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Turbulent boundary layer effects on chemical and kinetic measurements of gas mixture composition from nonuniform shock tube flow
Laminar boundary layers effect on chemical-kinetic measurements in shock tube, applying correction by computer program for subsonic diffuser
A generalized methodology currently employed at JPL, was used to develop an analytical model for effects of high-energy electrons and interactions between electron and ultraviolet effects. Chemical kinetic concepts were applied in defining quantifiable parameters; the need for determining short-lived transient species and their concentration was demonstrated. The results demonstrates a systematic and cost-effective means of addressing the issues and show qualitative and quantitative, applicable relationships between space radiation and simulation parameters. An equally important result is identification of critical initial experiments necessary to further clarify the relationships. Topics discussed include facility and test design; rastered vs. diffuse continuous e-beam; valid acceleration level; simultaneous vs. sequential exposure to different types of radiation; and interruption of test continuity.
There is a growing practical and theoretical interest in developing accurate macroscopic modelling for flows arising in chemical or physical vapor transport (VT) crystal growth experiments, including those conducted in reduced gravity environments. Rosner was the first person to point out that previously neglected rarefield gas dynamics phenomena (Stefan and bouyancy-driven flows) become rather important sources of convection. In particular, the combination of rarefaction and strong gradients of temperature (and/or concentration) tangential to the side-walls of the ampoule induces convective flows known as thermal (and concentration) 'creep' respectively. His order-of-magnitude estimates revealed that thermal creep effects can be non-negligible even at normal gravitational levels. On the macroscopic level, the bulk fluid mechanics can be adequately described by the familiar macroscopic equations as long as the boundary conditions are modified to account for the integrated effect of kinetic boundary layers adjacent to solid boundaries. Motivated by the growing importance of these phenomena, we have embarked on a series of computational studies to elucidate these fundamental creep-induced effects for a rarefied gas in simple, two-dimensional confined geometries. However, unlike previous related studies, we resort to a microscopic description of the gas, mathematically expressed by the Boltzmann integro-differential equation. We employ the direct simulation Monte Carlo (DSMC) method of Bird, the theoretical foundations and several practical applications. In the case of thermally induced flows, the no-time counter method of Bird is used, as implemented for a hard-sphere gas. The scheme has been also extended to account for realistic molecular interaction models, an extension necessary if the diffusion physics underlying concentration creep are to be captured.
Fluorescence in situ hybridization with a composite probe for human chromosome 4 and a probe that stained all centromeres was used to study gamma-ray induced breakage, rejoining and misrejoining in prematurely condensed chromosomes in human lymphocytes. Dose-response curves for the induction of all types of aberrations in prematurely condensed human chromosomes 4 were determined immediately after irradiation and after 8 h postirradiation incubation. In addition, aberrations were measured after various incubation times from 0 to 18 h after a dose of 7 Gy. Unrejoined chromosome breaks were the most frequent type of aberration observed immediately after irradiation. Approximately 15% of total aberrations observed were chromosome exchanges. After 8 h postirradiation incubation, the frequency of breaks in prematurely condensed chromosomes declined to about 20% of the initial value, and chromosomal exchanges became the most frequent aberration. Results of metaphase analysis were similar to those for prematurely condensed chromosomes after 8 h incubation with the exception that a significantly lower frequency of fragments was observed. Symmetrical and asymmetrical interchanges were found at similar frequencies at all doses. No complex exchanges were observed in lymphocyte chromosomes immediately after exposure. They accounted for about 1% of total exchanges in metaphase chromosomes at doses <3 Gy and about 14% at 7 Gy. Incomplete exchanges amounted to approximately 15% of total exchanges at all doses. The kinetics of break rejoining was exponential, and the frequency of exchanges increased with kinetics similar to that observed for the rejoining of the breaks. This increase in the total exchanges as a function of the time between irradiation and fusion was due to a rapid increase in reciprocal interchanges, and a slower increase in complex exchanges; the frequency of incomplete exchanges increased initially, then decreased with prolonged incubation to the level observed in metaphase. It is concluded that the formation of each kind of chromosome aberrations follows different kinetics.
