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NASA NTRS1995

Polyazomethines containing trifluoromethylbenzene units

Soluble, amorphous, aromatic polyazomethine polymers and copolymers were prepared by reacting a dialdehyde monomer with a diamine monomer containing trifluoromethylbenzene and various combinations thereof in a solvent, such as N,N-dimethylacetamide. The reaction was heated to reflux yielding a polyazomethine which, after cooling to room temperature, was precipitated. These polymers and copolymers may be used to make films, coatings, composites and adhesives.

Bryant, Robert G.↗
NASA NTRS1995

Hypervelocity impact survivability experiments for carbonaceous impactors, part 2

Hypervelocity impact experiments were performed to further test the survivability of carbonaceous impactors and to determine potential products that may have been synthesized during impact. Diamonds were launched by the Ames two-stage light gas gun into Al plate at velocities of 2.75 and 3.1 km sec(exp -1). FESEM imagery confirms that diamond fragments survived in both experiments. Earlier experiments found that diamonds were destroyed on impact above 4.3 km sec(exp -1). Thus, the upper stability limit for diamond on impact into Al, as determined from our experimental conditions, is between 3.1 and 4.3 km sec(exp -1). Particles of the carbonaceous chondrite Nogoya were also launched into Al at a velocity of 6.2 km sec (exp -1). Laser desorption (L (exp 2) MS) analyses of the impactor residues indicate that the lowest and highest mass polycyclic aromatic hydrocarbons (PAH's) were largely destroyed on impact; those of intermediate mass (202-220 amu) remained at the same level or increased in abundance. In addition, alkyl-substituted homologs of the most abundant pre-impacted PAH's were synthesized during impact. These results suggest that an unknown fraction of some organic compounds can survive low to moderate impact velocities and that synthesized products can be expected to form up to velocities of, at least, 6.5 km sec(exp -1). We also present examples of craters formed by a unique microparticle accelerator that could launch micron-sized particles of almost any coherent material at velocities up to approximately 15 km sec(exp -1). Many of the experiments have a direct bearing on the interpretation of LDEF craters.

Bunch, T. E.↗
NASA NTRS1995

The effect of simulated low earth orbit radiation on polyimides (UV degradation study)

UV degradation of polyimide films in air and vacuum were studied using UV-visible, ESR, FTIR, and XPS spectroscopies. The UV-visible spectra of polyimide films showed a blue shift in the absorption compared to Kapton. This behavior was attributed to the presence of bulky groups and kinks along the polymer chains which disrupt the formation of a charge transfer complex. The UV-visible spectra showed also that UV irradiation of polyimides result extensively in surface degradation, leaving the bulk of the polymer intact. ESR spectra of polyimides irradiated in vacuum revealed the formation of stable carbon-centered radicals which give a singlet ESR spectrum, while polyimides irradiated in air produced an asymmetric signal shifted to a lower magnetic field, with a higher g value and line width. This signal was attributed to oxygen-cenetered radicals of peroxy and/or alkoxy type. The rate of radical formation in air was two fold higher than for vacuum irradiation, and reached a plateau after a short time. This suggests a continuous depletion of radicals on the surface via an ablative degradation process. FTIR, XPS, and weight loss studies supported this postulate. An XPS study of the surface indicated a substantial increase in the surface oxidation after irradiation in air. The sharp increase in the C-O binding energy peak relative to the C-C peak was believed to be associated with an aromatic ring opening reaction.

Forsythe, John S.↗
NASA NTRS1995

The surface properties of fluorinated polyimides exposed to VUV and atomic oxygen

The effect of atomic oxygen flux and VUV radiation alone and in combination on the surface of fluorinated polyimide films was studied using XPS spectroscopy. Exposure of fluorinated polyimides to VUV radiation alone caused no observable damage to the polymer surface, while an atomic oxygen flux resulted in substantial oxidation of the surface. On the other hand, exposure to VUV radiation and atomic oxygen in combination caused extensive oxidation of the polymer surface after only 2 minutes of exposure. The amount of oxidized carbon on the polymer surface indicated that there is aromatic ring opening oxidation. The changes in the O1s/C1s, N1s/C1s, and F1s/C1s ratios suggested that an ablative degradation process is highly favorable. A synergistic effect of VUV radiation in the presence of atomic oxygen is clearly evidenced from the XPS study. The atomic oxygen could be considered as the main factor in the degradation process of fluorinated polyimide films exposed to a low earth orbit environment.

