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At least 577 records · Page 32

Collisional processes in cometary plasmas

The interaction of the solar wind with comets is initiated at large distances from the nucleus by the ionization of cometary neutrals. The resulting contamination of the solar wind with cometary ions mass-loads the solar wind flow, causing it to slow down. The plasma-comet interaction is largely collisionless at large cometocentric distances. However, collisional processes become important in the inner coma (within the cometopause). Collisional processes include charge-transfer between solar wind protons and neutrals, ion-neutral friction, electron and ion thermal cooling, and ion-neutral chemistry. For example, the magnetometer on the Giotto spacecraft observed a diamagnetic cavity near closest approach. This cavity is a consequence of the balance between an inward-directed magnetic pressure gradient force and an outward ion-netural frictional force. Thermalization of the cometary ion distribution function by Coulomb collisions is another important process in the inner coma of an active comet.

Cravens, T. E.↗

Magnetospheres of the outer planets

The magnetospheres of the outer planets have been shown by Voyager explorations to strongly interact with the surfaces and atmospheres of their planetary satellites and rings. In the cases of Jupiter, Saturn and Uranus, the processes of charged particle sputtering, neutral gas cloud formation, and rapid plasma injection from the ionization of the neutral clouds, have important implications both for the magnetospheres as a whole and for the surfaces and atmospheres of their satellites. The general methodology employed in these researches has involved comparisons of the planetary magnetospheres in order to identify common physical processes.

Cheng, Andrew F.↗

Reionization of the Universe and the Photoevaporation of Cosmological Minihalos

The first sources of ionizing radiation to condense out of the dark and neutral Intergalactic Medium (IGM) sent ionization fronts sweeping outward through their surroundings, overtaking other condensed objects and photoevaporating them. This feedback effect of universal reionization on cosmic structure formation is demonstrated here for the case of a cosmological minihalo of dark matter and baryons exposed to an external source of ionizing radiation with a quasar-like spectrum, just after the passage of the global ionization front created by the source. We model the pre-ionization minihalo as a truncated, nonsingular isothermal sphere in hydrostatic equilibrium following its collapse out of the expanding background universe and virialization. Results are presented of the first, gas dynamical simulations of this process, including radiative transfer. A sample of observational diagnostics is also presented, including the spatially-varying ionization levels of C, N, and O in the flow if a trace of heavy elements is present and the integrated column densities of H I, He I and He II, and C IV through the photoevaporating gas at different velocities, which would be measured in absorption against a background source like that responsible for the ionization.

Shapiro, Paul R.↗

Spacecraft mass spectrometer ion source employing field emission cathodes

An ion source that utilizes a pair of thin-film field emission cathodes to provide current for electric impact ionization is studied. The field emission cathodes are composed of microscopically small needle tips and an extraction electrode; the cathodes generate a 200-eV, 0.1-mA electron beam. The multistep process for the manufacturing of the field emission cathodes is examined. The operation of the ion source, which ionizes atoms and molecules that enter the mass spectrometer with a ram velocity of about 80 km/sec, is described.

Curtis, C. C.↗

Radiological Degradation of Tetraoctyl Diglycolamide in n-Alkyl Solvents: Influence of Solvent Ionization Potential

Reprocessing of used nuclear fuel reduces the requirements for long-term storage repositories. Cost-efficient processes depend on knowledge of radiation effects, but gaps occur in understanding how radiation results in the degradation of fuel separation molecules. This project investigates the influence of different n-alkyl solvents on the radiolytic fragmentation behavior of N,N,N',N'-Tetraoctyl-3-oxapentane-1,5-diamide (TODGA), a promising ligand for extraction of the lanthanides and minor actinides from dissolved nuclear fuel. Findings from this work suggest a linkage between the ionization potential of the solvent and the degradation products observed in the resulting mass spectrum.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

The acceleration of heavy nuclei in solar flares

The overabundance of heavy nuclei in solar cosmic rays of energy approximately 5 Mev/nucleon is explained by taking into account the pre-flare ionization states of these nuclei in the region where they are accelerated. A model is proposed which considers two-step accelerations associated with the initial development of solar flares. The first step is closely related to the triggering process of flares, while the second one starts with the development of the explosive phase. Further ionization of medium and heavy nuclei occurs through their interaction with Kev electrons accelerated by the first-step acceleration. It is suggested that the role of these electrons is important in producing fully ionized atoms in the acceleration regions.

