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NASA NTRS2017

Mapping Vinyl Cyanide and Other Nitriles in Titan's Atmosphere Using ALMA

Vinyl cyanide (C2H3CN) is theorized to form in Titan's atmosphere via high-altitude photochemistry and is of interest regarding the astrobiology of cold planetary surfaces due to its predicted ability to form cell membrane-like structures (azotosomes) in liquid methane. In this work, we follow up on the initial spectroscopic detection of C2H3CN on Titan by Palmer et al. with the detection of three new C2H3CN rotational emission lines at submillimeter frequencies. These new, high-resolution detections have allowed for the first spatial distribution mapping of C2H3CN on Titan. We present simultaneous observations of C2H5CN, HC3N, and CH3CN emission, and obtain the first (tentative) detection of C3H8 (propane) at radio wavelengths. We present disk-averaged vertical abundance profiles, two-dimensional spatial maps, and latitudinal flux profiles for the observed nitriles. Similarly to HC3N and C2H5CN, which are theorized to be short-lived in Titan's atmosphere, C2H3CN is most abundant over the southern (winter) pole, whereas the longer-lived CH3CN is more concentrated in the north. This abundance pattern is consistent with the combined effects of high-altitude photochemical production, poleward advection, and the subsequent reversal of Titan's atmospheric circulation system following the recent transition from northern to southern winter. We confirm that C2H3CN and C2H5CN are most abundant at altitudes above 200 km. Using a 300 km step model, the average abundance of C2H3CN is found to be 3.03 +/- 0.29ppb, with a C2H5CN/C2H3CN abundance ratio of 2.43 +/- 0.26. Our HC3N and CH3CN spectra can be accurately modeled using abundance gradients above the tropopause, with fractional scale-heights of 2.05 +/- 0.16 and 1.63 +/- 0.02, respectively.

Lai, J. C.-Y.↗
NASA NTRS1972

Origin of organic matter in early solar system. VI - Catalytic synthesis of nitriles, nitrogen bases and porphyrin-like pigments.

A variety of nitrogen compounds have been synthesized by a static Fischer-Tropsch type reaction from CO, D2 and ND3, with Ni-Fe and Al2O3 catalysts. In this reaction, the gas is heated to 500-700 C for about 0.5 hr, and then cycled through lower temperatures (100-400 C) for 1-14 days. Products were analyzed by mass spectrometry in conjunction with gas chromatography and other chromatographic techniques. Compounds produced include alkyl cyanides, pyrroles, porphyrin-like compounds, guanidines, hydantoin, uracil and its derivatives, thymine, adenine, guanine, xanthine, melamine, as well as alkanes, alkenes and aromatic hydrocarbons. Such reactions may have been involved in the production of interstellar molecules, organic compounds in meteorites, and prebiotic organic matter on planets.

Hayatsu, R.↗
NASA NTRS1997

Rate Coefficients for Reactions of Ethynyl Radical (C2H) With HCN and CH3CN: Implications for the Formation of Comples Nitriles on Titan

Rate coefficients for the reactions of C2H + HCN yields products and C2H + CH3CN yields products have been measured over the temperature range 262-360 K. These experiments represent an ongoing effort to accurately measure reaction rate coefficients of the ethynyl radical, C2H, relevant to planetary atmospheres such as those of Jupiter and Saturn and its satellite Titan. Laser photolysis of C2H2 is used to produce C2H, and transient infrared laser absorption is employed to measure the decay of C2H to obtain the subsequent reaction rates in a transverse flow cell. Rate constants for the reaction C2H + HCN yields products are found to increase significantly with increasing temperature and are measured to be (3.9-6.2) x 10(exp 13) cm(exp 3) molecules(exp -1) s(exp -1) over the temperature range of 297-360 K. The rate constants for the reaction C2H + CH3CN yields products are also found to increase substantially with increasing temperature and are measured to be (1.0-2.1) x 10(exp -12) cm(exp 3) molecules(exp -1) s(exp -1) over the temperature range of 262-360 K. For the reaction C2H + HCN yields products, ab initio calculations of transition state structures are used to infer that the major products form via an addition/elimination pathway. The measured rate constants for the reaction of C2H + HCN yields products are significantly smaller than values currently employed in photochemical models of Titan, which will affect the HC3N distribution.

