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DOE OSTI2025

Dehydration of Methyl Lactate on Alkali Cation-Exchanged Faujasite: Effects of Metal Cation Identity and Water Pressure

Turnover rates for the catalytic dehydration of methyl lactate (ML) over ion-exchanged faujasite (FAU) catalysts depend on the identity of alkali metal cations (Na + , K + , Cs + ) and local solvation effects. Analysis of rate measurements and in situ infrared spectroscopy gives evidence that the reaction involves kinetically relevant dissociation of adsorbed methyl lactate upon alkali metal cations. This process involves concerted methyl transfer to the surface and dissociation of the alkali metal from the framework, which occurs at cationic active sites that remain predominantly unoccupied under relevant conditions (0.5–10 kPa ML, 0.5–15 kPa H 2 O, 563–583 K). Despite the mechanistic similarities, apparent activation enthalpies (ΔH app ‡ ) decrease linearly (47 kJ mol –1 from Na + to Cs + ) with ionization energy and cationic radius, and apparent activation entropies (ΔS app ‡ ) decrease 74 J mol –1 K –1 . These trends reflect electrostatic interactions that stabilize the cations to the anionic sites on the zeolite: stronger association between these charges leads to increasingly endothermic processes to displace the alkali metal to form a cationic methoxy and an intrapore metal lactate intermediate. Water physisorption measurements suggest alkali metal ions bind superstoichiometric quantities of water within FAU pores, and in situ infrared spectra suggest the concerted adsorption of ML requires reorganization of this water. Consequently, these processes introduce entropic gains that partially offset entropy losses associated with ML adsorption. Hence, turnover rates differ only by a factor of 2 among Na-, K-, and Cs-FAU at 573 K (ΔΔG app ‡ = 5 kJ mol –1 ). These findings demonstrate the interplay of alkali metal ions with zeolite active sites and intrapore water clusters for ML dehydration, indicating that these interactions can be leveraged to deliver optimal performance under different reaction conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1974

The abundances of nuclei in the cosmic radiation

The relative abundances are treated as a consequence of processes in cosmic ray transport occurring during passage of the radiation through interstellar material at high velocity. Some of the subjects mentioned are nuclear fragmentation and the production of secondary nuclei, nuclear reactions, energy loss and nuclear decay, ionization, the range-energy relation and propagation variables, capture and loss of electrons, the propagation of nuclei, the transport equation, equilibrium solutions, energy-dependent path length distribution, exponential path length distributions, discrete spectra, sources, supernovae, and the origin of the abundances. The connection between the space-time features of the sources, the material traversed, and the effects of magnetic fields is established by describing the particle-field interaction as a diffusive or random-walk process.

Reames, D. V.↗

DOE OSTI2022

Assessing high fidelity multi-component models to facilitate safeguards at Gas Centrifuge Enrichment Plants

We report that the International Atomic Energy Agency (IAEA) inspectors routinely carry out environmental sampling (ES) as a verification method. Collection of environmental swipe samples at various locations in Gas Centrifuge Enrichment Facilities (GCEPs) is an important process in detecting misuse of a declared facility and possibly the existence of undeclared nuclear material. These samples are measured for isotopic composition in uranium containing particles by Thermal Ionization Mass Spectrometry (TIMS) or Inductively Coupled Plasma Mass Spectrometry (ICP-MS). Even though ES is highly effective in detecting the absolute value of enrichments and their deviations from the declared values, it cannot explain the cause of those changes. Several potential explanations can serve as possibilities for particles detected above or other than the declared enrichment. These include normal and non-malicious events such as the design of the enrichment cascades, unintentional failures of the machines, or overshoot during startup of a cascade. It can also be the result of deliberate misuse by the facility operators. The primary objective of this work is to understand how these factors affect the enrichments produced by a cascade and quantify anticipated multi-isotopic concentrations for each case. The following methodology is employed to determine signatures at a particular facility. 1) Utilize a new two-dimensional multi-component diffusion code to obtain centrifuge performance data and use that information to design and perform cascade analysis. Compare and contrast the results with previous 1-D radially averaged solutions from the Pancake code. 2) Design a GCEP cascade with the production goal of 19.75% 235 U for each set of machine data above. Investigate two cascade scenarios that include enrichment of natural uranium (NU) feed to 19.75% 235U in a single cascade compared to a two-step process of NU to 5% and then 5% to 19.75%. 3) Simulate the intentional vs. unintentional off-normal scenarios in the cascades to assess the differences in isotopic concentrations. A non-ideal squared-off cascade model developed at the University of Virginia is used to calculate flow rates and isotopic concentrations of the process gas. The analysis is performed using the Rome machine model operated at 600 m/s rotor speed. The upper and lower bounds of normal and abnormal enrichments in a typical facility are used in conjunction with ES results to understand the root causes of such observations.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