Sakurai, K.↗

The acceleration of heavy nuclei in solar flares

The overabundance of heavy nuclei in solar cosmic rays of energy below about 10 MeV/nucleon is explained by taking into account the pre-flare ionization states of these nuclei in the region where they are accelerated. A model is proposed which considers two-step accelerations associated with the initial development of solar flares. The first step is closely related to the triggering process of flares, while the second one starts with the development of the explosive phase. Further ionization of medium and heavy nuclei occurs through their interaction with keV electrons accelerated by the first-step acceleration. It is suggested that the role of these electrons is important in producing fully ionized atoms in the acceleration regions.

Sakurai, K.↗

Influence of strong Coulomb coupling on diffusion in atmospheric pressure plasmas

Ion diffusion in atmospheric pressure plasmas is examined and particular attention is paid to the fact that ion–ion interactions can be influenced by strong Coulomb coupling. Three regimes are identified. At low ionization fractions (x i ≲ 10 —6 ), standard weakly correlated ion-neutral interactions set the diffusion rate. At moderate ionization fractions (10 —6 ≲ x i ≲ 10 —2 ) there is a transition from ion-neutral to ion–ion collisions setting the diffusion rate. In this regime, the effect of strong Coulomb coupling in ion–ion collisions is accounted for by applying the mean force kinetic theory. Since both ion-neutral and ion–ion interactions contribute a comparable amount to the total diffusion rate, models (such as particle-in-cell or fluid) must account for both contributions. At high ionization fractions (x i ≳ 10 —2 ), strongly correlated ion–ion collisions dominate and the plasma is heated substantially by a disorder-induced heating (DIH) process associated with strong correlations. The temperature increase due to DIH strongly influences the ion diffusion rate. This effect becomes even more important, and occurs at lower ionization fractions, as the pressure increases above atmospheric pressure. In addition to ion diffusion, DIH affects the neutral gas temperature, therefore influencing the neutral diffusion rate. Model predictions are tested using molecular dynamics simulations, which included a Monte Carlo collision routine to simulate the effect of ion-neutral collisions at the lowest ionization fractions. The model and simulations show good agreement over a broad range of ionization fractions. Importantly, the results provide a model for ion diffusion, on a wide range of ionization fractions and pressures, solely considering the elastic contribution to the diffusion coefficient—as an illustration of how strong Coulomb coupling influences diffusion processes in general.

fast neutral gas heating↗

Collaborative Research: Natural Organic Matter and Microbial Controls on Mobilization/Immobilization of I and Pu in Soils and Waters Affected by Radionuclide Releases in USA and Japan

