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At least 667 records · Page 37

Comment on 'A non-mass-dependent isotopic fractionation effect' by F. Robert, J. Halbout and J. Baudon

The fractionation model of Robert et al. (1988) treats the gas-phase isotopic exchange reaction between kinetically excited atoms aX and diatomic MbX yielding bX and MaX and finds an abundance-dependent fractionation superimposed on the usual mass dependent fractionation. This paper shows that the treatment of Robert et al. is in error and presents a more straightforward treatment of the same system. This model shows only mass-dependent fractionation.

Sund, Mark T.↗

Know the enemy: 2D Fermi liquids

Highlights: • Regime of validity of the Fermi liquid theory in 2D interacting Fermi systems has been investigated. • Phase diagram for hydrodynamic and ballistic regimes in the frequency–temperature space has been obtained. • Temperature correction to quasiparticle effective mass has been calculated. • 2D Wiedemann–Franz law and 2D Kadawoki–Woods relation have been discussed. We describe an analytical theory investigating the regime of validity of the Fermi liquid theory in interacting, via the long-range Coulomb coupling, two-dimensional Fermi systems comparing it with the corresponding 3D systems. We find that the 2D Fermi liquid theory and 2D quasiparticles are robust up to high energies and temperatures of the order of Fermi energy above the Fermi surface, very similar to the corresponding three-dimensional situation. We calculate the phase diagram in the frequency–temperature space separating the collisionless ballistic regime and the collision-dominated hydrodynamic regime for 2D and 3D interacting electron systems. We also provide the temperature corrections up to third order for the renormalized effective mass, and comment on the validity of 2D Wiedemann–Franz law and 2D Kadawoki–Woods relation.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Mass fractionation of the lunar surface by solar wind sputtering

The sputtering of the lunar surface by the solar wind is examined as a possible mechanism of mass fractionation. Simple arguments based on current theories of sputtering and the ballistics of the sputtered atoms suggest that most ejected atoms will have sufficiently high energy to escape lunar gravity. However, the fraction of atoms which falls back to the surface is enriched in the heavier atomic components relative to the lighter ones. This material is incorporated into the heavily radiation-damaged outer surfaces of grains where it is subject to resputtering. Over the course of several hundred years an equilibrium surface layer, enriched in heavier atoms, is found to form. The dependence of the calculated results upon the sputtering rate and on the details of the energy spectrum of sputtered particles is investigated. It is concluded that mass fractionation by solar wind sputtering is likely to be an important phenomenon on the lunar surface.

Switkowski, Z. E.↗

Modeling of pickup ion distributions in the Halley cometosheath: Empirical limits on rates of ionization, diffusion, loss and creation of fast neutral atoms

The shape of the velocity distribution of water group ions observed by the Giotto ion mass spectrometer on its approach to comet Halley is modeled to derive empirical values for the rates of ionization, energy diffusion, and loss in the midcometosheath. The model includes the effect of rapid pitch angle scattering into a bispherical shell distribution as well as the effect of the magnetization of the plasma on the charge exchange loss rate. It is found that the average rate of ionization of cometary neutrals in this region of the cometosheath appears to be of the order of a factor 3 faster than the `standard' rates approx. 1 x 10(exp -6)/s that are generally assumed to model the observations in most regions of the comet environment. For the region of the coma studied in the present work (approx. 1 - 2 x 10(exp 5) km from the nucleus), the inferred energy diffusion coefficient is D(sub 0) approx. equals 0.0002 to 0.0005 sq km/cu s, which is generally lower than values used in other models. The empirically obtained loss rate appears to be about an order of magnitude greater than can be explained by charge exchange with the `standard' cross section of approx. 2 x 10(exp -15)sq cm. However such cross sections are not well known and for water group ion/water group neutral interactions, rates as high as 8 x 10(exp -15) sq cm have previously been suggested in the literature. Assuming the entire loss rate is due to charge exchange yields a rate of creation of fast neutral atoms of the order of approx. 10(exp -4)/s or higher, depending on the level of velocity diffusion. The fast neutrals may, in turn, be partly responsible for the higher-than-expected ionization rate.

