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At least 73 records · Page 4

Reaction Pathways and Energy Consumption in NH 3 Decomposition for H 2 Production by Low Temperature, Atmospheric Pressure Plasma

Pathways for NH 3 decomposition to N 2 and N 2 H 4 by atmospheric pressure nonthermal plasma are analyzed using a combination of molecular beam mass spectrometry measurements and zero-dimensional kinetic modeling. Experimental measurements show that NH 3 conversion and selectivity towards N 2 formation scale monotonically with the specific energy input into the plasma with ~ 100% selectivity to N 2 formation achieved at specific energy inputs above 0.12 J cm −3 (3.1 eV (molecule NH 3 ) −1 ). The kinetic model recovers these trends, although it underpredicts N 2 selectivity at low specific energy input. These discrepancies can be explained by the underestimation of reaction rate coefficients for reactions that consume N 2 H x species in collisions with H radicals and/or radial nonuniformities in power deposition, gas temperature, and species concentrations that are not represented by the plug flow approximation used in the model. The kinetic model shows that N 2 formation proceeds through N 2 H x decomposition pathways rather than NH x decomposition pathways in low temperature, atmospheric pressure plasma. Higher selectivity toward N 2 production can be achieved by operating at higher NH 3 conversion and with a higher gas temperature. Furthermore, the high energy cost of NH 3 decomposition by atmospheric pressure nonthermal plasma found in this work (25–50 eV (molecule NH 3 converted) −1 ; 17–33 eV (molecule H 2 formed) −1 ) is a result of the energy requirement for electron-impact dissociation of NH 3 and the significant re-formation of NH 3 by three-body recombination reactions between NH 2 and H.

Nonthermal plasma↗

The influence of autoionization accompanied by excitation on dielectronic recombination and ionization equilibrium

In the process of dielectronic recombination, the doubly excited state formed by radiationless capture may autoionize preferentially into an excited state of the recombining ion. This additional autoionization process has not been discussed in previous treatments of dielectronic recombination. The dielectronic recombination rates for certain nonhydrogenic Fe ions, although still larger than the direct radiative recombination rates, are found to be substantially reduced by the inclusion of the additional autoionization rate in the branching ratio for the stabilizing radiative transition. Consequently, the temperatures of maximum equilibrium abundance are significantly lower than those predicted by recent calculations. Finally, the radiative energy loss rate coefficients are calculated for radiation processes involving electron Fe-ion collisions in high-temperature plasmas. Electron impact excitation of resonance line radiation is the dominant radiative cooling mechanism in steady-state plasmas at temperatures where ions with bound electrons are abundant. However, it is found that the radiation emitted during dielectronic recombination can be more important than direct recombination radiation and bremsstrahlung.

Jacobs, V. L.↗

Feasibility of hydroxyl concentration measurements by laser-saturated fluorescence in high-pressure flames

The effect of pressure on the laser-saturated fluorescence method for measuring OH concentration in high-pressure flames is studied using calculations for the burned-gas region of a stoichiometric H2-O2 flame at 2000 K. A numerical model of the excitation dynamics of OH is developed to explore the validity of the balanced cross-rate model at higher pressures. It is shown that depopulation of the laser-coupled levels is sensitive to collisions which depopulate v-double-prime (VDP) = 0 and to rate coefficients for rotational transfer in the ground state which are smaller than those in the excited state. In particular, it is shown that the depopulation of VDP = 0, and hence the laser-coupled levels, depends on the probability of electronic quenching to vibrational levels for which VDP is greater than 0 and vibrational relaxation to VDP = 0.

Carter, Campbell D.↗

Departures of the electron energy distribution from a Maxwellian in hydrogen. I - Formulation and solution of the electron kinetic equation. II - Consequences

The problem of calculating the steady-state free-electron energy distribution in a hydrogen gas is considered in order to study departures of that distribution from a Maxwellian at sufficiently low degrees of ionization. A model kinetic equation is formulated and solved analytically for the one-particle electron distribution function in a steady-state partially ionized hydrogen gas, and it is shown that the formal solution can be accurately approximated by using the WKB method. The solutions obtained indicate that the high-energy tail of the distribution is susceptible to distortion by imbalanced inelastic collisions for ionization fractions not exceeding about 0.1 and that such departures from a Maxwellian can lead to significant changes in the collisional excitation and ionization rates of ground-state hydrogen atoms. Expressions for the electron-hydrogen collision rates are derived which explicitly display their dependence on the hydrogen departure coefficients. The results are applied in order to compare self-consistent predictions with those based on the a priori assumption of a Maxwellian distribution for models of the thermal ionization equilibrium of hydrogen in the optically thin limit, spectral-line formation by a gas consisting of two-level atoms, and radiative transfer in finite slabs by a gas of four-level hydrogen atoms.