Forsythe, John S.↗
NASA NTRS1993

Laboratory simulated hydrothermal alteration of sedimentary organic matter from Guaymas Basin, Gulf of California

High temperature alteration of sedimentary organic matter associated with marine hydrothermal systems involves complex physical and chemical processes that are not easily measured in most natural systems. Many of these processes can be evaluated indirectly by examining the geochemistry of the hydrothermal system in the laboratory. In this investigation, an experimental organic geochemical approach to studying pyrolysis of sedimentary organic matter is applied to the hydrothermal system in the Guaymas Basin, Gulf of California. A general survey of hydrothermal oils and extractable organic matter (bitumen) in hydrothermally altered sediments identified several homologous series of alkanones associated with a high temperature hydrothermal origin. The alkanones range in carbon number from C11 to C30 with no carbon number preference. Alkan-2-ones are in highest concentrations, with lower amounts of 3-, 4-, 5- (and higher) homologs. The alkanones appear to be pyrolysis products synthesized under extreme hydrothermal conditions. Hydrous pyrolysis and confinement pyrolysis experiments were performed to simulate thermally enhanced diagenetic and catagenetic changes in the immature sedimentary organic matter. The extent of alteration was measured by monitoring the n-alkanes, acyclic isoprenoids, steroid and triterpenoid biomarkers, polycyclic aromatic hydrocarbons and alkanones. The results were compared to bitumen extracts from sediments which have been naturally altered by a sill intrusion and accompanied hydrothermal fluid flow. These pyrolysis experiments duplicated many of the organic matter transformations observed in the natural system. Full hopane and sterane maturation occurred after 48 hr in experiments at 330 deg C with low water/rock mass ratios (0.29). A variety of radical and ionic reactions are responsible for the organic compound conversions which occur under extreme hydrothermal conditions. Short duration pyrolysis experiments revealed that a portion of the hydrocarbons generated from kerogen was observed to go through alkene intermediates, and the rate of alkene isomerization was influenced by the ionic strength and catalytic mineral phases. Confinement of the organic pyrolysate to the bulk sediment accelerated the rates of the biomarker epimerization reactions, suggesting that these reactions are influenced strongly by the association of the inorganic matrix, and that the relative rates of some ionic and radical reactions can be influenced by the water/rock ratio during the pyrolysis experiments.

Leif, Roald N.↗
NASA NTRS1995

Environment applications for ion mobility spectrometry

The detection of environmentally important polychlorinated aromatics by ion mobility spectrometry (IMS) was investigated. Single polychlorinated biphenyl (PCB) isomers (congeners) having five or more chlorine atoms were reliably detected in isooctane solution at levels of 35 ng with a Barringer IONSCAN ion mobility spectrometer operating in negative mode; limits of detection (LOD) were extrapolated to be in the low ng region. Mixtures of up to four PCB congeners, showing characteristic multiple peaks, and complex commercial mixtures of PCBs (Aroclors) were also detected. Detection of Aroclors in transformer oil was suppressed by the presence of the antioxidant BHT (2,6-di-t-butyl4-methylphenol) in the oil. The wood preservative pentachlorophenol (PCP) was easily detected in recycled wood shavings at levels of 52 ppm with the IONSCAN; the LOD was extrapolated to be in the low ppm region.

Ritchie, Robert K.↗
NASA NTRS1995

Direct analysis of organic priority pollutants by IMS

Many routine methods for monitoring of trace amounts of atmospheric organic pollutants consist of several steps. Typical steps are: (1) collection of the air sample; (2) trapping of organics from the sample; (3) extraction of the trapped organics; and (4) identification of the organics in the extract by GC (gas chromatography), HPLC (High Performance Liquid Chromatography), or MS (Mass Spectrometry). These methods are often cumbersome and time consuming. A simple and fast method for monitoring atmospheric organics using an IMS (Ion Mobility Spectrometer) is proposed. This method has a short sampling time and does not require extraction of the organics since the sample is placed directly in the IMS. The purpose of this study was to determine the responses in the IMS to organic 'priority pollutants'. Priority pollutants including representative polycyclic aromatic hydrocarbons (PAHs), phthalates, phenols, chlorinated pesticides, and polychlorinated biphenyls (PCB's) were analyzed in both the positive and negative detection mode at ambient atmospheric pressure. Detection mode and amount detected are presented.

