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NASA NTRS2018

Stable Isotope Fractionation in Titan Aerosol Formation

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.

Ugelow, M. S.↗

NASA NTRS2009

Lightning and Mass Independent Oxygen Isotopic Fractionation in Nebular Silicates

Lightning has long been postulated as the agent of Chondru|e formation in the solar nebula, but it may have an additional role to play as well. Lightning bolts of almost any scale will both vaporize dust and liberate oxygen atoms that will then interact with both nebular gases as well as the refractory silicate vapor as it re-condenses. Such processes should result in the addition of the heavy oxygen isotopes to the growing silicate grains while the light oxygen-16 becomes part of the gas phase water. This process will proceed to some extent throughout the history of any turbulent nebula and will result in the gradual increase of O-16 in the gas phase and in a much larger relative increase in the O-17 and O-18 content of the nebular dust. Laboratory experiments have demonstrated the production of such "heavy oxygen enriched", non-mass-dependently-fractionated dust grains in a high voltage discharge in a hydrogen rich gas containing small quantities of silane, pentacarbonyl iron and oxygen.

Nuth, Joseph A.↗

NASA NTRS1981

Influence of hydrogen chemisorption kinetics on the interpretation of hydrogen transport through iron membranes

The influence of a specific surface reaction on the transport of gas-phase hydrogen through iron membranes has been investigated on the basis of model calculations. The surface reaction involves an adsorbed molecular hydrogen precursor between the gas phase and the dissociated chemisorbed state. The calculations demonstrate that the surface reaction for the H2/Fe system makes significant contributions to the time delay associated with the transient hydrogen transport through iron membranes, even under conditions where the steady-state hydrogen transport is independent of the surface reaction. These contributions to the time delay are interpreted in terms of an effective diffusivity, which is a function of the pressure on the entrance side and the thickness of the membrane.

Shanabarger, M. R.↗

NASA NTRS1996

Phoretic and Radiometric Force Measurements on Microparticles in Microgravity Conditions

Thermophoretic, diffusiophoretic and radiometric forces on microparticles are being measured over a wide range of gas phase and particle conditions using electrodynamic levitation of single particles to simulate microgravity conditions. The thermophoretic force, which arises when a particle exists in a gas having a temperature gradient, is measured by levitating an electrically charged particle between heated and cooled plates mounted in a vacuum chamber. The diffusiophoretic force arising from a concentration gradient in the gas phase is measured in a similar manner except that the heat exchangers are coated with liquids to establish a vapor concentration gradient. These phoretic forces and the radiation pressure force acting on a particle are measured directly in terms of the change in the dc field required to levitate the particle with and without the force applied. The apparatus developed for the research and the experimental techniques are discussed, and results obtained by thermophoresis experiments are presented. The determination of the momentum and energy accommodation coefficients associated with molecular collisions between gases molecules and particles and the measurement of the interaction between electromagnetic radiation and small particles are of particular interest.

Davis, E. James↗

NASA NTRS1992

Effect of gas mass flux on cryogenic liquid jet breakup

A scattered-light scanning instrument developed at NASA Lewis Research Center was used to measure the characteristic drop size of clouds of liquid nitrogen droplets. The instrument was calibrated with suspensions of monosized polystyrene spheres. In this investigation of the mechanism of liquid nitrogen jet disintegration in a high-velocity gas flow, the Sauter mean diameter, D32, was found to vary inversely with the nitrogen gas mass flux raised to the power 1.33. Values of D32 varied from 5 to 25 microns and the mass flux exponent of 1.33 agrees well with theory for liquid jet breakup in high-velocity gas flows. The loss of very small droplets due to the high vaporization rate of liquid nitrogen was avoided by sampling the spray very close to the atomizer, i.e., 1.3 cm downstream of the nozzle orifice. The presence of high velocity and thermal gradients in the gas phase also made sampling of the particles difficult. As a result, it was necessary to correct the measurements for background noise produced by both highly turbulent gas flows and thermally induced density gradients in the gas phase.