Hoobler, Ray J.↗
NASA NTRS1999

Use of Several Thermal Analysis Techniques to Study the Cracking of a Nitrile Butadiene Rubber (NBR) Insulator on the Booster Separation Motor (BSM) of the Space Shuttle

Two different vendor rubber formulations have been used to produce the silica-filled NBR insulators for the BSM of each of the two Solid Rocket Boosters (SRBs) on the Space Shuttle. Each cured insulator is bonded to the BSM aluminum aft closure with an epoxy adhesive, and some of the curved areas in the rubber may have significant residual stresses. A number of recently bonded NBR insulators have shown fine surface cracks, and stressed insulator areas may be aging at a faster rate than unstressed areas, thus hastening the surface cracking. Thermal analysis data on both vendor insulators by Dynamic Mechanical Analysis (DMA) through a temperature/frequency sweep from 24 to 74 C have shown a higher flexural storage modulus and Arrhenius activation energy for the stressed area than for the unstressed area. Other thermal analysis techniques are being used to study the insulator surface vs. bulk interior for better understanding this anomaly.

Wingard, Charles D.↗
NASA NTRS2000

Use of Several Thermal Analysis Techniques to Study the Cracking of an Nitrile Butadiene Rubber (NBR) Insulator on the Booster Separation Motor (BSM) of the Space Shuttle

Two different vendor rubber formulations have been used to produce the silica-filled NBR insulators for the BSM used on both of the Solid Rocket Boosters (SRBs) of the Space Shuttle. A number of lots of the BSM insulator in 1998-99 exhibited surface cracks and/or crazing. Each insulator is bonded to the BSM aluminum aft closure with an epoxy adhesive. Induced insulator stresses from adhesive cure are likely greatest where the insulator/adhesive contour is the greatest, thus showing increased insulator surface cracking in this area. Thermal analysis testing by Dynamic Mechanical Analyzer (DMA) and Thermomechanical Analysis (TMA) was performed on one each of the two vendor BSM insulators previously bonded that exhibited the surface cracking. The TMA data from the film/fiber technique yielded the most meaningful results, with thin insulator surface samples containing cracks having roughly the same modulus (stiffness) as thin insulator bulk samples just underneath.

Wingard, Charles D.↗
NASA NTRS1997

Polarization and Piezoelectric Properties of a Nitrile Substituted Polyimide

This research focuses on the synthesis and characterization of a piezoelectric (beta-CN)- APB/ODPA polyimide. The remanent polarization and piezoelectric d(sub 31) and g(sub 33) coefficients are reported to assess the effect of synthesis variations. Each of the materials exhibits a level of piezoelectricity which increases with temperature. The remanent polarization is retained at temperatures close to the glass transition temperature of the polyimide.

Simpson, Joycelyn↗
NASA NTRS2010

Infrared Spectra, Index of Refraction, and Optical Constants of Nitrile Ices Relevant to Titan's Atmosphere

Spectra and optical constants of nitrite ices known or suspected to be in Titan's atmosphere are presented from 2.5 to 200 microns (4000 to 50 per cm ). These results are relevant to the ongoing modeling of Cassini CIRS observations of Titan's winter pole. Ices studied include: HCN, hydrogen cyanide; C2N2, cyanogen; CH3CN, acetonitrile; C 2H5CN, propionitrile; and HC3N, cyanoacetylene. For each of these molecules we report new measurements of the index of refraction, n, determined in both the amorphous- and crystallinephase at 670 nm. Spectra were measured and optical constants were calculated for each nitrite at a variety of temperatures including 20, 35, 50, 75, 95, and 110 K, in the amorphous- and crystalline-phase. This laboratory effort uses a dedicated FTIR spectrometer to record transmission spectra of thin-film ice samples. Laser interference is used to measure film thickness during condensation onto a transparent cold window attached to the tail section of a closed-cycle helium cryostat. Optical constants, real (n) and imaginary (k) refractive indices, are determined using Kramers-Kronig (K-K) analysis. Our calculation reproduces the complete spectrum, including all interference effects. Index of refraction measurements are made in a separate dedicated FTIR spectrometer where interference deposit fringes are measured using two 670 nm lasers at different angles to the ice substrate. A survey of these new measurements will be presented along with a discussion of their validation, errors, and application to Titan data.