DOE OSTI2021

Low-dose high-resolution $\mathrm{TOF}$-$\mathrm{PET}$ using ionization-activated multi-state low-$\mathrm{Z}$ detector media

We propose PET scanners using low atomic number media that undergo a persistent local change of state along the paths of the Compton recoil electrons. Measurement of the individual scattering locations and angles, deposited energies, and recoil electron directions allows using the kinematical constraints of the 2-body Compton scattering process to perform a statistical time-ordering of the scatterings, with a high probability of precisely identifying where the gamma first interacted in the detector. In these cases the Line-of-Response is measured with high resolution, determined by the underlying physics processes and not the detector segmentation. There are multiple such media that act through different mechanisms. As an example in which the change of state is quantum-mechanical through a change in molecular configuration, rather than thermodynamic, as in a bubble chamber, we present simulations of a two-state photoswitchable organic dye, a ‘Switchillator’, that is activated to a fluorescent-capable state by the ionization of the recoil electrons. The activated state is persistent, and can be optically excited multiple times to image individual activated molecules. Energy resolution is provided by counting the activated molecules. Location along the LOR is implemented by large-area time-of-flight MCP-PMT photodetectors with single photon time resolution in the tens of ps and sub-mm spatial resolution. Simulations indicate a large reduction of dose.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2025

First Measurement of 87 Rb( α , xn ) Cross Sections at Weak r -process Energies in Supernova ν -driven Ejecta to Investigate Elemental Abundances in Low-metallicity Stars

Observed abundances of Z ∼ 40 elements in metal-poor stars vary from star to star, indicating that the rapid and slow neutron capture processes may not contribute alone to the synthesis of elements beyond iron. The weak r-process was proposed to produce Z ∼ 40 elements in a subset of old stars. Thought to occur in the ν-driven ejecta of a core-collapse supernova, ( α, xn ) reactions would drive the nuclear flow toward heavier masses at T = 2−5 GK. However, current comparisons between modeled and observed yields do not bring satisfactory insights into the stellar environment, mainly due to the uncertainties of the nuclear physics inputs where the dispersion in a given reaction rate often exceeds 1 order of magnitude. Involved rates are calculated with the statistical model where the choice of an α -optical-model potential ( α OMP) leads to such a poor precision. The first experiment on 87 Rb( α, xn ) reactions at weak r -process energies is reported here. Total inclusive cross sections were assessed at E c.m. = 8.1−13 MeV (3.7−7.6 GK) with the active target MUlti-Sampling Ionization Chamber. With an N = 50 seed nucleus, the measured values agree with statistical model estimates using the α OMP Atomki-V2. A reevaluated reaction rate was incorporated into new nucleosynthesis calculations, focusing on ν-driven ejecta conditions known to be sensitive to this specific rate. These conditions were found to fail to reproduce the lighter heavy element abundances in metal-poor stars.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2022

Effects of Desiccation and Freezing on Microbial Ionizing Radiation Survivability: Considerations for Mars Sample Return

Increasingly, national space agencies are expanding their goals to include Mars exploration with sample return. To better protect Earth and its biosphere from potential extraterrestrial sources of contamination, as set forth in the Outer Space Treaty of 1967, international efforts to develop planetary protection measures strive to understand the danger of cross-contamination processes in Mars sample return missions. We aim to better understand the impact of the martian surface on microbial dormancy and survivability. Radiation resistance of microbes is a key parameter in considering survivability of microbes over geologic times on the frigid, arid surface of Mars that is bombarded by solar and galactic cosmic radiation. We tested the influence of desiccation and freezing on the ionizing radiation survival of six model microorganisms: vegetative cells of two bacteria (Deinococcus radiodurans, Escherichia coli) and a strain of budding yeast (Saccharomyces cerevisiae); and vegetative cells and endospores of three Bacillus bacteria (B. subtilis, B. megaterium, B. thuringiensis). Desiccation and freezing greatly increased radiation survival of vegetative polyploid microorganisms when applied separately, and when combined, desiccation and freezing increased radiation survival even more so. Thus, the radiation survival threshold of polyploid D. radiodurans cells can be extended from the already high value of 25 kGy in liquid culture to an astonishing 140 kGy when the cells are both desiccated and frozen. However, such synergistic radioprotective effects of desiccation and freezing were not observed in monogenomic or digenomic Bacillus cells and endospores, which are generally sterilized by 12 kGy. This difference is associated with a critical requirement for survivability under radiation, that is, repair of genome damage caused by radiation. Deinococcus radiodurans and S. cerevisiae accumulate similarly high levels of the Mn antioxidants that are required for extreme radiation resistance, as do endospores, though they greatly exceed spores in radioresistance because they contain multiple identical genome copies, which in D. radiodurans are joined by persistent Holliday junctions. We estimate ionizing radiation survival limits of polyploid DNA-based life-forms to be hundreds of millions of years of background radiation while buried in the martian subsurface. Our findings imply that forward contamination of Mars will essentially be permanent, and backward contamination is a possibility if life ever existed on Mars.

