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NASA NTRS1995

Gas-phase chemistry in dense interstellar clouds including grain surface molecular depletion and desorption

We present time-dependent models of the chemical evolution of molecular clouds which include depletion of atoms and molecules onto grain surfaces and desorption, as well as gas-phase interactions. We have included three mechanisms to remove species from the grain mantles: thermal evaporation, cosmic-ray-induced heating, and photodesorption. A wide range of parameter space has been explored to examine the abundance of species present both on the grain mantles and in the gas phase as a function of both position in the cloud (visual extinction) and of evolutionary state (time). The dominant mechanism that removes molecules from the grain mantles is cosmic-ray desorption. At times greater than the depletion timescale, the abundances of some simple species agree with abundances observed in the cold dark cloud TMC-1. Even though cosmic-ray desorption preserves the gas-phase chemistry at late times, molecules do show significant depletions from the gas phase. Examination of the dependence of depletion as a function of density shows that when the density increases from 10(exp 3)/cc to 10(exp 5)/cc several species including HCO(+), HCN, and CN show gas-phase abundance reductions of over an order of magnitude. The CO: H2O ratio in the grain mantles for our standard model is on the order of 10:1, in reasonable agreement with observations of nonpolar CO ice features in rho Ophiuchus and Serpens. We have also examined the interdependence of CO depletion with the space density of molecular hydrogen and binding energy to the grain surface. We find that the observed depletion of CO in Taurus in inconsistent with CO bonding in an H2O rich mantle, in agreement with observations. We suggest that if interstellar grains consist of an outer layer of CO ice, then the binding energies for many species to the grain mantle may be lower than commonly used, and a significant portion of molecular material may be maintained in the gas phase.

Bergin, E. A.↗

NASA NTRS1994

Physical and chemical structure of the IC 63 nebula. 1: Millimeter and far-infrared observations

We present results of a (sub)millimeter and far-infrared study of the reflection/emission nebula IC 63, located close to the BO.5p star gamma Cas. The source has been mapped in the (12)CO 2 - 1 and 3 - 2, (13)CO 2 - 1, and CS 2 - 1 lines and shows a small molecular cloud less than 1'x 2' in extent, which coincides with the brightest optical nebulosity and IRAS 100 micrometer emission. IC 63 is therefore an excellent example of a nearby (d approximately = 230 pc), edge-on photon-dominated region (PDR). Various other molecules have been observed at the peak position through their rotational transitions, in order to probe the physical parameters and to derive abundances. The measured CO, HCO(+) HCN, CS and H2CO line ratios suggest that the cloud is warm, T approximately = 50 K, and dense, n (H2) approximately = 5 x 10(exp 4)/cu cm. Excitation of molecules by electrons may play a significant role in this PDR. On the basis of these physical conditions, column densities have been determined from the observed line strengths. Several different methods are discussed to constrain the H2 column density, including the use of measured submillimeter continuum fluxes. The resulting abundances of species such as CN and CS are similar to those found in cold, dark clouds like TMC-1 and L134N. However, the abundances of other simple molecules such as HNC, HCO(+) and possibly C2H are lower by factors of at least three, probably because of the enhanced photodissociation rates at a distance of 1.3 pc from a B star. Surprisingly, only the abundance of the H2S molecule appears enhanced. More complex, volatile molecules such as CH3OH CH3CN and HNCO, and the sulfur-oxides SO and SO2 have not been found in this cloud. Limited observations of molecules in the reflection nebulea NGC 2023 are presented as well, and the resulting molecular abundances are compared with those found for IC 63.

Jansen, David J.↗

NASA NTRS1994

A CCD survey for faint high-latitude carbon stars

We describe a wide-area CCD survey to search for faint high-latitude carbon (FHLC) stars. Carbon giants provide excellent probes of the structure and kinematics of the outer Galactic halo. We use two-color photometric selection with large-format CCDs to cover 52 sq deg of sky to a depth of about V = 18. Of 94 faint C star candidates from our own CCD survey, one highly ranked V = 17 candidate was found to have a strong carbon and CN bands. We estimate that, to a depth of V = 18, the surface density of FHLC stars is 0.02 deg(exp -2). An updated FHLC sample is used to constrain halo kinematic and structural parameters. Although larger samples are needed, the effective radius of FHLC giants, assuming a de Vancouleurs law distribution, is larger than that for Galactic globular clusters.