In this project, the relationship between natural organic matter (NOM) and two radioactive elements that are relevant to nuclear waste disposal were studied: Plutonium (Pu) and Iodine. The human and environmental risks associated with Pu stem mainly from the very long half-lives of several of its isotopes ( 238 Pu, 88 yr; 239 Pu, 24,100 yr; 240 Pu, 6560 yr) and its radiotoxicity. Understanding Pu biogeochemical behavior in both near-field (>10-11M) and far-field scales (<10-11M) is imperative to the development of approaches for reprocessing Pu, remediation of Pu contamination and accurate assessment of risks posed by disposal practices for Pu-bearing wastes. The environmental mobility of Pu can be affected by redox potential, pH, adsorption, precipitation, complexation, colloid formation, and microbial activity, of which the first characteristic has the most profound influence. Numerous studies have shown high affinity of Pu towards NOM, as well as to mineral phases. NOM is ubiquitous in the environment, e.g., both fulvic and humic acids are able to reduce Pu(V,VI) to Pu(IV) and the redox potential of NOM is positively related to the abundance of phenolic/acidic OH groups. NOM can either facilitate or limit actinide migration, depending on specific biogeochemical conditions including pH, mineral and organic matter characteristics, etc. The other radionuclide of interest is radioiodine ( 129 I). 129I is a major by-product of nuclear fission and of serious concern to the Department of Energy (DOE) as it is among the top risk drivers at existing and potential radiowaste-contaminated sites. The risk of 129 I stems largely from its high bioconcentration factor (90% of the body’s iodine is accumulated in the thyroid), a high inventory at source terms, a very long-half life (16M years), and rapid mobility in the subsurface environment. As a consequence, 129 I has the lowest drinking water standard (1 pCi/L) among all radionuclides in the Federal Register. With a novel and sensitive gas chromatography-mass spectrometry (GC-MS) method developed in our lab, it is possible to quickly and simultaneously determine the distribution of 129 I and stable 127 I forms in environments, as low as 2 pCi/L for 129 I. This method was subsequently validated using accelerator mass spectroscopy, AMS. IO 3 - and organo-I were determined as major species in the groundwater of SRS and the Hanford Site, contrary to thermodynamic predictions that I- should be the dominant species at these sites. Mobility of 129 I was also demonstrated to depend greatly on the I species and its concentration, sediment pH, and redox state, with times to achieve equilibrium taking up to 12 weeks. Along the groundwater pathway in the F-Area of SRS, 129 I- supplied from the seepage basins was transformed to 129 IO 3 - and organo- 129 I with increasing iodine sediment sorption, causing the lower total 127 I and 129 I concentrations along the gradient transect of the waste plume. By contrast, groundwater 129 I concentrations in the wetlands (as high as 1617.3 pCi/L) were greatly elevated with respect to the source term (159.3 pCi/L). While the NOM promoted the uptake of 129 I to the wetland sediment, it also promoted the formation of soluble organic fraction. A small fraction of NOM that is bound to iodine can behave as a mobile organo-I source. Iodide was enzymatically incorporated into NOM, whereas both iodide and iodate were abiotically bound to NOM, under certain conditions. Iodate removal from the mobile aqueous phase can also occur through incorporation into carbonate (e.g., at the Hanford Site, USA). Thus immobilization and re-mobilization of iodine species were influenced by pH, Eh and the presence of NOM and metal oxides, which adds to the complexity of site remediation action. A ground-breaking result was to elucidate the products (i.e. organo-iodine moieties formed via enzymatic and non-enzymatic processes) at the molecular level by nuclear magnetic resonance (NMR) and electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry (ESI-FTICRMS). We found that iodine-NOM interactions may be influenced by NOM hydrophobic aliphatic moieties. From the perspective of ESI-FTICRMS, organo-iodine formulas were ascribed to the groups of unsaturated hydrocarbons, lignins and proteins. Iodate is likely abiotically reduced to reactive iodine species by lignin- and tannin-like compounds or carboxylic-rich alicyclic molecules (CRAM). We also investigated microbial mechanisms in iodine incorporation into NOM. We established that soil bacteria isolated from F-Area of SRS did not accumulate significant amounts of I- (0.2-2%). Intracellular uptake of I- decreases with increasing pH when pH ranged from 4 to 6. In contrast, 44 out of 84 strains isolated from the F-Area of SRS can transform I- to IO 3 - and organo-iodine. In some cases, oxidation was facilitated in the presence of H 2 O 2 . Microbes can also excrete organic acids that enhance I- oxidation by lowering the ambient pH and reacting with H 2 O 2 to form peroxy carboxylic acids. At lower pH values (≤5), H 2 O 2 hydrolysis was the driving force for iodide-oxidation; whereas, at pH ≥ 6, spontaneous decomposition of peroxy carboxylic acids, originating from H 2 O 2 and organic acids were the primary cause of iodide oxidation. Lastly, it was determined that microbial processes involved in Mn (II) are capable of directly oxidizing I- via enzymatic catalysis (i.e., multicopper oxidases), or indirectly through the formation of reactive oxygen species (ROS) and/or biogenic manganese oxides. ROS-mediated oxidation of I- was found to predominate at pH >5, whereas the enzymatic and Mn oxide pathways were more active at pH < 5. Together, this project has resulted in 9 publications in high-impact journals, and the training of 1 Ph.D and 4 undergraduate students.