The stability of collisionless tearing modes is examined in the presence of curvature drift resonances and the trapped particle effects. A kinetic description for both electrons and ions is employed to investigate the stability of a two-dimensional equilibrium model. The main features of the study are to treat the ion dynamics properly by incorporating effects associated with particle trajectories in the tail fields and to include the linear coupling of trapped particle modes. Generalized dispersion relations are derived in several parameter regimes by considering two important sublayers of the reconnecting region. For a typical choice of parameters appropriate to the current sheet region, we demonstrate that localized tearing modes driven by ion curvature drift resonance effects are excited in the current sheet region with growth time of the order of a few seconds. Also, we examine nonlocal characteristics of tearing modes driven by curvature effects and show that modes growing in a fraction of a second arise when mode widths are larger than the current sheet width. Further, we show that trapped particle effects, in an interesting frequency regime, significantly enhance the growth rate of the tearing mode. The relevance of this theory for substorm onset phase and other features of the substorms is briefly discussed.
No abstract available
Recent evidence has indicated a significant role for the cGMP second messenger system in vertebrate olfactory transduction but no clear functions have been identified for cGMP so far. Here, we have examined the effects of 8-Br-cGMP and carbon monoxide (CO) on odour responses of salamander olfactory receptor neurons using perforated patch recordings. We report that 8-Br-cGMP strongly down-regulates the odour sensitivity of the cells, with a K1/2 of 460 nM. This adaptation-like effect can be mimicked by CO, an activator of soluble guanylyl cyclase, with a K1/2 of 1 microM. Sensitivity modulation is achieved through a regulatory chain of events in which cGMP stimulates a persistent background current due to the activation of cyclic nucleotide-gated channels. This in turn leads to sustained Ca2+ entry providing a negative feedback signal. One consequence of the Ca2+ entry is a shift to the right of the stimulus-response curve and a reduction in saturating odour currents. Together, these two effects can reduce the sensory generator current by up to twenty-fold. Thus, cGMP functions to control the gain of the G-protein coupled cAMP pathway. Another consequence of the action of cGMP is a marked prolongation of the odour response kinetics. The effects of CO/cGMP are long-lasting and can continue for minutes. Hence, we propose that cGMP helps to prevent saturation of the cell's response by adjusting the operational range of the cAMP cascade and contributes to olfactory adaptation by decreasing the sensitivity of olfactory receptor cells to repeated odour stimuli.
Triple oxygen isotope methods (e.g., using δ 18 O, and Δ′ 17 O) have been used to classify meteorites, to constrain atmospheric chemistry, and to estimate primary productivity, among other uses. Such utility relies on the mass dependency of most chemical reactions: δ 17 O is proportional to δ 18 O by roughly a factor of 0.5. However, in detail, mass-dependency factors vary. While constraints on mass dependency are well established for equilibrium isotope effects, similar constraints for kinetic isotope effects are lacking. Using an ab initio Monte Carlo approach (see envelopes in Figure 1), we find the range of kinetic isotope effects (i.e., resulting from unidirectional chemical reactions) contains and exceeds the range of accessible equilibrium isotope effects for the 16 O 17 O 18 O system (Hayles and Killingsworth, 2022). Accessible kinetic isotope effects can yield Δ′ 17 O variations as large 0.8 ‰ from a single kinetic fractionation step. Reactions that yield the largest deviations from equilibrium are those with the largest molecular mass difference between decomposition fragments, typically the two products such as a gas and solid generated from the thermal decomposition of an initial solid. Comparison of DFT transition state model results against previously published experiments on the thermal decomposition of calcite (CaCO 3 ) (Miller et al., 2002) and dehydroxylation of brucite (Mg(OH) 2 ) (Clayton and Mayeda, 2009) show they are matched with mass-dependent kinetic isotope effects. This approach can be applied to any system with more than two isotopes.
Merchant and Davis performed a linear stability analysis on a model for the directional solidification of a dilute binary alloy valid for all speeds. The analysis revealed that nonequilibrium segregation effects modify the Mullins and Sekerka cellular mode, whereas attachment kinetics has no effect on these cells. In this paper, the nonlinear stability of the steady cellular mode is analyzed. A Landau equation is obtained that determines the amplitude of the cells. The Landau coefficient here depends on both nonequilibrium segregation effects and attachment kinetics. This equation gives the ranges of parameters for subcritical bifurcation (jump transition) or supercritical bifurcation (smooth transition) to cells.
