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At least 109 records · Page 6
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Extreme Molecular Complexity Resulting in a Continuum of Carbonaceous Species in Biomass Burning Tar Balls from Wildfire Smoke

Biomass burning emits a wide range of carbonaceous particles into the atmosphere and has negative impacts on human health and the Earth’s radiative balance. Nonvolatile spherical organic aerosol particles, commonly known as tar balls, represent one of the most abundant particles in aged biomass burning smoke. However, the detailed molecular-level composition of ambient tar balls is largely unknown but critical to access their environmental impacts. Ambient aerosol samples collected during a wildfire event, which were ~90% tar balls by number fraction, were analyzed using ultrahigh resolution Orbitrap Elite mass spectrometry with four complementary ionization modes. Our results show the molecular composition of tar balls to be complex, composed of over 10,000 molecular formulas. Model estimated saturation mass concentrations and relative humidity dependent glass transition temperatures were consistent with low volatility and solid morphology as expected for tar balls. Room-temperature evaporation kinetics showed that these particles were composed of ~90% non-volatile species. The molecular complexity detected here signifies a continuum of carbonaceous species, ranging from C3 to C45 with continuous ranges of oxygenation and hydrogen saturation for each Cn. Approximately 24% of molecular formulas were estimated the be highly aromatic, which could indicate chemical compounds with negative health effects, and which may contribute to visible light absorption. The carbon continuum observed here has significant implications for the molecular characterization of atmospheric organic matter. The level of complexity detected here should not be ignored in future studies and we demonstrate that multiple analytical methods may be required to suitably interpret this complexity on a molecular level.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

TRACER Carbonaceous Aerosols Thrust – University of California, Davis Field Campaign Report

The broader U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility’s TRacking Aerosol Convection interactions ExpeRiment (TRACER) campaign aims to increase our understanding of convective cloud life cycles and aerosol-convection interactions. Our TRACER Carbonaceous Aerosols Thrust-University of California, Davis (TRACER-CAT-UCDavis) study complemented these broader aims by characterizing and quantifying the optical properties and composition of carbonaceous aerosols during part of the TRACER intensive sampling period (July 1- July 31, 2022) at the first ARM Mobile Facility (AMF1) main site (M1) in La Porte, Texas. Our measurements complemented the suite of instrumentation already provided by the AMF1, expanding the capabilities through deployment of unique, state-of-the-science instrumentation. The instrumentation included: (i) two cavity-attenuated phase shift spectroscopy single-scatter albedo (CAPS-SSA) instruments operating at 530 nm and 630 nm, and that were modified to characterize particle light absorption, extinction, and scattering at elevated humidities; (ii) the UC Davis dual-wavelength cavity ringdown-photoacoustic spectrometer (CRD-PAS), which characterizes dry particle extinction and absorption at 405 nm and 532 nm; (iii) a soot particle aerosol mass spectrometer (SP-AMS) that operated in “laser only” mode that characterized the size-dependent compositions of black carbon (BC)-containing particles; (v) a thermal denuder, to remove coatings on particles; and (vi) a scanning electrical mobility sizer (SEMS), to characterize particle mobility diameters from 10-1300 nm. Our measurements occurred alongside complementary observations made by Los Alamos National Laboratory (LANL) during the TRACER-CAT-LANL study, including a humidified CAPS-SSA instrument operating at 450 nm. Our primary scientific interest is in understanding the relationship between particle composition and light absorption, with a particular focus on the influence of water uptake. While it is known that coatings on BC can enhance absorption, the extent to which this occurs in the atmosphere and the specific role that water plays as a coating remain unclear. The TRACER-CAT-UCDavis measurements were made with near-complete coverage for the CRD-PAS, SP-AMS, and SEMS throughout the intensive period. The UC Davis humidified CAPS-SSA instruments had significant challenges with operation owing to the demanding conditions (large temperature fluctuations, high humidity), exacerbated by supply chain issues that delayed resolution of these challenges. However, the humidified CAPS-SSA instrument operated by LANL operated throughout the intensive period with near-complete coverage. The dry light extinction measurements from the CRD-PAS measurements and the LANL CAPS-SSA exhibited a good correlation, although the CAPS-SSA systematically measured greater extinction values than expected. While all instruments, with the exception of an aerodynamic particle sizer (APS), measured behind a common particulate matter (PM)2.5 μm cyclone, the greater extinction measured by the LANL CAPS-SSA compared to the CRD-PAS may have resulted from different losses of larger particles in the sampling lines from the cyclone to the instruments; the tubing length was shorter from the cyclone to the LANL CAPS-SSA, consistent with this idea. A summary of the TRACER-CAT-UCDavis measurements, along with some of the TRACER-CAT-LANL measurements, are shown in the figure below. Notably, there were periods when the contributions of presumed dust were substantial and even dominated the observed light extinction and absorption. Also, there was a clear shift in the behavior of submicron particles from before July 16, 2022 to after, with the prior period exhibiting regular episodes of new particle formation and the latter period exhibiting rapid variations in the concentrations of small particles.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1972

Isotopic compositions of rare gases in the carbonaceous chondrites Mokoia and Allende.

