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At least 1,351 records · Page 75

Influence of counterion substitution on the properties of imidazolium-based ionic liquid clusters

Due to their unique physiochemical properties that may be tailored for specific purposes, ionic liquids (ILs) have been investigated for various applications, including chemical separations, catalysis, energy storage, and space propulsion. The different cations and anions comprising ILs may be selected to optimize a range of desired properties, such as thermal stability, ionic conductivity, and volatility, leading to the designation of certain ILs as designer “green” solvents. The effect of counterions on the properties of ILs is of both fundamental scientific interest and technological importance. Herein, we report a systematic experimental and theoretical investigation of the size, charge, stability toward dissociation, and geometric/electronic structure of 1-ethyl-3-methyl imidazolium (EMIM)-based IL clusters containing two different atomic counterions (i.e., bromide [Br − ] and iodide [I − ]). This work extends our studies of EMIM + cations with atomic chloride (Cl − ) and molecular tetrafluoroborate (BF 4 − ) anions reported previously by Baxter et al. [Chem. Mater. 34, 2612 (2022)] and Zhang et al . [J. Phys. Chem. Lett. 11, 6844 (2020)], respectively. Distributions of anionic IL clusters were generated in the gas phase using electrospray ionization and characterized by high mass resolution mass spectrometry, energy-resolved collision-induced dissociation, and negative ion photoelectron spectroscopy experiments. The experimental results reveal anion-dependent trends in the size distribution, relative abundance, ionic charge state, stability toward dissociation, and electron binding energies of the IL clusters. Complementary global optimization theory provides molecular-level insights into the bonding and electronic structure of a selected subset of clusters, including their low energy structures and electrostatic potential maps, and how these fundamental characteristics are influenced by anion substitution. Collectively, our findings demonstrate how the fundamental properties of ILs, which determine their suitability for many applications, may be tuned by substituting counterions. These observations are critical in the sub-nanometer cluster size regime where phenomena do not scale predictably to the bulk phase, and each atom counts toward determining behavior.

cluster↗

Automated imaging of the annihilation of a transverse domain wall in patterned magnetic thin films

Imaging the magnetic domain wall behavior in patterned thin films under external stimuli can enable understanding the underlying energy landscape and the role of local microstructure and defects. We present an automated workflow for in situ Lorentz transmission electron microscopy to image magnetic domain walls at the nanometer length scale and at a time resolution in the sub-millisecond regime—the latter of which is limited by the speed of the available camera. Our workflow is modular and can be broadly applied to various types of in situ experiments, taking us a step closer to the future of autonomous imaging of nanomagnetic films with electron microscopy. Using our workflow, we show the transformation of a transverse domain wall with sub-millisecond time resolution under the application of an in situ transverse magnetic field, a study of whose dynamics are essential in the design of future domain wall mediated spintronic device applications.

Algebraic topology↗

FLASH-therapy suitable single-pulse proton generation using TiH 2 under nanosecond laser irradiation

We investigated proton emission from titanium hydride (TiH 2 ) targets irradiated in vacuum by a 6-ns, 1064-nm Nd:YAG laser. Time-of-flight measurements with a Faraday cup and an electrostatic ion analyzer resolved distinct proton peaks at high pulse energies, with yields on the order of 10 9 protons per shot. Systematic scans over pulse energy and up to 1000 repeated shots showed that, while the peak amplitude gradually decreased, the integrated proton number remained nearly constant. This behavior is consistent with surface-induced broadening of the plasma expansion while bulk hydrogen is replenished by diffusion and repeated ablation of fresh TiH 2 layers. Using the measured proton numbers and pulse widths, a simple direct-plasma-injection-style scaling indicates peak currents of ∼100 mA and sub-microsecond pulse durations. The pulse structure and yield satisfy key ultra-high-dose-rate criteria and, together with sustained output over 1000 shots, support TiH 2 -based laser ion sources as practical candidates for FLASH-therapy (ultra-high-dose-rate)-oriented studies and injector development using direct plasma injection.