Moore, Marla↗
NASA NTRS2012

Comets as Messengers from the Early Solar System - Emerging Insights on Delivery of Water, Nitriles, and Organics to Earth

The question of exogenous delivery of water and organics to Earth and other young planets is of critical importance for understanding the origin of Earth's volatiles, and for assessing the possible existence of exo-planets similar to Earth. Viewed from a cosmic perspective, Earth is a dry planet, yet its oceans are enriched in deuterium by a large factor relative to nebular hydrogen and analogous isotopic enrichments in atmospheric nitrogen and noble gases are also seen. Why is this so? What are the implications for Mars? For icy Worlds in our Planetary System? For the existence of Earth-like exoplanets? An exogenous (vs. outgassed) origin for Earth's atmosphere is implied, and intense debate on the relative contributions of comets and asteroids continues - renewed by fresh models for dynamical transport in the protoplanetary disk, by revelations on the nature and diversity of volatile and rocky material within comets, and by the discovery of ocean-like water in a comet from the Kuiper Belt (cf., Mumma & Charnley 2011). Assessing the creation of conditions favorable to the emergence and sustenance of life depends critically on knowledge of the nature of the impacting bodies. Active comets have long been grouped according to their orbital properties, and this has proven useful for identifying the reservoir from which a given comet emerged (OC, KB) (Levison 1996). However, it is now clear that icy bodies were scattered into each reservoir from a range of nebular distances, and the comet populations in today's reservoirs thus share origins that are (in part) common. Comets from the Oort Cloud and Kuiper Disk reservoirs should have diverse composition, resulting from strong gradients in temperature and chemistry in the proto-planetary disk, coupled with dynamical models of early radial transport and mixing with later dispersion of the final cometary nuclei into the long-term storage reservoirs. The inclusion of material from the natal interstellar cloud is probable, for comets formed in the outer solar system.

Mumma, Michael J.↗
NASA NTRS2012

Observations of Nitrogen Fractionation in Prestellar Cores: Nitriles Tracing Interstellar Chemistry

Primitive materials provide important clues on the processes that occurred during the formation and early evolution of the Solar System. Space-based and ground-based observations of cometary comae show that comets appear to contain a mixture of the products of both interstellar and nebular chemistries. Significant 15-nitrogen enrichments have been measured in CN and HCN towards a number of comets and may suggest an origin of interstellar chemical fractionation. Additionally, large N-15 enhancements are found in meteorites and has also led to to the view that the N-15 traces material formed in the interstellar medium (ISM), although multiple sources cannot be excluded. Here, we show the results of observations of the nitrogen and carbon fractionation in prestellar cores for various N-bearing species to decipher the origin of primitive material isotopic enrichments.

Milam, S. N.↗
NASA NTRS2012

Titan's Stratospheric Condensibles at High Northern Latitudes During Northern Winter