59 BASIC BIOLOGICAL SCIENCES↗

NASA NTRS1990

The role of shocks in NGC 6240

The case of the infrared-bright system NGC 6240 encapsulates in many ways the major issues in understanding processes in infrared-bright systems in general. Its morphology strongly suggests that this is a merger in progress, with energetic phenomena being triggered as evidenced by strong radio emission and optical emission lines as well as the strong far-infrared output. Evidence has been produced supporting various schemes for producing the energy being radiated by this object. Early work on the optical spectrum suggested a Seyfert 2 classification, but the ionization level and spatial extent of the emission implied a more distributed source of energy. IR line studies found evidence for young supergiants, and for immense amounts of H2 excited by low-velocity shocks, which might contribute to a large enhancement in star-formation rate. Finally, the radio-continuum morphology shows compact sources possibly associated with active nuclei in both remnants of the merger. This is one of the nearest IR-bright galaxies objects at high luminosity (Cz = 7500 km s(exp -1), so that spatially resolved studies can yield further insight into which of these processes are most important - star formation, nuclear activity, or shock excitation. The velocity field, linewidth distribution, and ionization structure of the gas in NGC 6240 was mapped with the Dense-Pak fiber-optic array on the Kitt Peak 4-m telescope. In all, 135 spectra were obtained through an array of 2 inch apertures, with considerable overlap between many of the adjacent apertures produced by offsetting the telescope between the exposures. As the strongest features with lambda less than 1.1 ma, H alpha and the adjacent (NII) lines were observed, along with the neighboring (O I) and (S II) features. Maps of velocity and linewidth were constructed by interpolating measurements from these spectra onto a regular grid, and show irregular patterns with large velocity gradients and, particularly, an extended region of large local (shear?) velocity width.

Keel, William C.↗

NASA NTRS1980

Dielectronic recombination rates, ionization equilibrium, and radiative emission rates for calcium and nickel ions in low-density high-temperature plasmas

The total dielectronic recombination rates for Ca and Ni ions were calculated taking into account autoionization to excited states of the recombining ion and stabilizing radiative transitions of the recombining electron. Radiative transitions of the recombining ion are found to be the dominant stabilizing processes, and the relative importance of Delta n = 0 and Delta n not equal to 0 transitions in the relevant temperature region is determined for each ion. The relative importance of the Delta n = 0 and Delta n not equal to 0 contributions is significantly altered for some ions by the inclusion of autoionization to excited levels. The relative abundance of the various ionization stages has been determined by using a corona equilibrium model in which collisional ionization and inner-shell excitation followed by autoionization are balanced by direct radiative and dielectronic recombination.

Jacobs, V. L.↗

NASA NTRS1983

The solar wind ionization state as a coronal temperature diagnostic

The 'frozen' solar wind ionization state within a few solar radii of the photosphere suggests that ion measurements at 1 AU may yield information on the electron temperature conditions at the base of the coronal expansion. The freezing-in process is examined in light of traditional assumptions as to coronal expansion, where electron temperature decreases monotonically with height, the bulk flow of all charge states of a given ion species are equal to the proton speed, and the ion outflow is spherically symmetric. The consequences of the relaxation of these assumptions include the underestimation of the magnitude of a temperature maximum occurring near the freezing-in radius. Because it is associated with high speed, low density flow, an areal divergence that is faster than that in a spherical outflow lowers the ionization state freezing-in level relative to that which is typical in spherically symmetric expansion.