43 PARTICLE ACCELERATORS↗

H 0 without the sound horizon (or supernovae): A 2% measurement in DESI DR1

The sound horizon scale rs is a key source of information for measurements of H 0 from early-time data, and is therefore a common target of new physics proposed to solve the Hubble tension. We present a sub-2% measurement of the Hubble constant that is independent of this scale, using data from the first data release of the Dark Energy Spectroscopic Instrument (DESI DR1). Building on previous work, we remove dependency on the sound horizon size using a heuristic rescaling procedure at the power spectrum level. A key innovation is the inclusion of uncalibrated (agnostic to r s ) post-reconstruction BAO measurements from DESI DR1, as well as using the CMB acoustic scale θ* as a high-redshift anchor. Uncalibrated type-Ia supernovae are often included as an independent source of Ω m information; here we demonstrate the robustness of our results by additionally considering two supernova-independent alternative datasets. We find somewhat higher values of H 0 relative to our previous work: 69.2 +1.3 -1.4 , 70.3 +1.4 -1.2 , and 69.6 +1.3 -1.8 km s -1 Mpc -1 respectively when including measurements from i) Planck/ACT CMB lensing × unWISE galaxies, ii) the DES Year 3 6×2pt analysis, and iii) Planck/ACT CMB lensing + the DES Year 5 supernova analysis. These remarkably consistent constraints achieve better than 2% precision; they are among the most stringent sound horizon-independent measurements from LSS to date, and provide a powerful avenue for probing the origin of the Hubble tension.

79 ASTRONOMY AND ASTROPHYSICS↗

Image Quality on the KAO

Three flights of the Kuiper Airborne Observatory (KAO) were taken to study the cause of the point spread function (PSF) degradation. The preliminary conclusions are: (1) the KAO point spread function decreases in size with elapsed time at altitude; (2) image motion is occasionally comparable to the size of the image, but is usually a sub-arcsecond effect; and (3) star images show small scale internal structural changes on a 200 microsecond timescale.

Dunham, E. W.↗

Mixing in a stratified shear flow: Energetics and sampling

Direct numerical simulations of the time evolution of homogeneous stably stratified shear flows have been performed for Richardson numbers from 0 to 1 and for Prandtl numbers between 0.1 and 2. The results indicate that mixing efficiency R(sub f) varies with turbulent Froude number in a manner consistent with laboratory experiments performed with Prandtl numbers of 0.7 and 700. However, unlike the laboratory results, for a particular Froude number, the simulations do not show a clear dependence on the magnitude of R(sub f) on Pr. The observed maximum value of R(sub f) is 0.25. When averaged over vertical length scales of an order of magnitude greater than either the overturning or Ozmidov scales of the flow, the simulations indicate that the dissipation rate epsilon is only weakly lognormally distributed with an intermittency of about 0.01 whereas estimated values in the ocean are 3 to 7.

Ivey, G. N.↗

Determination of cosmic bodies size-velocity distribution by observation of current impacts on Mars

Collisions of cosmic bodies with terrestrial planets involve many physical processes such as deceleration and ablation during their flight through an atmosphere, the impact at a surface accompanied by cratering, melting and evaporation of surface material, generation of shock waves, etc. If body velocity is high enough then a thermal radiation is very important. All these processes on Mars proceed differently than on the other planets because of the low density of its atmosphere. In particular, this leads to the fact that smaller bodies of sizes of the order of 0.1-10 m strike the planet surface without being decelerated and perform some effects which may be detected by equipment placed on a board of artificial satellites, by a network of stations at the surface of Mars and even from the Earth. These observations can be used to determine size-velocity distribution of such bodies in the Solar System. Numerical simulation of the impacts at the surface of Mars have been carried out using two-dimensional gas dynamic code with detailed consideration of the thermal radiative transfer. This work is an extension of our previous paper. We have expanded a range of projectile sizes up to r sub 0 = 100 m. For such a large-scale body, the initial stage of the impact, involving crate ring and ejection of surface material, is very important. Thus, these effects have been taken into account.