54 ENVIRONMENTAL SCIENCES↗

Ionospheric chemistry

This report deals primarily with progress in the chemistry of minor neutrals and ionized constituents of the thermosphere. Significant progress was made over the last few years in quantitative studies of many chemical processes. This success was primarily due to the advent of multiparameter multisatellite programs which permitted accurate simultaneous measurements to be made of many important parameters. In many cases studies of chemical reactions were made with laboratory-like precision. Rate coefficients have been derived as functions of temperature for a number of important reactions. New information has been acquired on nearly every major process which occurs in the thermosphere, including the recombination rates of all major molecular ions, charge transfer reactions, ion atom interchange reactions, and reactions of neutral and ionized metastable atoms and molecules.

Torr, D. G.↗

Computer Modeling of Electrostatic Aggregation of Granular Materials in Planetary and Astrophysical Settings

Electrostatic forces strongly influence the behavior of granular materials in both dispersed (cloud) systems and semi-packed systems. These forces can cause aggregation or dispersion of particles and are important in a variety of astrophysical and planetary settings. There are also many industrial and commercial settings where granular matter and electrostatics become partners for both good and bad. This partnership is important for human exploration on Mars where dust adheres to suits, machines, and habitats. Long-range Coulombic (electrostatic) forces, as opposed to contact-induced dipoles and van der Waals attractions, are generally regarded as resulting from net charge. We have proposed that in addition to net charge interactions, randomly distributed charge carriers on grains will result in a dipole moment regardless of any net charge. If grains are unconfined, or fluidized, they will rotate so that the dipole always induces attraction between grains. Aggregates are readily formed, and Coulombic polarity resulting from the dipole produces end-to-end stacking of grains to form filamentary aggregates. This has been demonstrated in USML experiments on Space Shuttle where microgravity facilitated the unmasking of static forces. It has also been demonstrated in a computer model using grains with charge carriers of both sign. Model results very closely resembled micro-g results with actual sand grains. Further computer modeling of the aggregation process has been conducted to improve our understanding of the aggregation process, and to provide a predictive tool for microgravity experiments slated for Space Station. These experiments will attempt to prove the dipole concept as outlined above. We have considerably enhanced the original computer model: refinements to the algorithm have improved the fidelity of grain behavior during grain contact, special attention has been paid to simulation time steps to enable establishment of a meaningful, quantitative time axis, and calibration of rounding accuracies have been conducted to test cumulative numerical influences in the model. The model has been run for larger grain populations, variable initial cloud densities, and we have introduced random net charging to individual grains, as well as a net charge to the cloud as a whole. The model uses 3 positive and 3 negative charges randomly distributed on each grain, with up to 160 grains contained within various size "boxes" that define the initial number densities in the clouds. Each charge represents localized charged region on a grain, but does not necessarily imply single quantized charge carriers. The Coulomb equations are then allowed to interact for each monopole: dipoles and any higher order charge coupling is a natural product of these "free" interactions over which the modeler exerts no influence. The charges are placed on surfaces of grains at random locations. A series of runs was conducted for neutral grains that had a perfect balance of negative and positive char carriers. Runs were also conducted with grains having additional fractional charges ranging between 0 and 1. By adding fractional charges of one sign, the model created grain populations in which all grains had excess charges the same sign, giving the cloud an overall net charge. This simulates clouds subjected to ionizing radiation (e. protoplanetary debris disk around a protosun), or any other process of charge biasing in a grain population (e.g., volcanic plumes). In another run series, random fractional charges of either sign were added to the grains so th some grains had a slight net positive charge while others had a slight net negative charge. This simulates triboelectrically-charged grain populations in which acquisition of an electron by one surface is at the expense creating a hole elsewhere. This dual sign charging was applied in two ways: in one case the cloud remained neutral by ensuring that all grain excess charges added to zero; in the other case, the cloud was permitted slight net char by not imposing a charge-balance condition. Additional information is contained in the original.

Marshall, J.↗

Physical processes associated with current collection by plasma contactors

Recent flight data confirms laboratory observations that the release of neutral gas increases plasma sheath currents. Plasma contactors are devices which release a partially ionized gas in order to enhance the current flow between a spacecraft and the space plasma. Ionization of the expellant gas and the formation of a double layer between the anode plasma and the space plasma are the dominant physical processes. A theory is presented of the interaction between the contactor plasma and the background plasma. The conditions for formation of a double layer between the two plasmas are derived. Double layer formation is shown to be a consequence of the nonlinear response of the plasmas to changes in potential. Numerical calculations based upon this model are compared with laboratory measurements of current collection by hollow cathode-based plasma contactors.