Green, Paul J.↗

NASA NTRS1995

Detection of MgCn in IRC + 10216: A new metal-bearing free radical

A new metal-containing molecule, MgCN, has been detected toward the late-type star IRC + 10216, using the NRAO 12 m and IRAM 30 m telescopes. The N = 11 approaches 10, 10 approaches 9, and 9 approaches 8 transtions of this species which has a (sup 2)Sigma(sup +) ground state, have been observed in the outer envelope of this object at 3 mm. For the N = 11 approaches 10 transitions, the two spin-rotation components are clearly resolved and conclusively identify this new radical. These measurements imply a column of density for MgCN of N(sub tot) approximately 10(exp 12)/sq cm in the outer shell, which corresponds to a fractional abundance of f approximately 7x10(exp -10). This molecule, the metastable isomer of MgNC, is the third metal-bearing species thus far identified in the outer shell of IRC + 10216, and its detection implies a ratio of MgNC/MgCN approximately 22/1. MgCN may be formed through a reaction scheme involving magnesium and HNC or CN, both prominent outer shell molecules, or through synthesis on grains.

Ziurys, L. M.↗

NASA NTRS1995

Model atmospheres for M (sub)dwarf stars. 1: The base model grid

We have calculated a grid of more than 700 model atmospheres valid for a wide range of parameters encompassing the coolest known M dwarfs, M subdwarfs, and brown dwarf candidates: 1500 less than or equal to T(sub eff) less than or equal to 4000 K, 3.5 less than or equal to log g less than or equal to 5.5, and -4.0 less than or equal to (M/H) less than or equal to +0.5. Our equation of state includes 105 molecules and up to 27 ionization stages of 39 elements. In the calculations of the base grid of model atmospheres presented here, we include over 300 molecular bands of four molecules (TiO, VO, CaH, FeH) in the JOLA approximation, the water opacity of Ludwig (1971), collision-induced opacities, b-f and f-f atomic processes, as well as about 2 million spectral lines selected from a list with more than 42 million atomic and 24 million molecular (H2, CH, NH, OH, MgH, SiH, C2, CN, CO, SiO) lines. High-resolution synthetic spectra are obtained using an opacity sampling method. The model atmospheres and spectra are calculated with the generalized stellar atmosphere code PHOENIX, assuming LTE, plane-parallel geometry, energy (radiative plus convective) conservation, and hydrostatic equilibrium. The model spectra give close agreement with observations of M dwarfs across a wide spectral range from the blue to the near-IR, with one notable exception: the fit to the water bands. We discuss several practical applications of our model grid, e.g., broadband colors derived from the synthetic spectra. In light of current efforts to identify genuine brown dwarfs, we also show how low-resolution spectra of cool dwarfs vary with surface gravity, and how the high-regulation line profile of the Li I resonance doublet depends on the Li abundance.

Allard, France↗

NASA NTRS1995

Part A: Cirrus ice crystal nucleation and growth. Part B: Automated analysis of aircraft ice particle data

Specific measurement of cirrus crystals by aircraft and temperature modified CN are used to specify measurements necessary to provide a basis for a conceptual model of cirrus particle formation. Key to this is the ability to measure the complete spectrum of particles at cirrus levels. The most difficult regions for such measurement is from a few to 100 microns, and uses a replicator. The details of the system to automate replicator data analysis are given, together with an example case study of the system provided from a cirrus cloud in FIRE 2, with particles detectable by replicator and FSSP, but not 2DC.