Nemchinov, I. V.↗

Probing the interstellar medium with pulsars on AU scales

We present a new technique, multiepoch observations of 21 cm absorption against high-velocity pulsars, to probe the properties of the cold neutral hydrogen gas (H I) in the interstellar medium (ISM) at AU scales. In three epochs, over a 1.7 yr interval, we find evidence for significant opacity variations toward all of the pulsars in our sample. Small-scale structure in the ISM is detected on a range of scales from 5 AU to 100 AU, over a wide range of distances (50-2600 pc), opacities (tau(sub max) = 0.1 - 2.5) and directions (anticenter, interarm, high latitude, and local ISM). It appears that small-scale structure is a general property of the ISM and is not confined to special lines of sight. A significant fraction (10%-15%) of the cold H I gas is in this form. These opacity variations do not show any strong correlations with such parameters as transverse distance or integrated opacity, and there is no obvious relation between these structures and those seen in the ionized phase of the ISM.

Frail, Dale A.↗

A similarity hypothesis for the two-point correlation tensor in a temporally evolving plane wake

The analysis demonstrated that the governing equations for the two-point velocity correlation tensor in the temporally evolving wake admit similarity solutions, which include the similarity solutions for the single-point moment as a special case. The resulting equations for the similarity solutions include two constants, beta and Re(sub sigma), that are ratios of three characteristic time scales of processes in the flow: a viscous time scale, a time scale characteristic of the spread rate of the flow, and a characteristic time scale of the mean strain rate. The values of these ratios depend on the initial conditions of the flow and are most likely measures of the coherent structures in the initial conditions. The occurrences of these constants in the governing equations for the similarity solutions indicates that these solutions, in general, will only be the same for two flows if these two constants are equal (and hence the coherent structures in the flows are related). The comparisons between the predictions of the similarity hypothesis and the data presented here and elsewhere indicate that the similarity solutions for the two-point correlation tensors provide a good approximation of the measures of those motions that are not significantly affected by the boundary conditions caused by the finite extent of real flows. Thus, the two-point similarity hypothesis provides a useful tool for both numerical and physical experimentalist that can be used to examine how the finite extent of real flows affect the evolution of the different scales of motion in the flow.

Ewing, D. W.↗

Subsonic and Transonic Dynamic Stability Characteristics of the X-33

Dynamic stability testing was conducted on a 2.5% scale model of the X-33 technology demonstrator sub-orbital flight-test vehicle. This testing was conducted at the NASA Langley Research Center (LaRC) l6-Foot Transonic Wind Tunnel with the LaRC High-speed Dynamic Stability system. Forced oscillation data were acquired for various configurations over a Mach number range of 0.3 to 1.15 measuring pitch, roll and yaw damping, as well as the normal force due to pitch rate and the cross derivatives. The test angle of attack range was from -2 to 24 degrees, except for those cases where load constraints limited the higher angles of attack at the higher Mach numbers. A variety of model configurations with and without control surfaces were employed, including a body alone configuration. Stable pitch damping is exhibited for the baseline configuration throughout the angle of attack range for Mach numbers 0.3, 0.8, and 1.15. Stable pitch damping is present for Mach numbers 0.9 and 0.6 with the exception of angles 2 and 16 degrees, respectively. Constant and stable roll damping were present for the baseline configuration over the range of Mach numbers up to an angle of attack of 16 degrees. The yaw damping for the baseline is somewhat stable and constant for the angle of attack range from -2 to 8 degrees, with the exception of Mach numbers 0.6 and 0.8. Yaw damping becomes highly unstable for all Mach numbers at angles of attack greater than 8 degrees.