Giam, C. S.↗
NASA NTRS1990

Benzenoid hydrocarbons in space: The evidence and implications

Many different celestial objects emit an infrared spectrum which has been attributed to infrared fluorescence from a family of highly vibrationally excited benzenoid hydrocarbons referred to as polycyclic aromatic hydrocarbons (PAHs). The most intense emitters contain between 20 to 50 carbon atoms, although larger species also contribute to the emission. This assignment is based on a rough resemblance of the interstellar emission spectra to the vibrational spectra of PAHs and related materials such as chars and soots which contain PAH mixtures. The spectroscopic assignments of the features between 3200 and 700/cm are discussed in detail. Much laboratory work on PAHs which are larger than those previously studied, isolated, ionized and dehydrogenated is called for to fully exploit this model. As PAHs are thought to be ubiquitous throughout the interstellar medium and more abundant than all other known polyatomic, interstellar molecules, they possess great potential as important probes of conditions in many different kinds of astronomical objects. Conversely, astronomical observations are extending our knowledge of these exotic materials by probing regions in which some conditions may be impossible to duplicate in the laboratory.

Allamandola, Louis J.↗
NASA NTRS1995

Toward the detection of pure carbon clusters in the Interstellar Medium (ISM)

Determination of the form and distribution of carbon in the universe is critical to understanding the origin of life on Earth and elsewhere. Two potentially large reservoirs of carbon in the interstellar medium (ISM) remain unexplored. These are polycyclic aromatic hydrocarbons (PAH) and pure carbon clusters. Little information exists on the structures, properties, and transition frequencies of pure carbon clusters. The work described is designed to provide a specific inventory of laboratory frequencies and physical properties of this carbon clusters so that efforts can be made to detect them in cold interstellar sources by far-infrared astronomy. Data is given from infrared laser spectroscopy determination of the structure of C3, C4, C5, C6, C7, and C9.

Heath, J. R.↗
NASA NTRS1994

High-resolution mid-infrared observations of NGC 7469

We present a high-resolution 11.7 micrometer image of the starburst/Seyfert hybrid galaxy NGC 7469 using the Hale 5 m telescope at Palomar Observatory. Our map, with diffraction limited spatial resolution of 0.6 sec, shows a 3 sec diameter ring of emission around an unresolved nucleus. The map is similar to the Very Large Array (VLA) 6 cm map of this galaxy made with 0.4 sec resolution by Wilson et al. (1991). About half of the mid-infrared flux in our map emerges from the unresolved nucleus. We also present spatially resolved low resolution spectra that show that the 11.3 micrometer polycyclic aromatic hydrocarbon (PAH) feature comes from the circumnuclear ring but not from the nucleus of the galaxy.

Miles, J. W.↗
NASA NTRS1994

COBE diffuse infrared background experiment observations of Galactic reddening and stellar populations

This Letter describes the results of an initial study of Galactic extinction and the colors of Galactic stellar populations in the near-IR using the Diffuse Infrared Background Experiment (DIRBE) aboard the Cosmic Background Explorer (COBE) spacecraft. The near-IR reddening observed by DIRBE is consistent with the extinction law tabulated by Rieke & Lebofsky (1985). The distribution of dust and stars in most of the first and fourth quadrants of the Galactic plane (0 deg less than l less than 90 deg, and 270 deg less than l less than 360 deg, respectively) can be modeled as a stellar background source seen through up to approximately 4 mag of extinction at 1.25 micrometers. The unreddened near-IR colors of the Galactic disk are similar to those of late-K and M giants. The Galactic bulge exhibits slightly bluer colors in the 2.2-3.5 micrometers range, as noted by Terndrup et al. (1991). Star-forming regions exhibit colors that indicate the presence of a approximately 900 K continuum produced by hot dust or polycyclic aromatic hydrocarbons (PAHs) contributing at wavelengths as short as 3.5 micrometers.

Arendt, R. G.↗
NASA NTRS1994

The origin of variations in the 2175 A extinction bump

In this paper, small graphite grains are assumed to produce the 2175 A interstellar extinction bump. The principal observational characteristic of the bump in the invariance of its central wavelength (2174 +/- 9 A) among various lines of sight through diverse environments. On the other hand, its Full Width at Half Maximum (FWHM) varies from about 0.80/micrometer to 1.2/micrometer among the same lines of sight. In this paper, the variations in bump width among different sight lines is attributed to coatings on the graphite grains. The necessary properties of the coating material are investigated. Simple neutral polycycli aromatic hydrocarbons (PAHs) have measured laboratory absorptions remarkably similar to those required to explain the broadening of the bump. Only 1.5% of cosmic carbon in PAHs is required to produce very broad bumps. Alternatively, about 2%-4% of the combined abundances of the refractory elements Fe and Mg, more highly depleted onto grains in dense regions than in the diffuse interstellar medium, could explain the mantles if their absorption rises rapidly with energy, as it does for MgO. Coatings of amorphous carbon, hydrogenated or not, diamond-like bonded carbon, or water ice do not have published optical constants that vary rapidly enough in wavenumber to produce the variations.