The results from studies on polar wind ion heating due to kinetic ion beam instabilities and the effects of such ion heating on the outflow of O(+) in the polar wind are presented and discussed. First, the linear instabilities associated with an O(+) and H(+) polar wind plasma in the presence of O(+) and H(+) beams for a range of O(+)/H(+) beam densities, T(sub e)/T(sub i), and ion beam speeds were examined. Then, nonlinear heating of the polar wind ions was studied, using numerical simulations. The O(+) and H(+) polar wind ions were modeled by isotropic Maxwellian distributions, and the electrons, O(+) beams, and H(+) beams were modeled by drifting Maxwellian distributions. The effects of the kinetic ion heating on the outflow of the polar wind ions were examined from the ionosphere, using a time-dependent hydrodynamic model. A numerical code to solve the O(+) and H(+) continuity and momentum equations in a flux tube from ionospheric to magnetospheric altitudes were developed. The effects of ion heating were included by allowing for the altitudinal variation of the ion temperatures in the momentum equation. The ion temperature profiles were specified based on the ion heating characteristics found from previous kinetic simulations. It was assumed that heating occurred above 1500 km and increased to a saturated value of temperature that was obtained directly from the kinetic simulation study. The characteristics of the dynamical polar wind without ion heating were studied, and a flux tube on closed field lines that suddenly became open at t = 0 was simulated. Then, the effects of ion heating were included. To gain some physical insight, two limiting cases were considered: preferential H(+) heating and preferential O(+) heating. How O(+) heating can lead to enhanced polar wind O(+) fluxes in the polar magnetosphere is shown.
Stable isotope ratio measurements are a powerful tool used to understand both ancient and modern planetary processes. Instruments on the Cassini- Huygens spacecraft along with ground-based observations have measured several isotope pairs, including C-13/C-12 and N-15/N-14, in Titan's atmosphere. This includes isotopic measurements of the major atmospheric species, CH4 and N2, along with HCN, HC3N, C2H2. C2H6 and C4H2. However, the isotopic fractionation of Titan's organic aerosol has not conclusively been measured and therefore the effect of aerosol formation as an isotopic fractionation pathway in Titan's atmosphere has not been considered. Laboratory studies have measured the carbon and/or nitrogen isotopic fractionation of Titan aerosol analogs. [18] found that the carbon fractionation of photochemical organic aerosol analogs are more enriched in C-13. This enrichment in the aerosol analogs is opposite of what is predicted for photochemical products by the kinetic isotope effect. Additionally, both [16] and [18] found that the nitrogen fractionation in the organic aerosol analogs are opposite of what is observed in Titan's atmospheric N2 and HCN, with the aerosol analogs being a light nitrogen sink. Here we monitor the gas phase during photochemical aerosol analog production as a function of reaction time. In a recirculation experiment, the isotopic fractionation of carbon within the gas-phase products is measured as the CH4 reservoir is depleted. This allows us to monitor the isotopic fractionation pathway during photochemical aerosol analog formation.
The objectives of Phase 1 were to evaluate analytically and experimentally the operation, performance, and lifetime of arcjet thrusters operating between 0.5 and 3.0 kW with catalytically decomposed hydrazine (N2H4) and to begin development of the requisite power control unit (PCU) technology. Fundamental analyses were performed of the arcjet nozzle, the gas kinetic reaction effects, the thermal environment, and the arc stabilizing vortex. The VNAP2 flow code was used to analyze arcjet nozzle performance with non-uniform entrance profiles. Viscous losses become dominant beyond expansion ratios of 50:1 because of the low Reynolds numbers. A survey of vortex phenomena and analysis techniques identified viscous dissipation and vortex breakdown as two flow instabilities that could affect arcjet operation. The gas kinetics code CREK1D was used to study the gas kinetics of high temperature N2H4 decomposition products. The arc/gas energy transfer is a non-equilibrium process because of the reaction rate constants and the short gas residence times. A thermal analysis code was used to guide design work and to provide a means to back out power losses at the anode fall based on test thermocouple data. The low flow rate and large thermal masses made optimization of a regenerative heating scheme unnecessary.