Huddleston, D. E.↗

Pulsed source of energetic atomic oxygen

A pulsed high flux source of nearly monoenergetic atomic oxygen was designed, built, and successfully demonstrated. Molecular oxygen at several atmospheres pressure is introduced into an evacuated supersonic expansion nozzle through a pulsed molecular beam valve. An 18 J pulsed CO2 TEA laser is focused to intensities greater than 10(9) W/sq cm in the nozzle throat to generate a laser-induced breakdown. The resulting plasma is heated in excess of 20,000 K by a laser supported detonation wave, and then rapidly expands and cools. Nozzle geometry confines the expansion to provide rapid electron-ion recombination into atomic oxygen. Average O atom beam velocities from 5 to 13 km/s were measured at estimated fluxes to 10(18) atoms per pulse. Preliminary materials testing has produced the same surface oxygen enrichment in polyethylene samples as obtained on the STS-8 mission. Scanning electron microscope examinations of irradiated polymer surfaces reveal an erosion morphology similar to that obtained in low Earth orbit, with an estimated mass removal rate of approx. 10(-24) cu cm/atom. The characteristics of the O atom source and the results of some preliminary materials testing studies are reviewed.

Caledonia, George E.↗

Rydberg-atom-based single-photon detection for haloscope axion searches

We propose a Rydberg-atom-based single-photon detector for signal readout in dark matter haloscope experiments between 40 μ eV and 200 μ eV (10 GHz and 50 GHz). At these frequencies, standard haloscope readout using linear amplifiers is limited by quantum measurement noise, which can be avoided by using a single-photon detector. Our single-photon detection scheme can offer scan rate enhancements up to a factor of 10 4 over traditional linear amplifier readout, and is compatible with many different haloscope cavities. We identify multiple haloscope designs that could use our Rydberg-atom-based single-photon detector to search for QCD axions with masses above 40 μ eV (10 GHz), currently a minimally explored parameter space. Published by the American Physical Society 2024

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Molecular beam simulation of planetary atmospheric entry - Some recent results.

Progress is reported in the development of molecular beam techniques to simulate entry into planetary atmospheres. Molecular beam sources for producing fast beams containing CO2 and atomic oxygen are discussed. Results pertinent to the design and calibration of a mass spectrometer ion source for measurement of the Martian atmosphere during the free molecule portion of the entry trajectory are also presented. The shortcomings and advantages of this simulation technique are discussed, and it is demonstrated that even with certain inadequacies much information useful to the ion source design was obtained. Particularly, it is shown that an open-cavity configuration retains sensitivity to atomic oxygen, provides reasonable signal enhancement from the stagnation effect, is not highly sensitive to pitch and yaw effects, and presents no unforeseen problems in measuring CO2 or atomic oxygen.

French, J. B.↗

Local Electric Field Effects on Water Dissociation in Bipolar Membranes Studied Using Core–Shell Catalysts

The local electric field strength is thought to affect the rate of water dissociation (WD) in bipolar membranes (BPMs) at the catalyst–nanoparticle surfaces. Here, we study core–shell nanoparticles, where the core is metallic, semiconducting, or insulating, to understand this effect. The nanoparticle cores were coated with a WD catalyst layer (TiO2 or HfO2) via atomic layer deposition (ALD), and the morphology was imaged with transmission electron microscopy. Irrespective of the core material, these core–shell catalysts displayed comparable WD overpotentials at optimal mass loading, despite the hypothesized differences in the electric field strength across the catalyst particle suggested by continuum electrostatic simulations. Substantial atomic interdiffusion between the core and shell was ruled out by X-ray absorption spectroscopy, X-ray photoelectron spectroscopy, and diffuse reflectance optical measurements. However, the optimal mass loading of catalyst was roughly 1 order of magnitude higher for the conductive and high dielectric core materials than for the low dielectric insulating cores. These findings are consistent with the hypothesis that electric field screening within the core material focuses the electric field drop between particles such that larger film thicknesses can be tolerated. Collectively, these data support the idea that it is the local electric field at the molecular level that controls proton-transfer rates and that the metal core/dielectric-shell constructs introduced here modulate that field. Further materials and synthetic design may enable optimization of the electric field strength across the proton-transfer trajectory at the material surface.