Owocki, S. P.↗

DOE OSTI2020

Similarity of capacitive radio-frequency discharges in nonlocal regimes

Similarity transformations are essential for correlating discharges at different scales, which are mostly utilized with local field or local energy approximations. In this work, we report the fully kinetic results from particle-in-cell/Monte Carlo collision simulations that unambiguously demonstrate the similarity of radio frequency (rf) discharges in nonlocal regimes where the electron energy relaxation length is much larger than the gap dimension. It is found that at a constant rf voltage amplitude, discharges will be similar if the gas pressure, inverse of gap distance, and rf driving frequency are all changed by the same scaling factor. The scaling relations of fundamental parameters are illustrated for rf discharges in the alpha-mode with secondary electron emission ignored, and the temporal electron kinetics are shown to have invariance in similar discharges. The results explicitly validate the scaling laws in nonlocal kinetic regimes, indicating promising application potentials of the similarity transformations across a wide range of kinetic regimes.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2025

Understanding the Quadrupole Mass Filter and Testing a High-Resolution QMS RGA for ITER

A common type of residual gas analyzer is the quadrupole mass spectrometer. One of the main components within this instrument is a mass filter known as the quadrupole. It is responsible for the selective throughput of the ionized gas particles - by ascending mass number - prior to ion impacts on the analyzer (or detector) surface from which the ion current signal is generated for processing. However, the quadrupole is not fully described in relation to the electric field characteristics and the function as an ion mass separator. This paper describes the basic origins of the electrical design, the intricate assembly criteria, and performance of the quadrupole within the spectrometer. A specialized quadrupole mass spectrometer is part of a configuration for a diagnostic gas analyzer system planned for ITER, a fusion research machine. It has a verified capability, essential as a diagnostic criterion for this reactor project, to successfully deconvolute the mass signals of Helium-4 and deuterium (reactor fuel exhaust gases, separated by only 0.026 atomic mass units), down to a relative three-percent concentration of the former gas. The associated preliminary testing, performed at the Oak Ridge National Laboratory, is also addressed. Finally, one of the key parameters used to express gas concentration, the relative sensitivity factor, will be explained, including an evaluation of dependency on other variables.

Marcus, Chris [ORNL] (ORCID:0000000190139636)↗

DOE OSTI2023

NGC 6302: The Tempestuous Life of a Butterfly

Abstract NGC 6302 (The Butterfly Nebula) is an extremely energetic and rapidly expanding bipolar planetary nebula (PN). If the central source is a single star, then its apparent location in an H-R diagram places it among the most massive, hottest, and presumably rapidly evolving of all central stars of PNe. Our proper motion study of NGC 6302, based on Hubble Space Telescope WFC3 images spanning 11 yr, has uncovered at least four different pairs of uniformly expanding internal lobes ejected at various times and orientations over the past two millennia at speeds ranging from 10–600 km s −1 . In addition, we find a pair of collimated off-axis flows in constant motion at ∼770 ± 100 km s −1 within which bright [Feii]feathersare conspicuous. Combining our results with those previously published, we find that the ensemble of flows has an ionized mass >0.1M ⊙ and its kinetic energy, between 10 46 and 10 48 erg, lies at the upper end of gravity-powered PNe ejection processes such as stellar mergers or mass accretion. We assemble our results into a plausible historical timeline of ejections from the nucleus and suggest that the ejections are powered by gravitational infall.

Astronomy & Astrophysics↗

NASA NTRS1964

Injection and distribution of liquids in the flow fields of blunt shapes at hypersonic speeds

A possible method for reducing the attenuation of radio transmission from hypersonic vehicles is by injection of a liquid into the flow field. The hot plasma layer surrounding the vehicle could presumably be quenched if the latent heat of the liquid and the heat capacity of the vapor could be utilized efficiently. In the case of stagnation-point injection, the momentum of the liquid could be utilized to modify the bow shock and possibly reduce the initial ionization. To attain these objectives of efficient coolant utilization or modification of the bow shock a knowledge of the liquid injection, atomization, spray penetration, and evaporation processes is required. This report presents the results of a study of liquid injection into hypersonic flow fields. A simplified theory for evaporation distances is derived and is shown to be in qualitative agreement with experimental data. Correlation of experimental data for maximum cross-current penetration of the liquid spray for injection near the shoulder pf a hemisphere cylinder, a sphere 9° cone, and a Mercury model are given. These data were obtained in the Langley Mach 8 variable density tunnel with both liquid nitrogen and water injection to provide a large range of liquid parameters. Flow-field disturbances, as indicated by schlieren photographs and surface pressures, increased with the ratio of coolant mass flux to airstream mass flux. For stagnation-point injection, the maximum shock standoff distance was correlated by the ratio of the liquid jet momentum flux to the airstream momentum flux.

Ivan E. Beckwith↗

NASA NTRS1974

Photoelectric spectrophotometry of OQ 172 and OH 471

Absolute spectral energy distributions for the large redshift quasars OQ 172 and OH 471 are discussed along with similar data for two other quasars 4C05.34 and PHL 957. Assuming cosmological redshifts, OQ 172 and OH 471 are not as luminous as PHL 957. If these quasars are basically similar and if radiative processes dominate, the strength of Ly alpha and the behavior of the continuum at the Lyman limit strongly suggest that these objects consist of a central ionizing source surrounded by discrete clouds, filaments or a gaseous structure such as a disk. This gaseous matter does not cover the whole solid angle surrounding the source.

