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NASA NTRS1998

Far Infrared Line Profiles from Photodissociation Regions and Warm Molecular Clouds

This report summarizes the work done under NASA Grant NAG2-1056 awarded to the University of Colorado. The aim of the project was to analyze data obtained over the past several years with the University of Colorado far-infrared heterodyne spectrometer (Betz Boreiko 1993) aboard the Kuiper Airborne Observatory. Of particular interest were observations of CO and ionized carbon (C II) in photodissociation regions (PDRS) at the interface between UV-ionized H II regions and the neutral molecular clouds supporting star formation. These data, obtained with a heterodyne spectrometer having a resolution of 3.2 MHz, which is equivalent to a velocity resolution of 0.2 km/s at 60 microns and 1.0 km/s at 300 microns, were analyzed to obtain physical parameters such as density and temperature in the observed PDR. The publication resulting from the work reported here is appended. No inventions were made nor was any federally owned property acquired as a result of the activities under this grant.

Boreiko, R. T.↗
NASA NTRS1998

Far Infrared Line Profiles from Photodissociation Regions and Warm Molecular Clouds

This report summarizes the work done under NASA Grant NAG2-1056 awarded to the University of Colorado. The aim of the project was to analyze data obtained over the past several years with the University of Colorado far-infrared heterodyne spectrometer (Betz & Boreiko 1993) aboard the Kuiper Airborne Observatory. Of particular interest were observations of CO and ionized carbon (C II) in photodissociation regions (PDRs) at the interface between UV-ionized H II regions and the neutral molecular clouds supporting star formation. These data, obtained with a heterodyne spectrometer having a resolution of 3.2 MHz, which is equivalent to a velocity resolution of 0.2 km/s at 60 microns and 1.0 km/s at 300 microns, were analyzed to obtain physical parameters such as density and temperature in the observed PDR. The publication resulting from the work reported here is appended. No inventions were made nor was any federally owned property acquired as a result of the activities under this grant.

Boreiko, R. T.↗
NASA NTRS1998

Far Infrared Line Profiles from Photodissociation Regions and Warm Molecular Clouds

This report summarizes the work done under NASA Grant NAG2-1056 awarded to the University of Colorado. The aim of the project was to analyze data obtained over the past several years with the University of Colorado far-infrared heterodyne spectrometer aboard the Kuiper Airborne Observatory. Of particular interest were observations of CO and ionized carbon (C II) in photodissociation regions (PDRS) at the interface between UV-ionized H II regions and the neutral molecular clouds supporting star formation. These data, obtained with a heterodyne spectrometer having a resolution of 3.2 MHz, which is equivalent to a velocity resolution of 0.2 km s(exp -1) at 60 microns and 1.0 km s(exp -1) at 300 microns, were analyzed to obtain physical parameters such as density and temperature in the observed PDR.

Boreiko, R. T.↗
NASA NTRS2014

Alteration of Basaltic Glass to Mg/Fe-Smectite under Acidic Conditions: A Potential Smectite Formation Mechanism on Mars