Shoub, E. C.↗

Cross sections and rate coefficients for inelastic interactions of heavy particles

The existing analytical inelastic cross-sections for direct atom-atom ionizing collisions of Firsov (1959), Fleischmann et al. (1972), and Drawin (1968) are discussed. General analytical expressions for direct ionization cross-sections in atom-atom collisions are derived. The main advantage of the present cross-sections is their generality, simplicity, and overall accuracy, which is acceptable in most applications and is better than the overall accuracy of the cross-sections of Firsov, Fleischmann et al., and Drawin. The atom-atom interaction is considered as a superposition of all the pairwise interactions between the test particle and all the electrons of the outer nl shell of the target atom. Such a picture of atom-atom collision is acceptable at low- and medium-impact energies because then the electrons of the outer shell of the target atom are most likely the ones that get ionized. At high-impact energy, the picture becomes inaccurate because of strong overlapping of the atomic shells.

Kunc, J. A.↗

Impacts of aerosol size-dependent below-cloud scavenging on tropospheric aerosol in the NASA GEOS model

Wet deposition is the major sink for a suite of tropospheric aerosols, and thus largely affects the global distribution and lifetime of aerosols as well as the formation of clouds in the atmosphere. In this study, we implement the aerosol size-dependent below-cloud scavenging (BCS; washout) parameterization of Croft et al. (Atmos. Chem. Phys., 2009; hereafter referred to as C09) in the GOCART bulk aerosol scheme coupled with the NASA Goddard Earth Observing System (GEOS) model, and evaluate the simulated tropospheric aerosols against surface, airborne, and satellite observations. The current below-cloud scavenging in GOCART employs a first-order removal function with a constant scavenging coefficient that is independent of aerosol sizes and precipitation fluxes. The C09 BCS parameterization instead calculates aerosol below-cloud scavenging coefficients based on a size-dependent collision efficiency between aerosol particles and raindrops (or snow crystals). A look-up table of compiled collision efficiencies provides scavenging coefficients for sixty aerosol sizes and nine rain flux rates. We determine instantaneous coefficients according to the C09 BCS look-up table, precipitation fluxes, and a log-normal size distribution of aerosols. The implemented BCS parameterization tends to result in a large diversity of scavenging coefficient values with higher magnitudes, leading to more efficient scavenging. The model-simulated global mean tropospheric Pb-210 aerosol lifetime decreases from 7.4 days to 5.8 days. The separate consideration of rain and snow conditions in the scavenging coefficient lookup table leads to a bi-mode distribution of scavenging coefficients. These changes also cause increased mass fractions of smaller aerosols compared to the current simulation. We examine the impacts of the C09 BCS parameterization on the simulated aerosol vertical profiles, tropospheric lifetimes, and deposition fluxes through comparisons with NASA aircraft measurements (ATom), surface observations of aerosol concentrations (IMPROVE) and wet deposition fluxes (NADP and APQMP), and MODIS aerosol optical depth (AOD) retrievals.

Aerosols↗

Investigation of forbidden transitions in argon ions

An attempt has been made to observe the visible forbidden argon coronal lines at 553.6 nm (Ar X), 691.7 nm (Ar XI), 847.6 nm (Ar XIII), and 441.2 nm (Ar XIV) in a deuterium-argon plasma produced in a large theta pinch. The electron temperature (250 eV) and the electron density (5 by 10 to the 16th power per cu cm) were measured by Thomson scattering of ruby laser radiation. This temperature is adequate to produce ionization stages up to Ar XIV, as was verified by photographic observation of Ar XIV lines. No line corresponding to the coronal lines was observed from the high-temperature plasma, but lines with wavelengths very nearly identical to those of two of the forbidden transitions were observed; these lines were due to allowed transitions of Ar II in a cooler portion of the plasma. Calculation of rate coefficients in the Coulomb-Born approximation shows that for laboratory experiments, electron collisions are much more important than radiative decay in depopulating the upper state of the forbidden lines.

Jalufka, N. W.↗

Atomic Data and Spectral Line Intensities for Ar XII

Electron impact collision strengths; energy levels; oscillator strengths and spontaneous radiative decay rates are calculated for Ar XII. The configurations used are 2s(exp 2)2p(exp 3), 2s2p(exp4), 2p(exp 5), 2s22p23s, 2s(exp 2)2p(exp 2)3p, and 2s(exp 2)2p(exp 2)3d giving rise to 72 fine-structure levels in intermediate coupling. Collision strengths are calculated at five incident energies: 35,70, 105, 140 and 175 Ry. They are complemented by Coulomb-Born limits towards infinite collision energy for forbidden transitions and line strengths for optically allowed transitions. Excitation rate coefficients are calculated as a function of electron temperature by assuming a Maxwellian electron velocity distribution. Using the excitation rate coefficients and the radiative transition rates, statistical equilibrium equations for level populations are solved at electron densities covering the range of 10(exp 8)-101(exp 14) cm(exp -3) at an electron temperature of log T(sub e)/K = 6.4, corresponding to maximum abundance of Ar XII. Relative spectral line intensities are calculated.