The Infrared Interferometer Spectrometer (IRIS) instrument on board Voyager 1 caught the first glimpse of an unidentified particulate feature in Titan's stratosphere that spectrally peaks at 221 per centimeter. Until recently, this feature that we have termed 'the haystack,' has been seen persistently at high northern latitudes with the Composite Infrared Spectrometer (CIRS) instrument onboard Cassini, The strength of the haystack emission feature diminishes rapidly with season, becoming drastically reduced at high northern latitudes, as Titan transitions from northern winter into spring, In contrast to IRIS whose shortest wavenumber was 200 per centimeter, CIRS extends down to 10 per centimeter, thus revealing an entirely unexplored spectral region in which nitrile ices have numerous broad lattice vibration features, Unlike the haystack, which is only found at high northern latitudes during northern winter/early northern spring, this geometrically thin nitrile cloud pervades Titan's lower stratosphere, spectrally peaking at 160 per centimeter, and is almost global in extent spanning latitudes 85 N to 600 S, The inference of nitrile ices are consistent with the highly restricted altitude ranges over which these features are observed, and appear to be dominated by a mixture of HCN and HC3N, The narrow range in altitude over which the nitrile ices extend is unlike the haystack, whose vertical distribution is significantly broader, spanning roughly 70 kilometers in altitude in Titan's lower stratosphere, The nitrile clouds that CIRS observes are located in a dynamically stable region of Titan's atmosphere, whereas CH4 clouds, which ordinarily form in the troposphere, form in a more dynamically unstable region, where convective cloud systems tend to occur. In the unusual situation where Titan's tropopause cools significantly from the HASI 70.5K temperature minimum, CH4 should condense in Titan's lower stratosphere, just like the aforementioned nitrile clouds, although in significantly larger abundances. We will present the spectral and vertical distribution of Titan's stratospheric particulates during northern winter on Titan. The drastically changing abundance of the haystack over a small latitude range will be highlighted, specifically comparing the IRIS and CIRS epochs, Finally, we will discuss the situation in which CH4 condenses in Titan's lower stratosphere, forming an unexpected quasi steady-state stratospheric Ice cloud.

Anderson, Carrie↗
NASA NTRS2003

The Infrared Spectrum of Matrix Isolated Aminoacetonitrile: A Precursor to the Amino Acid Glycine

We present infrared (IR) spectral data from matrix isolation experiments and density functional theory calculations on the pre-biologically interesting molecule aminoacetonitrile, a precursor to glycine. We find that this nitrile has an unusually weak nitrile (C=N) stretch in the infrared, in contrast to expectations based on measurements and models of other nitriles under astrophysical conditions. The absence of an observable nitrile absorption feature in the infrared will make the IR search for this molecule considerably more difficult, and will raise estimates of upper limits on nitriles in interstellar and outer Solar System ices. This is also of relevance to assessing the formation routes of the amino acid glycine, since aminoacetonitrile is the putative precursor to glycine via the Strecker synthesis, the mechanism postulated to have produced the amino acids in meteorites.

Bernstein, Max P.↗
NASA NTRS1982

Development of tough, moisture resistant laminating resins

Tough, moisture resistant laminating resins for employment with graphite fibers were developed. The new laminating resins exhibited cost, handleability and processing characteristics equivalent to 394K (250 F) curing epoxies. The laminating resins were based on bisphenol A dicyanate and monofunctional cyanates with hydrophobic substituents. These resins sorb only small quantities of moisture at equilibrium (0.5% or less) with minimal glass transition temperature depression and represent an improvement over epoxies which sorb around 2% moisture at equilibrium. Toughening was accomplished by the precipitation of small diameter particles of butadiene nitrile rubber throughout the resin matrix. The rubber domains act as microcrack termini and energy dissipation sites, allowing increased stress accommodation prior to catastrophic failure. A unique blend of amine terminated butadiene nitrile elastomer (MW 2,000) and a high nitrile content butadiene nitrile rubber yielded the desired resin morphology.

Brand, R. A.↗
NASA NTRS1973

The prospect of life on Jupiter.

We have simulated electrical discharges in the Jovian atmosphere, using anhydrous methane-ammonia mixtures, and shown the formation of simple aliphatic nitriles, amino-nitriles, and their oligomers. Including hydrogen sulfide in the gas mixture, it appears that sulfur-containing amino-nitriles are not formed, since the hydrolysate of the products did not contain the corresponding amino-acids. There is a strong analogy between these reactions and the classical spark reactions simulating the primitive earth's atmosphere. We are attempting a closer simulation of Jupiter's atmosphere by using appropriate temperature and pressure conditions. It seems that prebiotic synthesis on Jupiter may have reached an advanced state. As an alternative approach we have tested the survival ability of common terrestrial microorganisms in aqueous media at 102 atmospheres pressure and at 20 C in a simulated Jovian atmosphere. E. coli, S. marcescens, A. aerogenes, and B. subtilis will all tolerate 24 hr under these conditions with little death.