Katz, Ira↗

The poleward edge of the mid-latitude trough - Its formation, orientation and dynamics

Data from the Advanced Ionospheric Sounder (AIS) deployed at Halley, Antarctica (76-deg S, 27-deg W; L = 4.2) and the Dynamics Explorer-2 spacecraft (DE-2) are used to investigate several aspects of the formation processes and dynamics of the poleward edge of the midlatitude electron density trough. These include a study of the flux and energy of charged particles precipitating into the F-region as a function of Magnetic Local Time. It is found that local energetic electron precipitation is a major source of ionization of the poleward edge in the evening sector, but only after magnetic midnight transport processes become more important. Occasionally a significant increase in the flux of conjugate photoelectrons is colocated with the poleward edge of the trough in the morning sector. The combination of AIS and DE-2 data has allowed identification of significant longitudinal structure on the poleward edge of the trough that may be the result of substorm activity. It is found that the orientation of the poleward edge of the trough and the locus of the plasmapause predicted from the 'tear-drop' model vary in rather a similar manner with local time, though no close physical link between the two features is inferred from this coincidence.

Rodger, A. S.↗

Electrochemical Manipulation and Radiolytic Evaluation of Organic Phase Neptunium

Presentation for Seed LDRD proposal presentation: This Seed LDRD research proposes to test an innovative approach to precisely control the oxidation state distribution of neptunium (Np) under used nuclear fuel (UNF) reprocessing conditions using novel electrochemical methods. Current UNF reprocessing technologies are not financially viable in the US, requiring significant scientific and technological innovation to improve cost efficiency. Reducing the number of process cycles is one avenue for increasing cost efficiency, of which resolving the challenge associated with isolating Np is critical. Under envisioned process conditions, Np is present in a mixture of extractable (Np(IV) and Np(VI)) and inextractable (Np(V)) oxidation states, the distribution of which is dependent on several factors, including ionizing radiation dose, that change throughout a reprocessing scheme. Consequently, Np unintentionally partitions into various UNF reprocessing phases and product streams, ultimately increasing the number of process cycles to isolate UNF components. Here, we propose to employ novel, high surface area, optically transparent, Ligand Modified tin-doped indium oxide Electrodes (LMES). These LMEs bind Np, and therefore enable concurrent generation and spectroscopic characterization of Np oxidation states in organic solutions. These proof-of-concept experiments will: (i) facilitate optimization of the proposed electrochemical system conditions for Np oxidation state manipulation; (ii) identify the accessible electrochemical window for Np complexes in the organic phase; (iii) report characteristic optical spectra for each accessible complexed Np oxidation state; and (iv) determine the lifetime and partitioning of a given atypical Np oxidation state in the organic phase in the presence and absence of ionizing radiation fields. The data gathered by this Seed LDRD will provide support for the design of an electrochemical process concept for the precise manipulation of Np oxidation states in UNF reprocessing solvent systems, with the intention of providing advanced control over Np mass transfer, and thus greater process efficiency and economy.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Collisional-Radiative Nonequilibrium and Precursor Effects in a Nitrogen Shock Wave