Eissner, W.↗

Atomic Data and Spectral Line Intensities for Ar XII

Electron impact collision strengths, energy levels, oscillator strengths and spontaneous radiative decay rates are calculated for Ar XII. The configurations used are 2s(sup 2)p(sup 3), 2s(sup 2)p(sup 4), 2p(sup 5), 2s(sup 2)2p(sup 2)3s, 2s(sup 2)2p(sup 2)3p, and 2s(sup 2)2p(sup 2)3d giving rise to 72 fine-structure levels in intermediate coupling. Collision strengths are calculated at five incident energies: 35, 70, 105, 140 and 175 Ry. They are complemented by Coulomb-Born limits towards infinite collision energy for forbidden transitions and line strengths for optically allowed transitions. Excitation rate coefficients are calculated as a function of electron temperature by assuming a Maxwellian electron velocity distribution. Using the excitation rate coefficients and the radiative transition rates, statistical equilibrium equations for level populations are solved at electron densities covering the range of 10(exp 8)-10(exp 14)/cm(exp 3) at an electron temperature of log T(sub e)/K = 6.4, corresponding to maximum abundance of AR-XII. Relative spectral line intensities are calculated.

Eissner, W.↗

The origin of tektites.

Origin of Moung Nong type tektities detached by meteoritic impact, considering lunar origin based on diffusion rates in silicates

METEORITE COLLISION↗

Modeling of collision and coalescence of droplets during microgravity processing of Zn-Bi immiscible alloys

A population balance model is presented for the coarsening of the dispersed phase of liquid-liquid two-phase mixtures in microgravity due to gravity sedimentation and Marangoni migration, which lead to the collision and coalescence of droplets. The model is used to predict the evolution of the size distribution of the dispersed phase in a liquid-phase miscibility gap system, Zn-Bi, which has been used in a number of experimental microgravity processing studies in which significant phase segregation has been observed. The analysis shows that increasing the temperature gradient, gravity level, volume fraction of the dispersed phase, initial average drop radius, initial standard deviation of droplet radii, or the temperature coefficient of the interfacial tension leads to an increase in the rate of droplet growth due to collision and coalescence. Comparison of the distribution evolutions for unimodal and bimodal initial distributions shows that the latter yield significantly more rapid droplet growth. Finally, it is shown that droplet growth can be dramatically reduced with antiparallel orientation of the gravity vector and the temperature gradient, provided that the relative magnitude of these two vectors is properly chosen.

Davis, R. H.↗

Charge transfer and momentum exchange in exospheric D-H(+) and H-D(+) collisions

Mechanisms that control the escape of deuterium from planetary exospheres include the acceleration of D(+) in the polar wind, and the production of suprathermal D atoms through nonthermal collisions. In this paper we examine the effects of neutral-ion interactions involving deuterium and hydrogen on the velocity distribution of neutral D. A two-center scattering approximation is used as the basis for calculations of the differential cross sections for charge transfer and elastic scatter in collision of H with D(+) and of D with H(+) for ionosphere-exosphere collision energies below 10 e V. These data are used to derive temperature dependent rate coefficients for the charge transfer branches of these interactions, and to determine the effects of ion-neutral temperature differences on the rate of generation of suprathermal D through charge transfer and elastic scatter.

Hodges, R. R., Jr.↗

A Symmetric Time-Varying Cluster Rate of Descent Model

A model of the time-varying rate of descent of the Orion vehicle was developed based on the observed correlation between canopy projected area and drag coefficient. This initial version of the model assumes cluster symmetry and only varies the vertical component of velocity. The cluster fly-out angle is modeled as a series of sine waves based on flight test data. The projected area of each canopy is synchronized with the primary fly-out angle mode. The sudden loss of projected area during canopy collisions is modeled at minimum fly-out angles, leading to brief increases in rate of descent. The cluster geometry is converted to drag coefficient using empirically derived constants. A more complete model is under development, which computes the aerodynamic response of each canopy to its local incidence angle.