Ingebo, R. D.↗

NASA NTRS1994

Ion-assisted tropospheric OH measurement technique

The present technique measures atmospheric OH concentrations by first titrating OH into isotopically labeled H2(exp 34)SO4 by a series of gas phase reactions in an effectively wall-less flow tube reactor on a time-scale which is short in comparison to the OH lifetime. The gas phase H2SO4 concentration is then determined by reacting it with NO3(-)(center dot)HNO3 ions in a flow tube, and subsequently measuring the resulting (HSO4(-))/(NO3(-)) ion ratio. Since the determination of H2SO4 concentration does not depend on the measurement of an absolute photon flux or chemical concentration but rather only on the relative concentration measurement of two fairly similar mass ions in conjunction with a fixed reaction time and reaction rate coefficient, no in-field calibration technique should be required. The ion-assisted OH measurement technique provides a concentration measurement about once each 10 to 20 seconds and had a detection sensitivity less than or equal to 1 x 10(exp 5) molecules/cu cm (2 standard deviations) with an integration time of 5 minutes during the past field study. Typically, the total background signal level is in the low 10(exp 6) molecule/cu cm range with the scatter in this background (or background noise in 5 minutes) in the mid 10(exp 4) molecules/cu cm range.

Eisele, Fred L.↗

NASA NTRS1999

Development of an Advanced Computational Model for OMCVD of Indium Nitride

An advanced computational model is being developed to predict the formation of indium nitride (InN) film from the reaction of trimethylindium (In(CH3)3) with ammonia (NH3). The components are introduced into the reactor in the gas phase within a background of molecular nitrogen (N2). Organometallic chemical vapor deposition occurs on a heated sapphire surface. The model simulates heat and mass transport with gas and surface chemistry under steady state and pulsed conditions. The development and validation of an accurate model for the interactions between the diffusion of gas phase species and surface kinetics is essential to enable the regulation of the process in order to produce a low defect material. The validation of the model will be performed in concert with a NASA-North Carolina State University project.

Cardelino, Carlos A.↗

NASA NTRS2003

Low Stretch Solid-Fuel Flame Transient Response to a Step Change in Gravity

The effect of a step change in gravity level on the stability of low stretch diffusion flames over a solid fuel is studied both numerically and experimentally. Drop tower experiments have been conducted in NASA Glenn Research Center's 5.2 Zero Gravity Facility. In the experiments burning PMMA cylinders, a dynamic transition is observed when the steadily burning 1g flame is dropped and becomes a 0g flame. To understand the physics behind this dynamic transition, a transient stagnation point model has been developed which includes gas-phase radiation and solid phase coupling to describe this dynamic process. In this paper, the experimental results are compared with the model predictions. Both model and experiment show that the interior of the solid phase does not have time to change significantly in the few seconds of drop time, so the experimental results are pseudo-steady in the gas-phase, but the solid is inherently unsteady over long time scales. The model is also used to examine the importance of fractional heat losses on extinction, which clearly demonstrates that as the feedback from the flame decreases, the importance of the ongoing heat losses becomes greater, and extinction is observed when these losses represent 80% or more of the flame feedback.

Armstrong, J. B.↗

NASA NTRS2009

First Spectroscopic Identification of Massive Young Stellar Objects in the Galactic Center

We report the detection of several molecular gas-phase and ice absorption features in three photometrically-selected young stellar object (YSO) candidates in the central 280 pc of the Milky Way. Our spectra, obtained with the Infrared Spectrograph (IRS) onboard the Spitzer Space Telescope, reveal gas-phase absorption from CO2 (15.0 microns), C2H2 (13.7 microns) and HCN (14.0 microns). We attribute this absorption to warm, dense gas in massive YSOs. We also detect strong and broad 15 microns CO2 ice absorption features, with a remarkable double-peaked structure. The prominent long-wavelength peak is due to CH3OH-rich ice grains, and is similar to those found in other known massive YSOs. Our IRS observa.tions demonstra.te the youth of these objects, and provide the first spectroscopic identification of massive YSOs in the Galactic Center.

An, Deokkeun↗

NASA NTRS1987

Elucidation of the organometallic vapor phase epitaxial growth mechanism for InP

A new technique for tracing the organometallic vapor epitaxial growth is reported. The pyrolysis of PH3, alone and in the presence of trimethylindium (TMIn), and of TMIn alone was studied by conducting the epitaxial growth of InP in D2 as the carrier gas, tracing growth reactions by mass spectrometric analysis of the product molecules. The TMIn alone pyrolyzes mostly homogeneously in the gas phase, while the PH3 pyrolysis is completely heterogeneous at the InP surface. Adding TMIn to PH3 results in a dramatic decrease in the pyrolysis temperature. PH3 molecules which interact with TMIn in the gas phase pyrolyze at temperatures as low as 250, and those decomposing without TMIn interaction pyrolyze at temperatures approximately 200 C higher. Similarly, the presence of PH3 lowers the TMIn pyrolysis temperature by at least 50 C. TMIn alone in D2 produces mainly CH3D molecules. For high PH3:TMIn ratios, CH4 is the only carbon-containing reaction product.

