cobalt edge sites of cobalt oxide nanoislands. Surprisingly, we find that an additional water molecule acts to promote all the elementary steps of the dissociation process and subsequent hydrogen migration, revealing the important assisting role of a water molecule in its own dissociation process on a metal oxide. Inspired by the experimental findings, we theoretically model the oxygen evolution reaction activity of cobalt oxide nanoislands and show that the nanoparticle metal edges also display favourable adsorption energetics for water oxidation under electrochemical conditions.

36 MATERIALS SCIENCE↗

Periodic Excitation for Jet Vectoring and Enhanced Spreading

The effects of periodic excitation on the evolution of a turbulent jet were studied experimentally. A short, wide-angle diffuser was attached to the jet exit and excitation was introduced at the junction between the jet exit and the diffuser inlet. The introduction of high amplitude periodic excitation at the jet exit enhances the mixing and promotes attachment of the jet shear-layer to the diffuser wall. Vectoring is achieved by applying the excitation over a fraction of the circumference of the circular jet, enhancing its spreading rate on the excited side and its tendency to reattach to that side. Static deflection studies demonstrate that the presence of the wide-angle diffuser increases the effectiveness of the added periodic momentum due to a favorable interaction between the excitation, the jet shear-layer and the diffuser wall. This point was further demonstrated by the evolution of a wave packet that was excited in the jet shear-layer. Strong amplification of the wave packet was measured with a diffuser attached to the jet exit. The turbulent jet responds quickly (10-20 msec) to step changes in the level of the excitation input. The response scales with the jet exit velocity and is independent of the Reynolds number. Jet deflection angles were found to be highly sensitive to the relative direction between the excitation and the jet flow and less sensitive to the excitation frequency. The higher jet deflection angles were obtained for a diffuser length of about two diameters and for diffusers with half-angles greater than 15 degrees.

Pack, LaTunia G.↗