Arnott, William P.↗

NASA NTRS1995

Using the HARV simulation aerodynamic model to determine forebody strake aerodynamic coefficients from flight data

The method described in this report is intended to present an overview of a process developed to extract the forebody aerodynamic increments from flight tests. The process to determine the aerodynamic increments (rolling pitching, and yawing moments, Cl, Cm, Cn, respectively) for the forebody strake controllers added to the F/A - 18 High Alpha Research Vehicle (HARV) aircraft was developed to validate the forebody strake aerodynamic model used in simulation.

Messina, Michael D.↗

NASA NTRS1995

Composition/Structure/Dynamics of comet and planetary satellite atmospheres

This research program addresses two cases of tenuous planetary atmospheres: comets and Io. The comet atmospheric research seeks to analyze a set of spatial profiles of CN in comet Halley taken in a 7.4-day period in April 1986; to apply a new dust coma model to various observations; and to analyze observations of the inner hydrogen coma, which can be optically thick to the resonance scattering of Lyman-alpha radiation, with the newly developed approach that combines a spherical radiative transfer model with our Monte Carlo H coma model. The Io research seeks to understand the atmospheric escape from Io with a hybrid-kinetic model for neutral gases and plasma given methods and algorithms developed for the study of neutral gas cometary atmospheres and the earth's polar wind and plasmasphere. Progress is reported on cometary Hydrogen Lyman-alpha studies; time-series analysis of cometary spatial profiles; model analysis of the dust comae of comets; and a global kinetic atmospheric model of Io.

Combi, Michael R.↗

NASA NTRS1996

Processing of Icy Mantles in Protostellar Envelopes

The 4.5-4.8 micron spectral region provides two potential diagnostics of radiative or thermal processing of interstellar ices in the environs of embedded stars in molecular clouds. A broad absorption feature centered at 4.62 micron is seen in the spectra of several young stellar objects (YSO's) and attributed to C-N triple bonds in a nitrile or isonitrile. As CN-bearing solids in the laboratory are produced by energetic radiative processing of ices containing nitrogen, detection of this feature in YSO's is taken as evidence for (1) the presence of nitrogen in the unprocessed cloud ices, and (2) evolution of the ice in the vicinity of the embedded source. The adjacent feature at 4.67 micron, identified with solid CO, provides not only quantitative information on CO itself but also indirect evidence for the presence of other species; its position and profile are sensitive to the molecular environment of the CO molecules in the ice mantle, and may be used to constrain both the composition and thermal/radiative history of the ice. One important example is the possibility to detect CO2, which is produced easily in the laboratory by UV irradiation of CO-rich or CH3OH-rich ices. CO embedded in a CO2 matrix gives a characteristic spectral signature distinct from other CO-bearing mixtures investigated to date. We have obtained CO absorption profiles of three young stellar objects in order to investigate their ice mantle composition.

Chiar, J. E.↗

NASA NTRS1994

X-ray Photoelectron Spectroscopy Study of Argon-Plasma-Treated Fluoropolymers

Films of poly(tetrafluoroethylene) (PTFE) and of a tetrafluoroethylene-perfluoroalkyl vinyl ether (approximately 49:1) copolymer (PFA) were exposed to a radio-frequency argon plasma and then examined by X-ray photoelectron spectroscopy (XPS). The use of fluoropolymer films nearly free of surface hydrocarbon contamination as well as the use of a monochromatized X-ray source for XPS removed two factors contributing to conflicting reports on the effect of exposure time on the fluorine-to-carbon (F/C) and oxygen-to-carbon (O/C) ratios for several Ar-plasma-treated fluoropolymers. Contrary to literature indications, a common pattern was found for PTFE and PFA: a moderate decrease in F/C ratio (from 1.99 to 1.40, and from 1.97 to 1.57, respectively), together with a moderate increase in O/C ratio (from negligible to about 0.10, and from 0.012 to about O.10, respectively) at very short exposures, after which the F/C ratios remained essentially constant on prolonged exposures, while the O/C ratios for PTFE and PFA leveled off at 0.11 and 0.15, respectively. The XPS C(sub 1s), spectra for these polymers exposed to the Ar plasma for 20 min were similar and presented, besides a prominent peak at 292.0 eV (CF2,) and a minor peak at 294.0 or 294.1 eV (CF3), a composite band of four curve-resolved peaks (approximately 285-290 eV) representing various CH, CC, CO, CN, and CF functionalities.