Tomek, D.↗

The Jet/Disk Connection in AGN: Chandra and XMM-Newton Observations of Three Powerful Radio-Loud Quasars

The connection between the accretion process that powers AGN and the formation of jets is still poorly understood. Here we tackle this issue using new, deep Chandra and XMM-Newton observations of tlie cores of three powerful radio loud quasars: 1136-135, 1150+497 (Chandra), and 0723+679 (XMM-Newton), in the redshift range z=0.3-0.8. These sources are known from our previous Chandra siiapsliot survey to liave kpc-scale X-ray jets. In 1136-135 and 1150-1+497; evidence is found for the presence of diffuse thermal X-ray emission around the cores; on scales of 40-50 kpc and with luminosity L(sub 0.3-2 kev approx. 10(sup 43) erg per second, suggesting thermal emission from the host galaxy or a galaxy group. The X-ray continua of the cores in the three sources are described by an upward-curved (concave) broken power law, with photon indices GAMMA (sub soft) approx. 1.8 - 2.1 and GAMMA (sub hard) approx. 1.7 below and above approx. equal to 2 keV, respectively. There is evidence for an uiiresolved Fe K alpha line with EW approx. 70 eV in the three quasars. The Spectral Energy Distributions of the sources can be well described by a mix of jet and disk emission, with the jet dominating the radio and hard X-rays (via synchrotron and external Compton) and the disk dominating the optical/UV through soft X-rays. The ratio of the jet-to-disk powers is approx. 1, consistent with those derived for a number of gamma ray emitting blazars. This indicates that near equality of accretion and jet power may be common in powerful radio-loud AGN.

Sambruna, Rita↗

CdZnTeSe: Recent advances for radiation detector applications

The quest for cost-effective, high performing room temperature semiconductor detector (RTSD) materials for high energy gamma rays has been continuing for more than three decades. The requirements for RTSD materials, however, are more stringent as compared to other applications unrelated to detection of X- and gamma-rays, mainly due to the requirement of thick detectors for sufficient absorption of high-energy electromagnetic radiation and excellent charge-transport properties. The II-VI compound CdZnTe (CZT) with the composition of 10 atomic % Zn (Cd0.9Zn0.1Te) has been the material of choice over the past several years, and it has dominated the commercial market for RTSD materials and detectors. Despite its commercial success as a room temperature radiation detection material, CZT suffers from a lack of compositional homogeneity on both a micro- and macro-scale and the presence of high concentrations of sub-grain boundary (dislocation walls) networks and secondary phases (Te-rich inclusions). This chapter focuses on the presence of performance-limiting defects in CZT that hinder the yield and elevate the cost of high-quality detectors. The presence of such performance-limiting defects has restricted widespread deployment of CZT for a variety of potential applications, particularly for uses of relatively large detectors where the demands on material perfection are significantly greater. In the recent past, replacing some of the tellurium with selenium in the CZT matrix was found to be very effective in drastically reducing the Te-rich secondary phases and dislocation networks, plus

Roy, Utpal N.↗

Holocene paleoclimate change in the western US: The importance of chronology in discerning patterns and drivers

We report sediment in lakes and meadows forms a powerful archive that can be used to reconstruct environmental change through time. Reconstructions of lake level, of chemical, biological, and hydrological conditions, and of surrounding vegetation provide detailed information about past climate conditions, both locally and regionally. Indeed, most of our current knowledge of centennial- to millennial-scale climate variability in the arid western United States, where information about past hydroclimate is particularly important, comes from such sediment-based reconstructions. The pressing need for robust, precise predictions of future conditions is a significant motivation for paleoclimate science, and current research questions frequently require Holocene reconstructions to be resolved at sub-centennial timescales. Increasingly, regional syntheses seek to identify synoptic-scale patterns similar to those defined from modern observations (seasonal, interannual, multi-decadal, etc.) or to compare with the output of climate model simulations. However, the age control on existing records, especially those more than about 20 years old, is often sufficient only for millennial-scale interpretation. Here we assess the age control for 84 published and unpublished records from lakes and meadows in the Great Basin, California, and desert southwest, and use Bayesian modeling to evaluate the 95% uncertainty ranges for the 42 best-dated records. In the Late Holocene, about half of the 42 records have <400-year mean uncertainty ranges; however, high-precision age control is especially critical for young records, used to develop an accurate understanding of a proxy’s response to known climate variations. In the Middle Holocene, records vary from 400 to >800-year mean uncertainty and records of the Early Holocene have 600- to >1400-year mean uncertainty ranges. We find that the largest control on modeled uncertainties is dating density, with at least 2 dates/kyr being optimal and suggest obtaining “range-finder” dates at the onset of a study to better predict the total number of dates needed for an adequate age model. Such a density avoids a commonly observed phenomenon of significant peaks in uncertainty arising in gaps between age control points. Analysis of the uncertainties associated with proxy shifts reveal that more than half are >400 years. Although such large uncertainties currently prevent sub-centennial interpretations in most cases, increased dating density, strategic use of limited funds (including budgeting for a 2 date/kyr minimum at the proposal stage), construction of age-depth models with Bayesian methods, and critical evaluation of chronological uncertainty will shed light on past climate variability at finer timescales, enhancing our understanding of global and regional drivers of western U.S. climate.