It has been suggested that in photon-dominated regions, oxygen chemistry is initiated by the O+H2 yields OH+H reaction. The reaction has an energy barrier of about 0.4 eV with ground state reactants and it is slow at low temperatures. There is strong experimental evidence that vibrational excitation of the H2 molecule increases the reactivity significantly. We present extensive quantum calculations of cross sections and rate coefficients for the O+H2(v) reaction for v = 0 - 3 of the H2 molecule and show that the vibrational excitation of the molecule has a significant effect on reactivity, especially at low temperatures.
DNA double-strand breaks (DSBs) were measured within a 3.2-Mbp NotI fragment on chromosome 21 of cells of a normal human fibroblast cell line. Correct rejoining of DSBs was followed by measuring reconstitution of the original-size NotI fragment, and this was compared to total rejoining as measured by a conventional pulsed-field gel electrophoresis technique (FAR assay). After 80 Gy of particle irradiations with LETs in the range of 7-150 keV/microm, it was found that the repair kinetics was generally slower after irradiation with high-LET particles compared to X irradiation and that a larger proportion of the breaks remained unrepaired after 24 h. On the other hand, the misrejoining frequency as measured by the difference between correct and total rejoining after 24 h did not change with LET, but was approximately the same for all radiations at this dose, equal to 25-30% of the initial breaks. This result is discussed in relation to formation of chromosomal aberrations, deletion mutations and other biological end points.
The isotope effects associated with: (1) formation of H2S from HS- by protonation in aqueous solution; and (2) volatilization of H2S have been experimentally determined. Both isotopic distributions in closed systems at equilibrium and differential rates of volatilization of isotopic species in open systems were measured at 22 +/- 1 degrees C. It was found that, at equilibrium aqueous H2S is enriched in 34S by 2.0 - 2.7% relative to HS- and that H2S volatilized from solution is depleted in 34S by 0.5% relative to dissolved H2S. A small kinetic isotope effect accompanying volatilization of H2S was observed in the open-system experiments.
Both chromium and iron couples were studied on various electrode surfaces in acidic perchlorate solution by using rotating ring-disk techniques. It was found that chloride which forms inner sphere coordination complexes with the redox species enhances the electrode kinetics dramatically. The effects of lead underpotential deposition and surface alloy formation on the kinetics of the chromium couple on gold were studied using both linear sweep voltammetry and potential step techniques. The lad underpotential deposition was found to slow down the kinetics of the reduction of the Cr species on gold surfaces although increase the hydrogen overvoltage. The effect on the chromium kinetics can be explained in terms of principally a double layer effect. The underpotential deposition lead species with its positive charge results in a decrease in the concentration of the Cr species at the electrode surface. Similar phenomena were also observed with bismuth underpotential deposition on gold for the iron couple.
The aqueous phase oxidation of acetic acid, used as a model compound for the treatment of CELSS (Controlled Ecological Life Support System) waste, was carried out in the monolith froth reactor which utilizes two-phase flow in the monolith channels. The catalytic oxidation of acetic acid was carried out over a Pt/Al2O3 catalyst at temperatures and pressures below the critical point of water. The effect of externally controllable parameters (temperature, liquid flow rate, distributor plate orifice size, pitch, and catalyst distance from the distributor plate) on the rate of acetic acid oxidation was investigated. Results indicate reaction rate increased with increasing temperature and exhibited a maximum with respect to liquid flow rate. The apparent activation energy calculated from reaction rate data was 99.7 kJ/mol. This value is similar to values reported for the oxidation of acetic acid in other systems and is comparable to intrinsic values calculated for oxidation reactions. The kinetic data were modeled using simple power law kinetics. The effect of "froth" feed system characteristics was also investigated. Results indicate that the reaction rate exhibits a maximum with respect to distributor plate orifice size, pitch, and catalyst distance from the distributor plate. Fundamental results obtained were used to extrapolate where the complete removal of acetic acid would be obtained and for the design and operation of a full scale CELSS treatment system.