Sarma, Prasad V↗

Empirical model of atomic nitrogen in the upper thermosphere

Atomic nitrogen number densities in the upper thermosphere measured by the open source neutral mass spectrometer (OSS) on Atmosphere Explorer-C during 1974 and part of 1975 have been used to construct a global empirical model at an altitude of 375 km based on a spherical harmonic expansion. The most evident features of the model are large diurnal and seasonal variations of atomic nitrogen and only a moderate and latitude-dependent density increase during periods of geomagnetic activity. Maximum and minimum N number densities at 375 km for periods of low solar activity are 3.6 x 10 to the 6th/cu cm at 1500 LST (local solar time) and low latitude in the summer hemisphere and 1.5 x 10 to the 5th/cu cm at 0200 LST at mid-latitudes in the winter hemisphere.

Engebretson, M. J.↗

Stamping Nanoparticles onto the Electrode for Rapid Electrochemical Analysis in Microfluidics

Electrochemical analysis is an efficient way to study various materials. However, nanoparticles are challenging due to the difficulty in fabricating a uniform electrode containing nanoparticles. We developed novel approaches to incorporate nanoparticles as a working electrode (WE) in a three-electrode microfluidic electrochemical cell. Specifically, conductive epoxy was used as a medium for direct application of nanoparticles onto the electrode surface. Three approaches in this work were illustrated, including sequence stamping, mix stamping, and droplet stamping. Shadow masking was used to form the conductive structure in the WE surface on a thin silicon nitride (SiN) membrane. Two types of nanomaterials, namely cerium oxide (CeO2) and graphite, were chosen as representative nanoparticles. The as-fabricated electrodes with attached particles were characterized using atomic force microscopy (AFM) and time-of-flight secondary ion mass spectrometry (ToF-SIMS). Electrochemical analysis was performed to verify the feasibility of these nanoparticles as electrodes. Nanomaterials can be quickly assessed for their electrochemical properties using these new electrode fabrication methods in a microfluidic cell, offering a passport for rapid nanomaterial electrochemical analysis in the future.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Chemical identification of new particle formation and growth precursors through positive matrix factorization of ambient ion measurements

Abstract. In the lower troposphere, rapid collisions between ions and trace gases result in the transfer of positive charge to the highest proton affinity species and negative charge to the lowest proton affinity species. Measurements of the chemical composition of ambient ions thus provide direct insight into the most acidic and basic trace gases and their ion–molecule clusters – compounds thought to be important for new particle formation and growth. We deployed an atmospheric pressure interface time-of-flight mass spectrometer (APi-ToF) to measure ambient ion chemical composition during the 2016 Holistic Interactions of Shallow Clouds, Aerosols, and Land Ecosystems (HI-SCALE) campaign at the United States Department of Energy Atmospheric Radiation Measurement facility in the Southern Great Plains (SGP), an agricultural region. Cations and anions were measured for alternating periods of ∼ 24 h over 1 month. We use binned positive matrix factorization (binPMF) and generalized Kendrick analysis (GKA) to obtain information about the chemical formulas and temporal variation in ionic composition without the need for averaging over a long timescale or a priori high-resolution peak fitting. Negative ions consist of strong acids including sulfuric and nitric acid, organosulfates, and clusters of NO3- with highly oxygenated organic molecules (HOMs) derived from monoterpene (MT) and sesquiterpene (SQT) oxidation. Organonitrates derived from SQTs account for most of the HOM signal. Combined with the diel profiles and back trajectory analysis, these results suggest that NO3 radical chemistry is active at this site. SQT oxidation products likely contribute to particle growth at the SGP site. The positive ions consist of bases including alkyl pyridines and amines and a series of high-mass species. Nearly all the positive ions contained only one nitrogen atom and in general support ammonia and amines as being the dominant bases that could participate in new particle formation. Overall, this work demonstrates how APi-ToF measurements combined with binPMF analysis can provide insight into the temporal evolution of compounds important for new particle formation and growth.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

First experimental determination of the ⁴⁰Ar(𝑛, 2𝑛)³⁹Ar reaction cross section and ³⁹Ar production in Earth’s atmosphere