Oke, J. B.↗

NASA NTRS1992

Stochastic stellar wind models - Evolved stars

Observational, semiempirical, and theoretical results are presented for individual cool giants and supergiants which show that stochastic stellar wind flows are an extremely important feature in these stars. It is shown that the status of the existing theoretical models is very uncertain, due to the fact that appropriate models must simultaneously take into account a broad variety of strongly coupled physical processes. The potentially important physical processes include global oscillation modes; convection; magnetic fields; the generation, propagation, and interaction of stochastic waves; three-dimensional radiative transfer effects; time-dependent hydrogen ionization; thermal bifurcation and instabilities; and nonequilibrium chemistry, particularly the formation and destruction of molecules and dust.

Cuntz, Manfred↗

NASA NTRS2004

Polycyclic Aromatic Hydrocarbon Ionization Energy Lowering in Water Ices

In studying various interstellar and solar system ice analogs, we have recently found that upon vacuum ultraviolet photolysis, polycyclic aromatic hydrocarbons (PAHs) frozen in water ice at low temperatures are easily ionized and indefinitely stabilized as trapped ions (Gudipati; Gudipati & Allamandola). Here we report the first experimental study that shows that PAH ionization energy is significantly lowered in PAH/H2O ices, in agreement with recent theoretical work (Woon & Park). The ionization energy (IE) of the PAH studied here, quaterrylene (C40H20, IE = 6.11 eV), is lowered by up to 2.11 eV in water ice. PAH ionization energy reduction in low-temperature water ice substantially expands the astronomical regions in which trapped ions and electrons may be important. This reduction in ionization energy should also hold for other types of trapped species in waterrich interstellar, circumstellar, and solar system ices. Subject headings: ISM: clouds - methods: laboratory - molecular processes - radiation mechanisms: nonthermal -ultraviolet: ISM - ultraviolet: solar system

Gudipati, Murthy S.↗

DOE OSTI2020

Proton beam position measurement in air using a BPM

A Beam Position Monitor (BPM) is potentially useful to measure the position and phase of the beam in air in a non-destructive way. An air-gap BPM in experiments, such as beam-induced radioactive waste management and dynamic radiography applications, where a so-called air gap is needed, can be utilized to measure the beam position and phase. In this study, a stripline BPM was used in the air-gap of an 800 MeV proton beam transport line. The downstream end of the primary beamline exit window was made of a thin aluminum plate and allowed the beam to travel 1.2 m in ambient air before re-entering into a vacuum drift section. Such a configuration was arranged to examine the BPM effectiveness in atmospheric temperature and pressure where ionization of air occurs. In this study, a high energy (800 MeV), high current (0.6 A beam peak current/pulse) proton beam of 5 mm radius was transported in the air. The beam position relative to the axis was measured by detecting the signature of the beam in a nanosecond scale. This nanosecond scale detection ability was useful to identify other signals such as plasma effects. The BPM signals were processed at a frequency of 201 MHz; thus, one gets a stronger response in a stripline pattern as it was used in this study instead of a dot-type BPM. Experimental data show that the BPM works well in air, but ionization of air or plasma formation could not be measured over the BPM signal. The design, construction, and performance of a BPM in air environment are presented.

43 PARTICLE ACCELERATORS↗

NASA NTRS1981

Studies of the role of metastables and doubly ionized species in the chemical and thermal structure of the Venusian and Martian ionospheres

Models of the upper atmospheres of Mars and Venus were constructed using Viking and Pioneer Venus data. The neutral densities, with the exception of NO, N(4S), N(2D) and N(2P) were taken from the measured values, along with the neutral, ion, and electron temperatures. Using solar fluxes and relevant cross sections, the production rates of ions and neutral fragments by photo and electron impact processes were computed. These production rates were combined with chemical production rates and loss along with one dimensional transport eddy diffusion, molecular and ambi polar diffusion, and thermal diffusion, to determine the densities of ions and odd nitrogen species. Preliminary calculations show that the chemistry of metastables and doubly ionized species is important in the ionospheres of Mars and Venus. Production of N(+) in metastable reactions is particularly important, and it explains the discrepancy between the measurements of earlier models. Production of CO(+) is also affected. Reactions of O(++) and O(+)(2D) with N2 have important consequences for the escape rate of atomic nitrogen from the Martian atmosphere.

Fox, J. L.↗