Buchan, N. I.↗

NASA NTRS1982

The free radical chemistry of cloud droplets and its impact upon the composition of rain

Calculations are presented that simulate the free radical chemistries of the gas phase and aqueous phase within a warm cloud during midday. It is demonstrated that in the presence of midday solar fluxes, the heterogeneous scavenging of OH and HO2 from the gas phase by cloud droplets can represent a major source of free radicals to cloud water, provided the accommodation or sticking coefficient for these species impinging upon water droplets is not less than 0.0001. The aqueous-phase of HO2 radicals are found to be converted to H2O2 by aqueous-phase chemical reactions at a rate that suggests that this mechanism could produce a significant fraction of the H2O2 found in cloud droplets. The rapid oxidation of sulfur species dissolved in cloudwater by this free-radical-produced H2O2 as well as by aqueous-phase OH radicals could conceivably have a significant impact upon the chemical composition of rain.

Chameides, W. L.↗

NASA NTRS1990

Surface characterization of hydrogen charged and uncharged alpha-2 and gamma titanium aluminide alloys using AES and REELS

The surfaces of selected uncharged and hydrogen charged alpha-2 and gamma titanium aluminide alloys with Nb additions were characterized by Auger electron (AES) and reflected electron energy loss (REELS) spectroscopy. The alloy surfaces were cleaned before analysis at room temperature by ion sputtering. The low energy (500 eV) ion sputtering process preferentially sputtered the surface concentration. The surface concentrations were determined by comparing AES data from the alloys with corresponding data from elemental references. No differences were observed in the Ti or Nb Auger spectra for the uncharged and hydrogen charged alloys, even though the alpha-2 alloy had 33.4 atomic percent dissolved hydrogen. Also, no differences were observed in the AES spectra when hydrogen was adsorbed from the gas phase. Bulk plasmon energy shifts were observed in all alloys. The energy shifts were induced either by dissolved hydrogen (alpha-2 alloy) or hydrogen adsorbed from the gas phase (alpha-2 and gamma alloys). The adsorption induced plasmon energy shifts were greatest for the gamma alloy and cp-Ti metal.

Shanabarger, M. R.↗

NASA NTRS1990

Optical characterization of clouds of fine liquid-nitrogen particles

Characteristic drop size, D sub 32, of clouds of fine liquid nitrogen particles was measured with a scattered light scanning instrument developed at NASA-Lewis. Calibration of the instrument was accomplished with suspensions of monosized polystyrene spheres and the scattered light scanner was then used to investigate the mechanism of liquid nitrogen jet disintegration in high velocity gas flow. The Sauter mean diameter, D sub 32, was found to vary inversely with nitrogen gas mass-flux raised to the 1.33 power. Values of D sub 32 varied from 5 to 25 microns and the mass-flux exponent 1.33 agrees well with theory for liquid jet breakup in high velocity gas flow. Loss of fine particles due to the high vaporization rate of liquid nitrogen was avoided by sampling the spray 1.3 cm downstream of the nozzle orifice. The presence of high velocity and thermal gradients in the gas phase also made sampling of the particles quite difficult. As a result, it was necessary to correct the measurements for background noise produced by both highly turbulent gas flow and thermally induced density gradients in the gas phase.

Ingebo, Robert D.↗

NASA NTRS2000

Candle Flames in Non-Buoyant Atmospheres

This paper addresses the behavior of a candle flame in a long-duration, quiescent microgravity environment both on the space Shuttle and the Mir Orbiting Station. On the Shuttle, the flames became dim blue after an initial transient where there was significant yellow (presumably soot) in the flame. The flame lifetimes were typically less than 60 seconds. The safety-mandated candlebox that contained the candle flame inhibited oxygen transport to the flame and thus limited the flame lifetime. The flames on the Mir were similar, except that the yellow luminosity persisted longer into the flame lifetime because of a higher initial oxygen concentration, The Mir flames burned for as long as 45 minutes. The difference in the flame lifetime between the Shuttle and Mir flames was primarily the redesigned candlebox that did not inhibit oxygen transport to the flame. In both environments, the flame intensity and the height-to-width ratio gradually decreased as the ambient oxygen content in the sealed chamber slowly decreased. Both sets of experiments showed spontaneous, axisymmetric flame oscillations just prior to extinction. The paper also presents a numerical model of a candle flame. The formulation is two-dimensional and time-dependent in the gas phase with constant specific heats, thermal conductivity and Lewis number (although different species can have different Lewis numbers), one-step finite-rate kinetics, and gas-phase radiative losses from CO2 and H2O. The treatment of the liquid/wick phase assumes that the, fuel evaporates from a constant diameter sphere connected to an inert cone. The model predicts a steady flame with a shape and size quantitatively similar to the Shuttle and Mir flames. The computation predicts that the flame size will increase slightly with increasing ambient oxygen mole fraction. The model also predicts pre-extinction flame oscillations if the rate of decrease in ambient oxygen is small enough, such as that which would occur for a flame burning in a sealed ambient.