Phyllosilicates of the smectite group including Mg- and Fe-saponite and Fe(III)-rich nontronite have been identified on Mars. Smectites are believed to be formed under neutral to alkaline conditions that prevailed on early Mars. This hypothesis is supported by the observation of smectite and carbonate deposits in Noachian terrain on Mars. However, smectite may have formed under mildly acidic conditions. Abundant smectite formations have been detected as layered deposits hundreds of meters thick in intracrater depositional fans and plains sediments, while no large deposits of carbonates are found. Development of mildly acidic conditions at early Mars might allow formation of smectite but inhibit widespread carbonate precipitation. Little is known regarding the mechanisms of smectite formation from basaltic glass under acidic conditions. The objective of this study was to test a hypothesis that Mars-analogue basaltic glass alters to smectite minerals under acidic conditions (pH 4). The effects of Mg and Fe concentrations and temperature on smectite formation from basaltic glass were evaluated. Phyllosilicate synthesis was performed in batch reactors (Parr acid digestion vessel) under reducing hydrothermal conditions at 200 C and 100 C. Synthetic basaltic glass with a composition similar to that of the Gusev crater rock Adirondack (Ground surface APXS measurement) was used in these experiments. Basaltic glass was prepared by melting and quenching procedures. X-ray diffraction (XRD) analysis indicated that the synthesized glass was composed of olivine, magnetite and X-ray amorphous phase. Samples were prepared by mixing 250 mg Adirondack with 0.1 M acetic acid (final pH 4). In order to study influence of Mg concentration on smectite formation, experiments were performed with addition of 0, 1 and 10 mM MgCl2. After 1, 7 and 14 day incubations the solution composition was analyzed by Inductively Coupled Plasma Mass Spectrometry (ICP-MS) and the altered glass and formed phyllosilicates were examined by XRD analysis. Mineralogical changes were significant in Adirondack incubated with 10 mM MgCl2 at pH 4 and heated at 200 C. X-ray diffraction analysis revealed formation of phyllosilicate during 14 day incubation (Figure 1). Smectite was confirmed as the phyllosilicate after treatments with glycerol and KCl and heating to 550 C. The position of 02l (4.60 A) and 060 (1.54 A) diffraction bands were indicative of trioctahedral smectite such as saponite. Analysis of solution composition demonstrated that aqueous concentration of Mg decreased from 10 mM to approx.4 mM after 7 day incubation likely due to saponite formation. Smectite also formed in Adirondack incubated with 0 mM MgCl2 at pH 4 and heated at 200 C. However, diffraction peak positions of 02l (4.52 A) and 060 (1.51 A) suggested formation of dioctahedral nontronite. The 100degC Mg and Fe(II) treated basaltic glass experiments are ongoing and results will be presented.

Peretyazhko, Tanya↗
NASA NTRS1980

Molecular wake shield gas analyzer

Techniques for measuring and characterizing the ultrahigh vacuum in the wake of an orbiting spacecraft are studied. A high sensitivity mass spectrometer that contains a double mass analyzer consisting of an open source miniature magnetic sector field neutral gas analyzer and an identical ion analyzer is proposed. These are configured to detect and identify gas and ion species of hydrogen, helium, nitrogen, oxygen, nitric oxide, and carbon dioxide and any other gas or ion species in the 1 to 46 amu mass range. This range covers the normal atmospheric constituents. The sensitivity of the instrument is sufficient to measure ambient gases and ion with a particle density of the order of one per cc. A chemical pump, or getter, is mounted near the entrance aperture of the neutral gas analyzer which integrates the absorption of ambient gases for a selectable period of time for subsequent release and analysis. The sensitivity is realizable for all but rare gases using this technique.

Hoffman, J. H.↗
NASA NTRS1993

Low-gravity electrodeposition and growth of polymer thin films with large third-order optical nonlinearities by electrochemical processes for devices: Thiophene-based polymers

It has been proposed that NLO thin film properties may be improved by low-gravity processing. Strong candidates for NLO thin film applications are the polythiophenes. Polymeric thiophenes are attractive materials due to their ease of preparation, stability, and high X(exp 3). A simple and convenient method for preparation of polythiophenes is electrochemical oxidation. We will apply some of our experience and lessons learned in low-gravity metal, metal/cermet electrode position to improve the quality of polythiophene(s) thin films. In low gravity electrode position of Ni at a high rate on an Au substrate often results in the production of an x-ray non diffracting surface. Cobalt metal deposition does not give this result nor does Ni when deposited similarly on a glassy carbon substrate. Co/Ni alloy composition produced during electrode position is strongly dependent upon the amount of convection. Code position of neutral inert cermets with metals is influenced significantly by the presence of gravity and the size of the cermets. Tracks left in the 1-g surfaces by unsuccessful particle occlusion indicate suspension of the large particles is not the only reason for poor volume percentages of the larger particles in the deposits. All size particles are more homogeneously distributed in the deposits in low-gravity electrocodeposition than in 1-g. Low gravity gives larger volume percentages for the larger particles in the deposits, while 1-g gives larger volume percentages for the smaller particles. Intermediate size particles give mixed results. The experimental cells were constructed with flat electrode end plates such that 1-g bench reference electrode positions could be carried out at various orientations with respect to gravity. A series of bench studies using similar designed cells are suggested so that convection modification can be applied to electrochemical thin film preparation. Convection effects can then be coupled with other parameter variations in current, temperature, concentration, solvent, electrolyte, and anode substrates to optimize the properties of NLO thin films before resorting to low-gravity processing.