Ponnamperuma, C.↗
NASA NTRS1989

Triton - Stratospheric molecules and organic sediments

Continuous-flow plasma discharge techniques show production rates of hydrocarbons and nitriles in N2 + CH4 atmospheres appropriate to the stratosphere of Titan, and indicate that a simple eddy diffusion model together with the observed electron flux quantitatively matches the Voyager IRIS observations for all the hydrocarbons, except for the simplest ones. Charged particle chemistry is very important in Triton's stratosphere. In the more CH4-rich case of Titan, many hydrocarbons and nitriles are produced in high yield. If N2 is present, the CH4 fraction is low, but hydrocarbons and nitriles are produced in fair yield, abundances of HCN and C2H2 in Triton's stratosphere exceed 10 to the 19th molecules/sq cm per sec, and NCCN, C3H4, and other species are predicted to be present. These molecules may be detected by IRIS if the stratosphere is as warm as expected. Both organic haze and condensed gases will provide a substantial UV and visible opacity in Triton's atmosphere.

Thompson, W. Reid↗
NASA NTRS1994

Chemical investigation of Titan and Triton tholins

We report chromatographic and spectroscopic analyses of both Titan and Triton tholins, organic solids made from the plasma irradiation of 0.9:0.1 and 0.999:0.001 N2/CH4 gas mixtures, respectively. The lower CH4 mixing ratio leads to a nitrogen-richer tholin (N/C greater than 1), probably including nitrogen heterocyclic compounds. Unlike Titan tholin, bulk Triton tholin is poor in nitriles. From high-pressure liquid chromatography, ultraviolet and infrared spectroscopy, and molecular weight estimation by gel filtration chromatography, we conclude that (1) several H2O-soluble fractions, each with distinct UV and IR spectral signatures, are present, (2) these fractions are not identical in the two tholins, (3) the H2O-soluble fractions of Titan tholins do not contain significant amounts of nitriles, despite the major role of nitriles in bulk Titan tholin, and (4) the H2O-soluble fractions of both tholins are mainly molcules containing about 10 to 50 (C + N) atoms. We report yields of amino acids upon hydrolysis of Titan and Triton tholins. Titan tholin is largely insoluble in the putative hydrocarbon lakes or oceans on Titan, but can yield the H2O-soluble species investigated here upon contact with transient (e.g., impact-generated) liquid water.

Mcdonald, Gene D.↗
NASA NTRS1999

Molecular Modeling of the Poling of Piezoelectric Polyimides

The computational method described in this paper allows the calculation of the dielectric relaxation strength of an amorphous polymer based solely upon its chemical structure. The 4,4' oxydiphthalic anhydride (ODPA) dianhydride and bis-aminophenoxybenzene (APB) diamine based polyimides, (beta-CN) APB-ODPA and APB-ODPA were studied. Amorphous cells were constructed and then poled using molecular dynamics. Dielectric relaxation strengths of Delta(epsilon) = 17.8 for (beta-CN) APB-ODPA and Delta(epsilon) = 7.7 for APB-ODPA were predicted. These values are in excellent agreement with the experimental values. It was found that both the pendant nitrile dipole and the backbone anhydride residue dipole make significant contributions to the polyimides dielectric response. Specifically, it was shown that the difference in the magnitude of the dielectric relaxations is directly attributable to the nitrile dipole. The size of the relaxations indicate an absence of cooperative dipolar motions, The model was used to explain these results in terms of the average orientation of the nitrile and anhydride dipoles to within 51 deg. and 63 deg., respectively, of the applied electric field.

Young, J. A.↗