54 ENVIRONMENTAL SCIENCES↗

Horizontal Variability of Water and Its Relationship to Cloud Fraction near the Tropical Tropopause: Using Aircraft Observations of Water Vapor to Improve the Representation of Grid-scale Cloud Formation in GEOS-5

Large-scale models such as GEOS-5 typically calculate grid-scale fractional cloudiness through a PDF parameterization of the sub-gridscale distribution of specific humidity. The GEOS-5 moisture routine uses a simple rectangular PDF varying in height that follows a tanh profile. While below 10 km this profile is informed by moisture information from the AIRS instrument, there is relatively little empirical basis for the profile above that level. ATTREX provides an opportunity to refine the profile using estimates of the horizontal variability of measurements of water vapor, total water and ice particles from the Global Hawk aircraft at or near the tropopause. These measurements will be compared with estimates of large-scale cloud fraction from CALIPSO and lidar retrievals from the CPL on the aircraft. We will use the variability measurements to perform studies of the sensitivity of the GEOS-5 cloud-fraction to various modifications to the PDF shape and to its vertical profile.

climate modeling↗

Planetesimal Formation in the Protoplanetary Nebula

In this talk we will address two distinct phases of planetesimal formation, each of which is fundamentally dependent upon the coupled interactions of particles and turbulent nebula gas. It has been shown both numerically and experimentally that 3-D (three dimensional) turbulence concentrates aerodynamically size-selected particles by orders of magnitude. In a previous review chapter we illustrated the initial predictions of Turbulent Concentration (TC) as applied to the solar nebula. We predicted the particle size which will be most effectively concentrated by turbulence; it is the particle which has a gas drag stopping time equal to the overturn time of the smallest (Kolmogorov scale) eddy. The primary uncertainty is the level of nebula turbulence, or Reynolds number Re, which can be expressed in terms of the standard nebula eddy viscosity parameter alpha = Rev(sub m)/cH, where v(sub m) is molecular viscosity, c is sound speed, and H is vertical scale height. Several studies, and observed lifetimes of circumstellar disks, have suggested that the level of nebula turbulence can be described by alpha = 10(exp -2) - 10(exp -4). There is some recent concern about how energy is provided to maintain this turbulence, but the issue remains open. We adopt a canonical minimum mass nebula with a range of alpha is greater than 0. We originally showed that chondrule-sized particles are selected for concentration in the terrestrial planet region if alpha = 10(exp -3) - 10(exp -4). In addition, Paque and Cuzzi found that the size distribution of chondrules is an excellent match for theoretical predictions. One then asks by what concentration factor C these particles can be concentrated; our early numerical results indicated an increase of C with alpha, and were supported by simple scaling arguments, but the extrapolation range was quite large and the predictions (C is approximately equal to 10(exp 5) - 10(exp 6) not unlikely) uncertain. The work presented here, which makes use of our recent demonstration that the particle density field is a multifractal with flow-independent properties provides a far more secure ground for such predictions. We also indicate how fine-grained dust rims on chondrules might enter into constraining the situation. Once large particles (meter-size mass equivalent) reach the midplane, perhaps in the form of dense aggregates of the sort formed in 3D turbulence, they remain stable against gravitational instability but might grow rapidly by accretion of their drifting neighbors, depending on the level of global turbulence.