Mathis, John S.↗
NASA NTRS1994

Induced nucleation of carbon dust in red giant stars

This study quantitatively tests the proposed model of induced nucleation of carbonaceous grains in carbon-rich red giant stars. Induced nucleation is the process of grain growth initiated by the presence of reactive surfaces provided by seed particles. The numerical study was performed using a deailed chemical kinetic model of carbon deposition, grain coagulation, and homogeneous nucleation of polycyclic aromatic hydrocarbons (PAHs). The model uses a method of moments to keep track of developing grain population in the forming dust shell. We test the efficiency of grain formation for large ranges of dust shell parameters typical for carbon stars. Our model is capable of producing a range of optically thick and thin dust shells in carbon stars. Results are in accord with (IRAS) spectral classes of carbon stars. The resulting composite grains produced are consistent with those recently found in ancient meteorites. This model also provides a realistic explanation for high abundances of (PAHs) in the interstellar medium and some planetary nebulae.

Cadwell, Brian J.↗
NASA NTRS1994

IRAS colors within M31: Evidence for deficiency of very small grains?

Significant differences are found in the IRAS color-color diagrams of small regions (2 min x 2 min, or 0.4 x 1.8 kpc) within the disk of M31 compared to Galactic cirrus, most noticeably demonstrated by a trend of low 60 to 100 micrometer surface brightness ratio and high 12 to 25 micrometer ratio. Based on physical arguments, we conclude that these color differences are best explained by assuming that 'very small grains' (VSG; but not polycylic aromatic hydrocarbons) are only half as abundant in M31 as they are in Galactic cirrus. We confirm this conclusion and test its detailed agreement with data by using the phenomenological model of Desert et al. (1990). In particular, we show that the data cannot be explained by postulating weaker UV heating in the disk of M31. We also show that the VSG-deficient model predicts correctly the correspondence between the IRAS colors and the 100 micrometer emissivity per H I atom in the outer disk of M31. 'Very small grains' are a leading candidate for the carrier of the 2175 A bump in the extinction curve. Our suggested VSG deficiency in M31 is thus consistent with recent Hubble Space Telescope (HST) observations which show evidence for a weaker and narrower 2175 A bump on the M31 extinction curve. Some speculation is offered as to possible links between very small grains and the low rate of current star formation in M31.

Xu, Cong↗
NASA NTRS1994

Photon-dominated regions around cool stars: The effects of the color temperature of the radiation field

We have investigated the influence of the color temperature of the illuminating radiation field on the chemical and thermal structure of photon-dominated regions (PDRs). We present the results of a study of the photoelectric efficiency of heating by large molecules such as polycyclic aromatic hydrocarbons (PAHs) and very small grains for radiation fields characterized by different effective temperatures. We show that the efficiency for cooler (T(sub eff) approximately = 6000-10,000 K) stars is at most an order of magnitude smaller than that for hotter (T(sub eff) approximately = 20,000-30,000 K) stars. While cooler radiation fields result in less ultraviolet photons capable of heating, the efficiency per absorbed photon is higher, because the grains become less positively charged. We also present detailed calculations of the chemistry and thermal balance for generic PDRs (n(sub 0) approximately = 10(exp 3), G(sub 0) approximately = 10(exp 3)). For cooler radiation fields, the H/H2 and C(+)/C/CO transition layers shift toward the surface of the PDR, because fewer photons are available to photodissociate H2 and CO and to ionize C. The dominant cooling lines are the (C II) 158 micron and the (O I) 63 micron lines for the hotter radiation fields, but cooling by CO becomes dominant for a color temperature of 6000 K or lower. The (C II)/CO and (O I)/CO ratios are found to be very good diagnostics for the color temperature of the radiation field.