Golub, Morton A.↗

NASA NTRS1997

Construction of a Visible Diode Laser Source for Free Radical Photochemistry and Spectroscopy Experiments

Tunable diode lasers are reliable sources of narrow-band light and comparatively cheap. Optical feedback simplifies frequency tuning of the laser diodes. We are building an inexpensive diode laser system incorporating optical feedback from a diffraction grating. The external optical cavity can be used with lasers that emit between 2 and 100 mW, and will also work if they are pulsed, although this will significantly degrade the bandwidth. The diode laser output power and bandwidth are comparable to CW dye lasers used in kinetics and dynamics experiments. However, their cost and maintenance will be much less as will alignment time. We intend to use the diode lasers to investigate CN and C2 kinetics as well as to study dissociation dynamics of atmospherically important molecules.

Newman, Bronjelyn↗

NASA NTRS1995

Organic Compounds Produced by Photolysis of Realistic Interstellar and Cometary Ice Analogs Containing Methanol

The InfraRed (IR) spectra of UltraViolet (UV) and thermally processed, methanol-containing interstellar / cometary ice analogs at temperatures from 12 to 300 K are presented. Infrared spectroscopy, H-1 and C-13 Nuclear Magnetic Resonance (NMR) spectroscopy, and gas chromatography-mass spectrometry indicate that CO (carbon monoxide), CO2 (carbon dioxide), CH4 (methane), HCO (the formyl radical), H2CO (formaldehyde), CH3CH2OH (ethanol), HC([double bond]O)NH2 (formamide), CH3C([double bond]O)NH2 (acetamide), and R[single bond]C[triple bond]N (nitriles) are formed. In addition, the organic materials remaining after photolyzed ice analogs have been warmed to room temperature contain (in rough order of decreasing abundance), (1) hexamethylenetetramine (HMT, C6H12N4), (2) ethers, alcohols, and compounds related to PolyOxyMethylene (POM, ([single bond]CH2O[single bond](sub n)), and (3) ketones (R[single bond]C([double bond]O)[single bond]R') and amides (H2NC([double bond]O)[single bond]R). Most of the carbon in these residues is thought to come from the methanol in the original ice. Deuterium and C-13 isotopic labeling demonstrates that methanol is definitely the source of carbon in HMT. High concentrations of HMT in interstellar and cometary ices could have important astrophysical consequences. The ultraviolet photolysis of HMT frozen in H2O ice readily produces the 'XCN' band observed in the spectra of protostellar objects and laboratory ices, as well as other nitriles. Thus, HMT may be a precursor of XCN and a source of CN in comets and the interstellar medium. Also, HMT is known to hydrolyze under acidic conditions to yield ammonia, formaldehyde, and amino acids. Thus, HMT may be a significant source of prebiogenic compounds on asteroidal parent bodies. A potential mechanism for the radiative formation of HMT in cosmic ices is outlined.

Bernstein, Max P.↗

NASA NTRS1997

Summary of Research/Publications

Summary of research/publications include:(1) Comment on broadening of water microwave lines by collisions with helium atoms; (2) Calculations of ion-molecule deuterium fractionation reactions involving HD; (3) Ab initio predictions on the rotational spectra of carbon-chain carbene molecules; (4) Theoretical IR spectra of ionized naphthalene; (5) Improved collisional excitation rates for interstellar water; (6) Calculations on the competition between association and reaction for C3H+ + H2; (7) Theoretical infrared spectra of some model polycyclic aromatic hydrocarbons: effect of ionization; (8) Calculations concerning interstellar isomeric abundance ratios for C3H and C3H2; (9) New calculations on the ion-molecule processes C2H2+ + H2 C2H3+ + H and C2H2+ + H2 C2H4+; (10) Anisotropic rigid rotor potential energy function for H2O-H2; (11) A correlated ab initio study of linear carbon-chain radicals CnH (n=2-7); (12) Ab initio characterization of MgCCH, MgCCH+, and MgC2 and pathways to their formation in the interstellar medium; (13) Why HOC+ is detectable in interstellar clouds: The rate of the reaction between HOC+ and H2; (14) A correlated ab initio study of the X 2A 1 and A 2E states of MgCH3; (15) On the stability of interstellar carbon clusters: The rate of the reaction between C3 and O; and (16) The rate of the reaction between CN and C2H2 at interstellar temperatures.