The cosmogenic ³⁹Ar(t1∕2 = 268 years) isotope of argon is used for geophysical dating and tracing of underground and ocean water, as well as ice owing to its appropriate half-life and chemical inertness as a noble gas; ³⁹Ar serves also in nuclear weapon test monitoring. We measured for the first time the total cross section of the main ³⁹Ar cosmogenic production reaction in the atmosphere, namely ⁴⁰Ar(𝑛, 2𝑛)39 Ar, using 14.8 ± 0.3 MeV neutrons. The neutrons, produced by a deuterium-tritium generator, impinged on a stainless steel sphere filled with Ar gas highly enriched in the ⁴⁰Ar isotope and were monitored by a stack of fast-neutron activation foils. The reaction yield was measured by atom counting of long-lived ³⁹Ar with noble gas accelerator mass spectrometry and, independently, by decay counting relative to atmospheric argon (³⁹Ar/Ar= 8.12 × 10−16 ). A total ⁴⁰Ar(𝑛, 2𝑛)39 Ar cross section of 610 ± 100 mb was determined at 14.8 ± 0.3 MeV incident neutron energy. This result serves as a benchmark for recent theoretical calculations and evaluations, found to reproduce well the experimental total cross section. We use these energy-dependent theoretical cross sections together with experimental spectra of cosmogenic neutrons at different altitudes to calculate the global average rate of neutron-induced ³⁹Ar atmospheric production, resulting in 770 ± 240 39 Ar atoms/cm²/day. The secular equilibrium between the ³⁹Ar calculated production rate and radioactive decay rate leads to a partial isotopic abundance ³⁹Ar/Ar = (5.9 ± 1.8) × 10−16 , showing that ≈73% of atmospheric ³⁹Ar is produced by cosmogenic neutrons, the remaining part believed to be induced by muons and high-energy 𝛾 rays. The ⁴⁰Ar(𝑛, 2𝑛)³⁹Ar cross section at 14 MeV is also a key parameter for quantifying the anthropogenic contribution to atmospheric 39 Ar produced during the thermonuclear tests of the 1960s. We estimate that anthropogenic ³⁹Ar accounts for roughly 20% of the present atmospheric inventory.

39 Ar atmospheric production↗

Equatorial thermospheric composition and its variations

The neutral atmospheric composition experiment on the San Marco - 3 satellite has measured the composition of the equatorial atmosphere from 29 April to 29 November 1971. Preliminary results on the diurnal variation of atmospheric composition from 19 May to 30 June at 225 km. altitude are presented. The diurnal variation of helium is seen to reach its maximum near 0800 hours and its minimum in the late afternoon in contrast to the behavior of molecular nitrogen and argon. The atomic oxygen densities show smaller variations than the other gases. The mass densities calculated from the composition data agree well with those determined from the in situ drag force measurements and from orbital decay measurements.

Newton, G. P.↗

Results and progress on the NASA Lewis H2-O2 MHD program

A rocket test facility at the NASA Lewis Research Center has been used to develop interelectrode insulating materials, measure heat losses, and determine the fluid dynamic and electrical properties of MHD ducts and the cesium-seeded H2-O2 working fluid. Test results show that flame sprayed ceramic coatings on combustion chamber and nozzle walls permit operation with hot walls, eliminating problems associated with seed condensation; however, the net heat transfer was unexpectedly increased over that of cold copper walls. Pressure disturbances associated with oblique pressure waves were measured in a rocket nozzle designed to achieve low weight rather than perfectly parallel flow at the exit. Electrical conductivity measurements were in good agreement with theory except at low combustion pressures and/or high seed/oxygen mass flow ratios. The discrepancy is thought to result from poor atomization of the seed, producing droplets which do not completely vaporize during their residence time.

Smith, J. M.↗

Intercomparison of neutral composition measurements from the satellite Esro 4, Aeros A, Aeros B, and Atmosphere Explorer C

Number-density data obtained at orbital 'crossover' points with the neutral-gas mass spectrometers aboard the Esro 4, Aeros A, AE-C, and Aeros B satellites are intercompared. All the mass spectrometers were designed to measure the ambient number densities of atomic oxygen, molecular nitrogen, helium, and argon. It is found that the agreement for N2 and O is satisfactory within the experimental errors and that the He measurements exhibit unexpectedly large discrepancies far outside the error range. Calibration and instrument sources of error are considered.

Trinks, H.↗

Effects of oxygen dissociation on hypervelocity combustion experiments

Results are presented of a comparative experimental study conducted to measure the effects of the test gas oxygen dissociation produced in reflected shock tunnels on hypervelocity combustion. An identical combustor model was tested in a reflected shock tunnel with test gas containing about 50 pct by mass of oxygen in dissociated form, as either nitric oxide or atomic oxygen, and in an expansion tube with test gas having negligible dissociated oxygen. Comparisons are made at two test conditions that are energy equivalent to flight conditions at Mach 13.5 and 17.

Bakos, R. J.↗