Penn, Benjamin G.↗
NASA NTRS2006

Laboratory Spectroscopy of Large Carbon Molecules and Ions in Support of Space Missions. A New Generation of Laboratory & Space Studies

Polycyclic Aromatic Hydrocarbons (PAHs) are an important and ubiquitous component of carbon-bearing materials in space. A long-standing and major challenge for laboratory astrophysics has been to measure the spectra of large carbon molecules in laboratory environments that mimic (in a realistic way) the physical conditions that are associated with the interstellar emission and absorption regions [1]. This objective has been identified as one of the critical Laboratory Astrophysics objectives to optimize the data return from space missions [2]. An extensive laboratory program has been developed to assess the properties of PAHs in such environments and to describe how they influence the radiation and energy balance in space. We present and discuss the gas-phase electronic absorption spectra of neutral and ionized PAHs measured in the UV-Visible-NIR range in astrophysically relevant environments and discuss the implications for astrophysics [1]. The harsh physical conditions of the interstellar medium characterized by a low temperature, an absence of collisions and strong VUV radiation fields - have been simulated in the laboratory by associating a pulsed cavity ringdown spectrometer (CRDS) with a supersonic slit jet seeded with PAHs and an ionizing, penning-type, electronic discharge. We have measured for the {\it first time} the spectra of a series of neutral [3,4] and ionized [5,6] interstellar PAHs analogs in the laboratory. An effort has also been attempted to quantify the mechanisms of ion and carbon nanoparticles production in the free jet expansion and to model our simulation of the diffuse interstellar medium in the laboratory [7]. These experiments provide {\it unique} information on the spectra of free, large carbon-containing molecules and ions in the gas phase. We are now, for the first time, in the position to directly compare laboratory spectral data on free, cold, PAH ions and carbon nano-sized carbon particles with astronomical observations in the UV-NIR range (interstellar UV extinction, DIBs in the NUV-NIR range). This new phase offers tremendous opportunities for the data analysis of current and upcoming space missions geared toward the detection of large aromatic systems Le., the "new frontier space missions" (Spitzer, HST, COS, JWST, SOFIA,...).

Salama, Farid↗
NASA NTRS1995

Ultraviolet extinction to 10.8 inverse microns

UV extinction curves that represent observed variations i diffuse clouds (Zeta Oph, Xi Per, and Sigma Sco) have been derived by combining IUE and Voyager data and have been modeled by a multicomponent size distribution of silicate and carbonaceous giants. We have used theoretical model atmospheres as our reddening-free standards, and, in the case of Zeta Oph, also compare with the use of a stellar standard. An attempt was made to classify the UV spectra via theoretical spectral indices, but still missing line opacity appears to limit the use of this method at the present. The modeling includes five possible grain ingrediants, largge (0.015-0.25 micrometers) and small (0.005 micrometers) silicate grains, similarly large and small carbonaceous grains, and polycyclic aromatic hydrocarbons (PAHs). The observed extinction curves are fitted by the model via nonlinear Chi-square-minimization, varying the fractional amount of cosmic Si and C that are locked up in each igredient. The observed variation from 'steep' to 'flat' UV extinction curves is found to correspond to a modest model variation in the lower limit of the power-law size distribution of the large grains. Graphite is found to be necessary grain ingredient that cannot be replaced by the laboratory amorphous carbon materials. Carbonaceous mantles on the larger silicate grains provide no good fits to the observed curves. Using absorption properties of neutral laboratory PAHs limits PAHs to a few percent of the cosmic C abundance for acceptable fits that also give values for R(sub V) close to the observed values.