Source record↗

NASA NTRS1997

Global Troposphere Experiment Project

For the Global Troposphere Experiment project Pacific Exploratory Measurements West B (PEM West B), we made determinations of sulfur dioxide (SO2) and dimethyl sulfide (DMS) using gas chromatography-mass spectrometry with isotopically labelled internal standards. This technique provides measurements with precision of 1 part-per-trillion by volume below 20 pptv and 1% above 20 pptv. Measurement of DMS and SO2 were performed with a time cycle of 5-6 minutes with intermittent zero checks. The detection limits were about 1 pptv for SO2 and 2 pptv for DMS. Over 700 measurements of each compound were made in flight. Volcanic impacts on the upper troposphere were again found as a result of deep convection in the tropics. Extensive emission of SO2 from the Pacific Rim land masses were primarily observed in the lower well-mixed part of the boundary layer but also in the upper part of the boundary layer. Analyses of the SO2 data with aerosol sulfate, beryllium-7, and lead-210 indicated that SO2, contributed to half or more of the observed total oxidized sulfur (SO2 plus aerosol sulfate) in free tropospheric air. Cloud processing and rain appeared to be responsible for lower SO2 levels between 3 and 8.5 km than above or below this region. During both phases of PEM-West, dimethyl sulfide did not appear to be a major source of sulfur dioxide in the upper free troposphere over the western Pacific Ocean. In 1991 the sources Of SO2 at high altitude appeared to be both anthropogenic and volcanic with an estimated 1% being solely from DMS. The primary difference for the increase in the DMS source was the very low concentration of SO2 at high altitude. In the midlatitude region near the Asian land masses, DMS in the mixed layer was lower than in the tropical region of the western Pacific. Convective cloud systems near volcanoes in the tropical convergence in the western Pacific troposphere were a major source of SO2 at high altitudes during PEM-West B. High levels of SO2 were observed in several instances with large number concentrations of ultrafine CN above 9 km in the tropical convergence zone. Conversion of SO2, by OH to SO3 and subsequently to sulfuric acid may have been enhanced by lightning-produced NO levels exceeding 1 part per billion. Coupling of strong convection and volcanic sources of SO2 apparently is an important source of new particle formation at high altitude in the tropical convergence zone.

Bandy, Alan R.↗

NASA NTRS1997

Measurements of Ice Nucleating Aerosols in the Upper Troposphere and Lower Stratosphere

Our major accomplishments during Year 1 were: Development of aerosol and crystal collection techniques. Development of single-particle chemical characterization techniques. Modification of system design for DC-8 and initial testing. Our major accomplishments during Year 2 were: Completion of system design and proof-of-concept experiments. Participation in SUCCESS mission. Reporting of theoretical and laboratory findings in the scientific literature. Reporting of initial SUCCESS results at scientific meetings. Our major accomplishments during Year 3 were: Data reduction and submission of all SUCCESS data to the archive. Participation in SUCCESS data comparison workshops. Reporting of SUCCESS results at the AEAP Meeting. Organization of CN counter intercomparison workshop. Preparation of three manuscripts submitted to the GRL SUCCESS Special Issue.