Cuzzi, Jeffrey N.↗

A Study of Transport in the Near-Earth Plasma Sheet During A Substorm Using Time-Dependent Large Scale Kinetics

In this study we investigate the transport of H+ ions that made up the complex ion distribution function observed by the Geotail spacecraft at 0740 UT on November 24, 1996. This ion distribution function, observed by Geotail at approximately 20 R(sub E) downtail, was used to initialize a time-dependent large-scale kinetic (LSK) calculation of the trajectories of 75,000 ions forward in time. Time-dependent magnetic and electric fields were obtained from a global magnetohydrodynamic (MHD) simulation of the magnetosphere and its interaction with the solar wind and the interplanetary magnetic field (IMF) as observed during the interval of the observation of the distribution function. Our calculations indicate that the particles observed by Geotail were scattered across the equatorial plane by the multiple interactions with the current sheet and then convected sunward. They were energized by the dawn-dusk electric field during their transport from Geotail location and ultimately were lost at the ionospheric boundary or into the magnetopause.

El-Alaoui, M.↗

Proceedings of a Workshop on Assessment of Techniques for Measuring Tropospheric N sub x O sub y

Human impact on the troposphere, particularly on the regional to global scale is assessed. One area of required research is instrumentation development, which is aimed at improving the capability to measure important trace gases and aerosols which are key species in the major atmospheric biogeochemical cycles. To focus on specific needs, the Instrumentation Workshop for NxOy Tropospheric Species was conducted. The workshop discussed measurement needs and instrument capabilities for NxOy species, including NO, NO2, HNO3, HNO2, PAN, and NO3 aerosols. The status and measurement capabilities of various techniques (operational as well as conceptual) were discussed, along with future instrument and technology needs.

Source record↗

Turbulence, Chondrules, and Planetesimals

It has been shown both numerically and experimentally that 3-D turbulence concentrates aerodynamically size-selected particles by orders of magnitude. In a previous review chapter, in "Chondrules and the protoplanetary disk" we illustrated the initial predictions of Turbulent Concentration (TC) as applied to the solar nebula. We predicted the particle size which will be most effectively concentrated by turbulence; it is the particle which has a gas drag stopping time equal to the overturn time of the smallest (Kolmogorov scale) eddy. The primary uncertainty is the level of nebula turbulence, or Reynolds number Re, which can be expressed in terms of the standard nebula eddy viscosity parameter alpha = Re(nu)(sub m)/cH, where nu(sub m) is molecular viscosity, c is sound speed, and H is vertical scale height. Several studies, and observed lifetimes of circumstellar disks, have suggested that the level of nebula turbulence can be described by alpha = 10(exp -2) - 10(exp -4). There is some recent concern about how energy is provided to maintain this turbulence, but the issue remains open. We adopt a canonical minimum mass nebula with a range of alpha > 0. We originally showed that chondrule-sized particles are selected for concentration in the terrestrial planet region if alpha = 10(exp -3) - 10(exp -4). In addition, Paque and Cuzzi found that the size distribution of chondrules is an excellent match for theoretical predictions. One then asks by what concentration factor C these particles can be concentrated; our early numerical results indicated an increase of C with alpha, and were supported by simple scaling arguments, but the extrapolation range was quite large and the predictions (C ~ 10(exp 5) - 10(exp 6) not unlikely) uncertain. The work presented here, which makes use of our recent demonstration that the particle density field is a multifractal with flow-independent properties provides a far more secure ground for such predictions. We also indicate how fine-grained dust rims on chondrules might enter into constraining the situation.

Cuzzi, Jeffrey↗