Spaans, Marco↗
NASA NTRS1994

Detection of the overtone of the 3.3 micron emission feature in IRAS 21282+5050

The 1.6-1.8 micron spectrum of the planetary nebula, IRAS 21282+5050, a strong emitter of the unidentified interstellar bands, contains a 0.02 micron wide eimission feature centered at 1.680 micron, which is well matched by laboratory spectra of the 0-2 CH stretching mode in polycyclic aromatic hydrocarbons (PAHs). We identify the new feature as the overtone of the well-known 3.3 micron band. In view of the high excitation required for emission in this band, the identification indicates that the emission is by free molecules rather than molecular moieties in solid dust grains. Modeling of the intensity ratio of the 2-0 to 1-0 band implied that the PAHs emitting in these bands contain about 60 carbon atoms. It is inferred that the nu = 2-1 hot band of the CH stretching mode occurs at about 3.43 micron and contributes to the long-wavelength shoulder of the 3.40 micron feature. The main 3.40 micron feature probably is due to aliphatic sidegroups on PAH molecules.

Geballe, T. R.↗
NASA NTRS1994

Near-infrared absorption spectroscopy of interstellar hydrocarbon grains

We present new 3600 - 2700/cm (2.8 - 3.7 micrometer) spectra of objects whose extinction is dominated by dust in the diffuse interstellar medium. The observations presented here augment an ongoing study of the organic component of the diffuse interstellar medium. These spectra contain a broad feature centered near 3300/cm (3.0 micrometers) and/or a feature with a more complex profile near 2950/cm (3.4 micrometers), the latter of which is attributed to saturated aliphatic hydrocarbons in interstellar grains and is the primary interest of this paper. As in our earlier work, the similarity of the absorption bands near 2950/cm (3.4 micrometers) along different lines of sight and the correlation of these features with interstellar extinction reveal that the carrier of this band lies in the dust in the diffuse interstellar medium (DISM). At least 2.5% of the cosmic carbon in the local interstellar medium and 4% toward the Galactic center is tied up in the carrier of the 2950/cm (3.4 micrometer) band. The spectral structure of the diffuse dust hydrocarbon C-H stretch absorption features is reasonably similar to UV photolyzed laboratory ice residues and is quite similar to the carbonaceous component of the Murchison meteorite. The similarity between the DISM and the meteoritic spectrum suggests that some of the interstellar material originally incorporated into the solar nebula may have survived relatively untouched in primitive solar system bodies. Comparisons of the DISM spectrum to hydrogenated amorphous carbon and quenched carbonaceous composite are also presented. The A(sub V)/tau ratio for the 2950/cm (3.4 micrometer) feature is lower toward the Galactic center than toward sources in the local solar neighborhood (approximately 150 for the Galactic center sources vs. approximately 250 for the local ISM sources). A similar trend has been observed previously for silicates in the diffuse medium by Roche & Aitken, suggesting that (1) the silicate and carbonaceous materials in the DISM may be physically correlated and (2) there is either dust compositional variation in the galaxy or galactic variation in the grain population density distribution. We also note a possible absorption feature near 3050/cm (3.28 micrometers), a wavelength position that is characteristic of polycyclic aromatic hydrocarbons (PAHs).

Pendleton, Y. J.↗
NASA NTRS1995

10 micron spectroscopy of younger stars in the rho Ophiuchi cloud

Spectra in the 10 micrometer region were obtained of 14 young stars associated with the central core of the rho Oph dark cloud complex. Silicate dust emission and absorption features can be fairly well reproduced with simple models using the emissivity of the silicates in the Orion Trapezium region, believed to be typical of molecular cloud dust. A spectrum of the Trapezium star theta(sup 1) Ori D was obtained to define the emissivity more precisely. The emissivity of silicate dust around the late-type giant Mu Cep does not improve the fits to the absorption features and provides a poorer match to the emission features. None of the sources display a strong 11.2 micrometer peak like that seen in comet Halley and attributed to crystalline olivine. A broad weak feature near 11.2 micrometer, possibly related to the comet feature, may be present in the emission spectrum of the Herbig Ae star HD 150193. Absorption features toward two of the objects are narrower than would be expected from Trapezium-like silicates, suggesting differences in the composition of the silicates. The relation between the silicate extinction band depth and H2O ice band depths is determined for the deeply embedded objects. One late-type object, Elias 14, clearly shows the 11.25 micrometer aromatic hydrocarbon emission feature, possibly excited by the nearby B star, HD 147889, though the latter does not exhibit the feature.

Hanner, M. S.↗