Dietrich, D. L.↗

NASA NTRS1977

Combustion response modeling for composite solid propellants

A computerized mathematical model of the combustion response function of composite solid propellants was developed with particular attention to the contributions of the solid phase heterogeneity. The one-dimensional model treats the solid phase as alternating layers of ammonium perchlorate and binder, with an exothermic melt layer at the surface. Solution of the Fourier heat equation in the solid provides temperature and heat flux distributions with space and time. The problem is solved by conserving the heat flux at the surface from that produced by a suitable model of the gas phase. An approximation of the BDP flame model is utilized to represent the gas phase. By the use of several reasonable assumptions, it is found that a significant portion of the problem can be solved in closed form. A method is presented by which the model can be applied to tetramodal particle size distributions. A computerized steady-state version of the model was completed, which served to validate the various approximations and lay a foundation for the combustion response modeling. The combustion response modeling was completed in a form which does not require an iterative solution, and some preliminary results were acquired.

Source record↗

NASA NTRS1988

Numerical modeling of chemical vapor deposition (CVD) in a horizontal reactor

In the present numerical prediction of the deposition rate of silicon from silane in a CVD process, the conservation equations for mass, momentum, energy, and chemical species are solved on a staggered grid using the SIMPLE algorithm, while the rate of chemical reactions in the gas phase and on the susceptor surface is obtained from an Arrhenius rate equation. Predicted deposition rates as a function of position along the susceptor with and without the gas phase chemical reaction are compared with the available experimental and numerical data; agreement is excellent except at the leading edge of the susceptor, where the deposition rate is overpredicted.

Sheikholeslami, M. Z.↗

NASA NTRS2001

Spectroscopic diagnostics of organic chemistry in the protostellar environment

A combination of astronomical observations, laboratory studies, and theoretical modelling is necessary to determine the organic chemistry of dense molecular clouds. We present spectroscopic evidence for the composition and evolution of organic molecules in protostellar environments. The principal reaction pathways to complex molecule formation by catalysis on dust grains and by reactions in the interstellar gas are described. Protostellar cores, where warming of dust has induced evaporation of icy grain mantles, are excellent sites in which to study the interaction between gas phase and grain-surface chemistries. We investigate the link between organics that are observed as direct products of grain surface reactions and those which are formed by secondary gas phase reactions of evaporated surface products. Theory predicts observable correlations between specific interstellar molecules, and also which new organics are viable for detection. We discuss recent infrared observations obtained with the Infrared Space Observatory, laboratory studies of organic molecules, theories of molecule formation, and summarise recent radioastronomical searches for various complex molecules such as ethers, azaheterocyclic compounds, and amino acids.

Ethers/analysis/chemical synthesis/chemistry↗

NASA NTRS2004

Anomalous Oxygen and Krypton Abundances in Interstellar Gas

The primary objective of this program was to obtain FUSE observations of the interstellar H2 absorption toward a sample of stars observed with the HST STIS spectrograph as part of the ISM SNAP Survey. This Survey was designed to produce a database of high quality, high resolution W spectra from which interstellar gas-phase elemental abundances could be derived for large portions of the Galaxy. In particular, oxygen and krypton were chosen as excellent tracers for measuring the homogeneity of the interstellar gas due to their weak depletion into dust grains. The gas-phase 0 and Kr abundances relative to total hydrogen column density had previously been shown with HST GHRS measurements to be essentially constant in the local Milky Way. One of the main motivations of the ISM SNAP Survey was to determine if this constancy held at greater distances and in denser sightlines (where depletion into dust could be a possibility). The initial ISM SNAP STIS observations indicated a number of sightlines with unusual 0 and Kr abundances relative to the measured H I column densities. Since the appropriate benchmark for accurate abundance comparisons is the total hydrogen column density (H I plus H2), FUSE observations of interstellar H2 were carried out in these sightlines in order to determine if they represent cases of true abundance anomalies.

Meyer, David M.↗