Kreidenweis, S. M.↗

NASA NTRS1993

Detection of the 2165 Inverse Centimeter (4.619 Micron) XCN Band in the Spectrum of L1551 IRS 5

We report the detection of a broad absorption band at 2165 cm (4.619 microns) in the spectrum of L1551 IRS 5. New laboratory results over the 2200-2100 /cm wavenumber interval (4.55-4.76 microns), performed with realistic interstellar ice analogs, suggest that this feature is due to a CN-containing compound. We will refer to this compound as XCN. We also confirm the presence of frozen CO (both in nonpolar and polar matrices) through absorption bands at 2140 /cm (4.67 microns) and 2135 /cm (4.68 microns). The relative abundance of solid-state CO to frozen H2O is approx. 0.13 while the abundance of XCN seems comparable to that of frozen CO.

Tegler, Stephen C.↗

NASA NTRS1997

Characterization of Aircraft Produced Soot and Contrails Near the Tropopause

Participation in the SUCCESS project primarily involved development and deployment of specific instruments for characterizing jet aircraft exhaust emissions as particulates and their subsequent evolution as contrail particles, either liquid or solid, as cirrus. Observations can be conveniently considered in two categories - close or distant from the aircraft. Thus close to the aircraft the exhaust is mixing through the engine turbulence with a much drier and colder environment and developing water/ ice supersaturation along the trail depending on circumstances (near field), whereas distant from the aircraft (far field) the exhaust has cooled essentially to ambient temperature, the turbulence has decayed and any particle growth or evaporation is controlled by the prevailing ambient conditions. Intermediate between these two regions the main aircraft vortices form (one on each side of the aircraft) which tend to inhibit mixing under some conditions, a region extending from a few aircraft lengths to sometimes a hundred times this distance. Our approach to the problem lay in experience gained in characterizing the smoke from hydrocarbon combustion in terms of its cloud forming properties and its potential influence on the radiation properties of the smoke and subsequent cloud from the viewpoint of reduction (absorbtion and scattering ) of solar radiation flux leading to significant global cooling (Hudson et al 1991; Hallett and Hudson 1991). Engine exhaust contains a much smaller proportion of the fuel carbon than is sometimes present in ordinary combustion (less than 0.01% compared with 10%) and influences condensation in quite different ways, to be characterized by the Cloud Condensation Nucleus, CCN - supersaturation spectrum. The transition to ice is to be related to the dilution of solution droplets to freeze by homogeneous nucleation at temperatures somewhat below -40C (Pueschel et al 1998). The subsequent growth of ice particles depends critically on temperature, supersaturation and to some extent pressure, as is demonstrated in an NSF funded project being carried out in parallel with the work reported here. As will be discussed below, nucleation processes themselves and also exhaust impurities also influence the growth of ice particles and may control some aspects of growth of ice in contrails. Instrumentation was designed to give insight into these questions and to be flown on the NASA DC- 8 as a platform. In addition a modest program was undertaken to investigate the properties of laboratory produced smoke produced under controlled conditions from the viewpoint of forming both CCN and CN. The composition of the smoke could inferred from a thermal characterization technique; larger particles were captured by formvar replicator for detailed analysis; ice particles were captured and evaporated in flight on a new instrument, the cloudscope, to give their mass, density and impurity content.

Hallett, John↗

NASA NTRS1997

A 2D Microphysical Analysis of Aerosol Nucleation in the Polar Winter Stratosphere: Implications for H2SO4 Photolysis and Nucleation Mechanisms

Each spring a layer of small particles forms between 20 and 30 km in the polar regions. Results are presented from a 2D microphysical model of sulfate aerosol, which provide the first self-consistent explanation of the observed "CN layer." Photochemical conversion of sulfuric acid to SO2 in the upper stratosphere and mesosphere is necessary for this layer to form. Recent laboratory measurements of H2SO4 and SO3 photolysis rates are consistent with such conversion, though an additional source of SO2 may be required. Nucleation throughout the polar winter extends the top of the aerosol layer to higher altitudes, despite strong downward transport of ambient air. This finding may be important to heterogeneous chemistry at the top of the aerosol layer in polar winter and spring.

Mills, Michael J.↗