Ray, Eric S.↗

Electron recombination of rotationally cold D 2 H + ions

Dissociative recombination (DR) of electrons with small molecular ions is a fundamental process for the physics and chemistry of the interstellar medium and planetary atmospheres. In previous DR studies, detailed analysis of the experimental rate coefficients has been hindered by the difficulty of preparing the ions in well-defined quantum states. For polyatomic ions in particular, truly state-selective measurements have been elusive, allowing only qualitative benchmarks of theory. Here, we present DR studies of the deuterated triatomic hydrogen ion D 2 H + , where the molecular ions were stored for up to 1000 seconds inside the Cryogenic Storage Ring (CSR) prior to the DR measurements. Our experiments with rotationally cold D 2 H + ions allow for detailed comparison to state-of-the-art theoretical calculations. We obtain very good agreement between experiment and theory even in the important collision energy range from 1 meV to 0.5 eV, where a multitude of Rydberg resonances reveal their imprint on the rate coefficient.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Altitude Variation of the CO2(V2)-O Quenching Rate Coefficient in Mesosphere and Lower Thermosphere

Among the processes governing the energy balance in the mesosphere and lower thermosphere (MLT), the quenching of CO2(v2) vibrational levels by collisions with oxygen atoms plays an important role. However, the k(CO2-O) values measured in the lab and retrieved from atmospheric measurements vary from 1.5 x 10(exp -12)cu cm/s through 9.0 x 10(exp -12)cu cm/s that requires further studying. In this work we used synergistic data from a ground based lidar and a satellite infrared radiometer to estimate k(CO2-O). We used the night- and daytime temperatures between 80 and 110 km measured by the Colorado State University narrow-band sodium (Na) lidar located at Fort Collins, Colorado (41 N, 255E) as ground truth of the SABER/TIMED nearly simultaneous ( +/-10 minutes) and common volume (within +/-1 degree in latitude, +/-2 degrees in longitude) observations. For each altitude in 80-110 km interval we estimate an 'optimal" value of k(CO2-O) needed to minimize the discrepancy between the simulated 15 micron CO2 radiance and that measured by the SABER/TIMED instrument. The k(CO2-O) obtained in this way varies in altitude from 3.5 x 10(exp -12)cu cm/s at 80 km to 5.2 x 10(exp -12)cu cm/s for altitudes above 95 km. We discuss this variation of the rate constant and its impact on temperature retrievals from 15 pm radiance measurements and on the energy budget of MLT.

Feofilov, A.↗

Altitude Variation of the CO2 (V2)-O Quenching Rate Coefficient in Mesosphere and Lower Thermosphere

Among the processes governing the energy balance in the mesosphere and lower thermosphere (mlt), the quenching of CO2(N2) vibrational levels by collisions with oxygen atoms plays an important role. However, the k(CO2-O) values measured in the lab and retrieved from atmospheric measurements vary from 1.5 x 10(exp -12) cubic centimeters per second through 9.0 x 10(exp -12) cubic centimeters per second that requires further studying. In this work we used synergistic data from a ground based lidar and a satellite infrared radiometer to estimate K(CO2-O). We used the night- and daytime temperatures between 80 and 110 km measured by the colorado state university narrow-band sodium (Na) lidar located at fort collins, colorado (41N, 255E) as ground truth of the saber/timed nearly simultaneous (plus or minus 10 minutes) and common volume (within plus or minus 1 degree in latitude, plus or minus 2 degrees in longitude) observations. For each altitude in 80-110 km interval we estimate an "optimal" value of K(CO2-O) needed to minimize the discrepancy between the simulated 15 mm CO2 radiance and that measured by the saber/timed instrument. The K(CO2-O) obtained in this way varies in altitude from 3.5 x 10(exp -12) cubic centimeters per second at 80 km to 5.2 x 10(exp -12) cubic centimeters pers second for altitudes above 95 km. We discuss this variation of the rate constant and its impact on temperature retrievals from 15 mm radiance measurements and on the energy budget of mlt.

Feofilovi, Artem↗

Atomic Data and Spectral Line Intensities for Ni XXI

Electron impact collision strengths, energy levels, oscillator strengths and spontaneous radiative decay rates are calculated for Ni XXI. The configurations used are 2s(sup 2)2p(sup 4), 2s2p(sup 5), 2p(sup 6), 2s(sup 2)2p(sup 3)3s, and 2s(sup 2)3p(sup 3)3d giving rise to 58 fine-structure levels in intermediate coupling. Collision strengths are calculated at five incident energies, 85, 170, 255, 340, and 425 Ry. Excitation rate coefficients are calculated by assuming a Maxwellian electron velocity distribution at an electron temperature of log T(sub e)(K)=6.9, corresponding to maximum abundance of Ni XXI. Using the excitation rate coefficients and the radiative transition rates, statistical equilibrium equations for level populations are solved at electron densities 10(exp 8)-10(exp 14) per cubic centimeter. Relative spectral line intensities are calculated. Proton excitation rates between the lowest three levels have been included in the statistical equilibrium equations. The predicted intensity ratios are compared with available observations.

Bhatia, A. K.↗