Aannestad, Per A.↗
NASA NTRS2006

Astrochemistry: Recent Advances in the Study of Carbon Molecules in Space

Carbon molecules and ions play an important role in space. Polycyclic Aromatic Hydrocarbons (PAHs) are the best-known candidates to account for the infrared emission bands (UIR bands) and PAH spectral features are now being used as probes of the interstellar medium in Galactic and extra-galactic environments. PAHs are also thought to be among the carriers of the diffuse interstellar absorption bands (DIBs). In the model dealing with the interstellar spectral features, PAHs are present as a mixture of radicals, ions and neutral species. PAH ionization states reflect the ionization balance of the medium while PAH size, composition, and structure reflect the energetic and chemical history of the medium. A major challenge for laboratory Astrochemistry is to reproduce (in a realistic way) the physical conditions that exist in the emission and absorption interstellar zones. An extensive laboratory program has been developed in various laboratories to characterize the physical and chemical properties of PAHs in astrophysical environments and to describe how they influence the radiation and energy balance in space and the interstellar chemistry. In particular, laboratory experiments provide measurements of the spectral characteristics of interstellar PAH analogs from the ultraviolet and visible range to the infrared range for comparison with astronomical data. The harsh physical conditions of the interstellar medium - characterized by a low temperature, an absence of collisions and strong ultraviolet radiation fields - are simulated in the laboratory by associating a molecular beam with an ionizing discharge to generate a cold plasma expansion. PAH ions are formed from the neutral precursors in an isolated environment at low temperature (of the order of 100 K). The spectra of neutral and ionized PAHs are measured using the high sensitivity methods of cavity ring down spectroscopy (CRDS). These experiments provide unique information on the spectra of free, cold large carbon molecules and ions in the gas phase.

Salama, Farid↗
NASA NTRS1980

Properties of clusters in the gas phase. V - Complexes of neutral molecules onto negative ions

Ion-molecules association reactions of the form A(-)(B)n-1 + B = A(-)(B)n were studied over a range of temperatures in the gas phase using high pressure mass spectrometry. Enthalpy and entropy changes were determined for the stepwise clustering reactions of (1) sulfur dioxide onto Cl(-), I(-), and NO2(-) with n ranging from one to three or four, and onto SO2(-) and SO3(-) with n equal to one; and (2) carbon dioxide onto Cl(-), I(-), NO2(-), CO3(-), and SO3(-) with n equal to one. From these data and earlier hydration results, the order of the magnitude of the enthalpy changes on the association of the first neutral for a series of negative ions was found to parallel the gas-phase basicity of those anions.

Keesee, R. G.↗
NASA NTRS1979

Venus upper atmosphere neutral gas composition - First observations of the diurnal variations

Measurements of the composition, temperature, and diurnal variations of the major neutral constituents in the thermosphere of Venus are being made with a quadrupole mass spectrometer on the Pioneer Venus Orbiter. Concentrations of carbon dioxide, carbon monoxide, molecular nitrogen, atomic oxygen, and helium are presented, in addition to an empirical model of the data. The concentrations of the heavy gases, carbon dioxide, carbon monoxide, and molecular nitrogen, rapidly decrease from the evening terminator toward the nightside; the concentration of atomic oxygen remains nearly constant and the helium concentration increases, an indication of a nightside bulge. The kinetic temperature inferred from scale heights drops rapidly from 230 K at the terminator to 130 K at a solar zenith angle of 120 deg, and to 112 K at the antisolar point.

Niemann, H. B.↗
NASA NTRS2021

Venus' Mass Spectra Show Signs of Disequilibria in the Middle Clouds

We present a re‐examination of mass spectral data obtained from the Pioneer Venus Large Probe Neutral Mass Spectrometer. Our interpretations of differing trace chemical species are suggestive of redox disequilibria in Venus' middle clouds. Assignments to the data (at 51.3 km) include phosphine, hydrogen sulfide, nitrous acid, nitric acid, carbon monoxide, hydrochloric acid, hydrogen cyanide, ethane, and potentially ammonia, chlorous acid, and several tentative PxOy species. All parent ions were predicated upon assignment of corresponding fragmentation products, isotopologues, and atomic species. The data reveal parent ions at varying oxidation states, implying the presence of reducing power in the clouds, and illuminating the potential for chemistries yet to be discovered. When considering the hypothetical habitability of Venus' clouds, the assignments reveal a potential signature of anaerobic phosphorus metabolism (phosphine), an electron donor for anoxygenic photosynthesis (nitrite), and major constituents of the nitrogen cycle (nitrate, nitrite, ammonia, and N2).

disequilibria↗
NASA NTRSDate not supplied

The Chemical Evolution of Cosmic Dust: From Gas-Phase Precursors to Solid Grains - Laboratory Studies with the COSmIC Facility