Improvements to a plasma code with a Collisional-Radiative (CR) non-equilibrium model are made, allowing for a more accurate description of the physical processes. The code allows for non-Boltzmann distributions of the electronic excited states by convecting separately each excited state, as a pseudo-specie. Each molecular state has also its own vibrational temperature, while a global rotational temperature is assumed. The free electron temperature is different from those of the excited states, and the electron heat conduction is also included. The CR model also uses a unique coupling between chemistry and vibrational energy (C-V coupling), which is fully coherent, and has the property of establishing thermal equilibrium as well as chemical equilibrium, on its own. We have also included a coupling between electronic excitations and vibrational energy (X-V coupling), which can have a strong influence on the vibrational temperature of some states. The recent improvements include the multi- temperature dependence of the chemical rates for associative ionization, as well as the estimation of the internal energies transferred during this process. Additionally, the distribution of energy into different translational modes (electron and heavy particles) is now correctly modeled. This provides a very rapid heating mechanism for the free electrons, since it is found that the electrons are generated with an average thermal energy of the same order as the heavy particle translational energy. This effect was observed by Gorelov et al in a recent paper, and lead to pronounced peaks in electron temperature immediately behind the shock. We will attempt ro reproduce this phenomenon. The last modification concerns the inclusion of the radiative terms into the calculations, thus enabling us to observe the effect of radiative losses and radiation transport. Preliminary tests have shown that the radiative losses are not negligible, i.e. the shock velocity drops when the radiative emission is included. In addition, we have observed some precursor excitation and ionization phenomena. These may be important at high shock velocities, and this will be investigated in detail. Precursor phenomena were also observed (in air) by Gorelov et al, and our results (for pure nitrogen) will be qualitatively compared with theirs.

Cambier, Jean-Luc↗

Non-Contact Conductivity Measurement for Automated Sample Processing Systems

A new method has been developed for monitoring and control of automated sample processing and preparation especially focusing on desalting of samples before analytical analysis (described in more detail in Automated Desalting Apparatus, (NPO-45428), NASA Tech Briefs, Vol. 34, No. 8 (August 2010), page 44). The use of non-contact conductivity probes, one at the inlet and one at the outlet of the solid phase sample preparation media, allows monitoring of the process, and acts as a trigger for the start of the next step in the sequence (see figure). At each step of the muti-step process, the system is flushed with low-conductivity water, which sets the system back to an overall low-conductivity state. This measurement then triggers the next stage of sample processing protocols, and greatly minimizes use of consumables. In the case of amino acid sample preparation for desalting, the conductivity measurement will define three key conditions for the sample preparation process. First, when the system is neutralized (low conductivity, by washing with excess de-ionized water); second, when the system is acidified, by washing with a strong acid (high conductivity); and third, when the system is at a basic condition of high pH (high conductivity). Taken together, this non-contact conductivity measurement for monitoring sample preparation will not only facilitate automation of the sample preparation and processing, but will also act as a way to optimize the operational time and use of consumables

Beegle, Luther W.↗

Mercury ion thruster research, 1977

The measured ion beam divergence characteristics of two and three-grid, multiaperture accelerator systems are presented. The effects of perveance, geometry, net-to-total accelerating voltage, discharge voltage and propellant are examined. The applicability of a model describing doubly-charged ion densities in mercury thrusters is demonstrated for an 8-cm diameter thruster. The results of detailed Langmuir probing of the interior of an operating cathode are given and used to determine the ionization fraction as a function of position upstream of the cathode orifice. A mathematical model of discharge chamber electron diffusion and collection processes is presented along with scaling laws useful in estimating performance of large diameter and/or high specific impluse thrusters. A model describing the production of ionized molecular nitrogen in ion thrusters is included.

Wilbur, P. J.↗

Electrospray Collection of Lunar Dust

A report describes ElectroSpray Ionization based Electrostatic Precipitation (ESIEP) for collecting lunar dust particles. While some HEPA filtration processes may remove a higher fraction (>99.9 percent) of the particles, the high efficiency may not be appropriate from an overall system standpoint, especially in light of the relatively large power requirement that such systems demand. The new electrospray particle capture technology is described as a variant of electrostatic precipitation that eliminates the current drawbacks of electrostatic precipitation. The new approach replaces corona prone field with a mist of highly charged micro-droplets generated by electrospray ionization (ESI) as the mechanism by which incoming particles are attracted and captured. In electrospray, a miniscule flow rate (microliters/minute) of liquid (typically water and a small amount of salt to enhance conductivity) is fed from the tip of a needle held at a high voltage potential relative to an opposite counter electrode. At sufficient field strength, a sharp liquid meniscus forms , which emits a jet of highly charged droplets that drift through the surrounding gas and are collected on the walls of a conductive tube. Particles in the gas have a high probability of contact with the droplets either by adhering to the droplets or otherwise acquiring a high level of charge, causing them to be captured on the collecting electrode as well. The spray acts as a filtration material that is continuously introduced and removed from the gas flow, and thus can never become clogged.

Dziekan, Michael↗