Cosmic dust in in its gas phase and solid phase components plays an essential role in the chemical and physical evolution of the universe. Our understanding of cosmic dust properties relies on a combination of astronomical observations, astrophysical modeling and laboratory studies of realistic analogs of cosmic dust being gas-phase molecules and/or solid grains. The COSmIC facility was developed at NASA Ames to study the evolution of cosmic carbon from circumstellar outflows to interstellar clouds to planetary atmospheres in the laboratory. COSmIC stands for “Cosmic Simulation Chamber” and is dedicated to the study of neutral and ionized molecules and grain particles under the low temperature and density conditions that are required to simulate space environments. It integrates a variety of instruments that allow generating, processing, and monitoring simulated space conditions in the laboratory. It is composed of a Pulsed Discharge Nozzle (PDN) expansion that generates a plasma in a free supersonic jet expansion, coupled to high-sensitivity, complementary in situ diagnostic tools used for the detection and characterization of the species present in the expansion: Cavity Ring Down Spectroscopy (CRDS) and fluorescence spectroscopy systems for photonic detection and an orthogonal Reflectron Time-Of-Flight Mass Spectrometer (oReTOF-MS) for mass detection. Recent advances achieved using COSmIC’s laboratory data in synergy with observational data will be presented. These results include the formation of dust grains and aerosols from gas-phase molecular precursors in environments as varied as circumstellar outflows of late AGB stars and planetary atmospheres [4] and the evolution of our understanding of the diffuse interstellar bands (DIBs) with applications to the ESO Diffuse Interstellar Bands Large Exploration Survey (EDIBLES). Plans for future laboratory developments and techniques to study the evolution of cosmic carbon molecules and grains (including NIR-MIR CRDS, laser induced fluorescence (LIF) and incandescence (LII)) will also be addressed as well as their astronomical applications.

Farid Salama↗
NASA NTRSDate not supplied

The Chemical Evolution of Cosmic Dust: From Gas-Phase Precursors to Solid Grains - Laboratory Studies with the COSmIC Facility

Cosmic dust in in its gas phase and solid phase components plays an essential role in the chemical and physical evolution of the universe. Our understanding of cosmic dust properties relies on a combination of astronomical observations, astrophysical modeling and laboratory studies of realistic analogs of cosmic dust being gas-phase molecules and/or solid grains. The COSmIC facility was developed at NASA Ames to study the evolution of cosmic carbon from circumstellar outflows to interstellar clouds to planetary atmospheres in the laboratory [1]. COSmIC stands for “Cosmic Simulation Chamber” and is dedicated to the study of neutral and ionized molecules and grain particles under the low temperature and density conditions that are required to simulate space environments. It integrates a variety of instruments that allow generating, processing, and monitoring simulated space conditions in the laboratory. It is composed of a Pulsed Discharge Nozzle (PDN) expansion that generates a plasma in a free supersonic jet expansion, coupled to high-sensitivity, complementary in situ diagnostic tools used for the detection and characterization of the species present in the expansion: Cavity Ring Down Spectroscopy (CRDS) and fluorescence spectroscopy systems for photonic detection and an orthogonal Reflectron Time-Of-Flight Mass Spectrometer (oReTOF-MS) for mass detection. Recent advances achieved using COSmIC’s laboratory data in synergy with observational data will be presented. These results include the formation of dust grains and aerosols from gas-phase molecular precursors in environments as varied as circumstellar outflows of late AGB stars [2, 3] and planetary atmospheres [4] and the evolution of our understanding of the diffuse interstellar bands (DIBs) with applications to the ESO Diffuse Interstellar Bands Large Exploration Survey (EDIBLES [5, 6]). Plans for future laboratory developments and techniques to study the evolution of cosmic carbon molecules and grains (including NIR-MIR CRDS, laser induced fluorescence (LIF) and incandescence (LII)) will also be addressed as well as their astronomical applications.

Planetary↗
NASA NTRS2019

The Chemical Evolution of Cosmic Carbon: Laboratory Studies with the COSmIC Facility

Cosmic dust plays an essential role in our understanding of the chemical and physical evolution of the universe. Our understanding of cosmic dust relies on a combination of astronomical observations (either remote or on extraterrestrial dust samples), astrophysical modeling and laboratory studies of realistic analogs of cosmic dust grains. The COSmIC facility was developed at NASA Ames to study the evolution of cosmic carbon from circumstellar outflows to interstellar clouds to planetary atmospheres in the laboratory [1]. COSmIC stands for “Cosmic Simulation Chamber” and is dedicated to the study of neutral and ionized molecules and grain particles under the low temperature and density conditions that are required to simulate space environments. COSmIC integrates a variety of instruments that allow generating, processing, and monitoring simulated space conditions in the laboratory. It is composed of a Pulsed Discharge Nozzle (PDN) expansion that generates a plasma in a free supersonic jet expansion, coupled to high-sensitivity, complementary in situ diagnostic tools used for the detection and characterization of the species present in the expansion: Cavity Ring Down Spectroscopy (CRDS) and fluorescence spectroscopy systems for photonic detection and an orthogonal Reflectron Time-Of-Flight Mass Spectrometer (oReTOF-MS) for mass detection. Recent advances achieved in laboratory astrophysics using COSmIC’s laboratory data in synergy with observational data will be presented. These results include the formation of dust grains and aerosols from gas-phase molecular precursors in environments as varied as circumstellar outflows of late AGB stars [2] and planetary atmospheres [3] and the evolution of our understanding of the diffuse interstellar bands (DIBs) with applications to the ESO Diffuse Interstellar Bands Large Exploration Survey (EDIBLES [4, 5]). Plans for future laboratory developments and techniques to study the evolution of cosmic carbon molecules and grains (including NIR-MIR CRDS, laser induced fluorescence (LIF) and incandescence (LII)) will also be addressed as well as their astronomical applications.

Salama, F.↗
NASA NTRS2000

Molecular Spectroscopy in Astrophysics: The Case of Polycyclic Aromatic Hydrocarbons

The role of molecular spectroscopy in astrophysics and astrochemistry is discussed in the context of the study of large, complex, carbon-bearing molecules, namely, Polycyclic Aromatic Hydrocarbons or PAHs. These molecular species are now thought to be widespread in the interstellar medium in their neutral and ionized forms. Identifying the carriers responsible for unidentified interstellar spectral bands will allow to derive important information on cosmic elemental abundances as well as information on the physical conditions (density, temperature) reigning in specific interstellar environments. These, in turn, are key elements for a correct understanding of the energetic mechanisms that govern the origin and the evolution of the interstellar medium. A multidisciplinary approach - combining astronomical observations with laboratory simulations and theoretical modeling - is required to address these complex issues. Laboratory spectra of several PAHs, isolated at low temperature in inert gas matrices or seeded in a supersonic jet expansion, are discussed here and compared to the astronomical spectra of reddened, early type, stars. The electronic spectroscopy of PAHs in the ultraviolet, visible, and near-infrared domains is reviewed and an assessment of the potential contribution of PAHs to the interstellar extinction in the ultraviolet and in the visible is discussed.

Salama, Farid↗
NASA NTRS2010

Polycyclic Aromatic Hydrocarbons

Carbonaceous materials play an important role in space. Polycyclic Aromatic Hydrocarbons (PAHs) are a ubiquitous component of the carbonaceous materials. PAHs are the best-known candidates to account for the IR emission bands. They are also thought to be among the carriers of the diffuse interstellar absorption bands (DIBs). PAH ionization states reflect the ionization balance of the medium while PAH size, composition, and structure reflect the energetic and chemical history of the medium. A major challenge is to reproduce in the laboratory the physical conditions that exist in the emission and absorption interstellar zones. The harsh physical conditions of the ISM -low temperature, collisionless, strong UV radiation fields- are simulated in the laboratory by associating a molecular beam with an ionizing discharge to generate a cold plasma expansion. PAH ions and radicals are formed from the neutral precursors in an isolated environment at low temperature and probed with high-sensitivity cavity ringdown spectroscopy in the NUV-NIR range. Carbon nanoparticles are also formed during the short residence time of the precursors in the plasma and are characterized with time-offlight mass spectrometry. These experiments provide unique information on the spectra of large carbonaceous molecules and ions in the gas phase that can now be directly compared to interstellar and circumstellar observations (IR emission bands, DIBs, extinction curve). These findings also hold great potential for understanding the formation process of interstellar carbonaceous grains. We will review recent progress in the experimental and theoretical studies of PAHs, compare the laboratory data with astronomical observations and discuss the global implications.

Salama, Farid↗