The isotopic compositions have been measured mass spectrometrically for neon, argon, krypton and xenon released from the carbonaceous chondrites Mokoia and Allende in stepwise heating experiments. The isotopic compositions of rare gases released from the meteorites at different temperatures varied quite considerably. A marked enrichment of Xe129 due to the decay of extinct nuclide I129 was observed in both meteorites. The variations of the isotopic ratios are partly caused by the presence of cosmic-ray spallation and neutron-capture products. In addition, however, a marked trend of mass-dependent variation of the isotopic ratios was observed in this work. The rare gas isotopes released from the meteorites appear to be systematically mass-fractionated relative to the relative abundances of the average carbonaceous chondrite. It seems that this phenomenon can be best explained as due to the fact that there exist reservoirs of two isotopically distinct gases in the meteorites and mixtures of these gases are being released at each temperature fraction.

Manuel, O. K.↗
NASA NTRS1972

Xenon in carbonaceous chondrites.

A table showing the relative amounts of xenon isotopes in carbonaceous chondrites is presented. It is found that the enrichment of heavy xenon isotopes released from carbonaceous chondrites in the approximate temperature range from 600 to 1000 C is accompanied by an enrichment of the light xenon isotopes. The high degree of correlation between these two isotopic anomalies suggests that both result from a common source. There is no known nuclear or physical process which could produce both anomalies in situ. It is, therefore, suggested that the anomalies are the result of the release of isotopically anomalous xenon which was trapped in the meteorites.

Manuel, O. K.↗
NASA NTRS1973

Inter-element relationships between trace elements in primitive carbonaceous and unequilibrated ordinary chondrites.

The results of a search for significant interelement relationships among 13 trace elements in carbonaceous chondrites and 26 elements and the disequilibrium parameter for silicate phases in unequilibrated ordinary chondrites (UOC) indicate pronounced differences in the formation processes of these two sorts of primitive chondrites. Twenty-six pairs of elements are correlated in carbonaceous chondrites and these correlations lend support to a model involving mixing in different ratios of material differing in thermal history. Comparison of the 26 elements in UOC shows that 39 pairs of elements are significantly related and only very volatile elements are correlated with the disequilibrium parameter. Each of the interelement relationships can be specifically ascribed to a metal-silicate fractionation in the solar nebula or to a thermal fractionation.

Kurimoto, R. K.↗
NASA NTRS1973

Solar wind xenon in some carbonaceous chondrites.

A table shows the isotopic composition of xenon from several carbonaceous chondrites in which the presence of solar xenon can be demonstrated. The data suggest the presence of a solar xenon component in these carbonaceous chondrites, but solar xenon in these meteorites can be more clearly demonstrated through correlation plots. It is argued that the incorporation of the solar type of noble gases must have occurred during the early history of meteoritic matter when this material consisted of fine-grained particles.

Sabu, D. D.↗
NASA NTRS1975

The low-temperature electrical properties of carbonaceous meteorites

Electrical conductivities and dielectric constants have been measured over the temperature range 90-300 K on several carbonaceous chondrites and some terrestrial analogues. The conductivities of meteorites of different petrologic subtypes range over many orders of magnitude and the low-temperature activation energies are typically much smaller than those observed in terrestrial materials at higher temperatures. The electrical properties of carbonaceous chondrites vary systematically with chemical-mineralogical characteristics in that: (1) activation energy at low temperature is greater in the more volatile-rich meteorites containing hydrated silicates, and (2) conductivity is greater in the more reduced meteorites of higher petrologic subtype. These new data on the electrical properties of chondrites hold important implications for both the thermal and magnetic histories of small bodies in the early solar system.

Brecher, A.↗
NASA NTRS1976

Carbonaceous chondritic xenoliths and planetary-type noble gases in gas-rich meteorites

The source of the planetary-type noble gases in gas-rich meteorites is identified as finely divided (submillimeter to millimeter-sized), widely dispersed carbonaceous chondritic fragments. Trace-element abundances, noble-gas elemental abundances and isotopic abundances of xenon are compatible with the hypothesis that the carbonaceous chondritic carrier is present in amounts of a few percent in the gas-bearing portions of gas-rich chondrites and achondrites.

Wilkening, L. L.↗
NASA NTRS1978

The composition of Phobos - Evidence for carbonaceous chondrite surface from spectral analysis

In connection with a need for more definitive information concerning the composition of Phobos in a study of its origin, an ultraviolet-visible-infrared reflectance spectrum of the Martian satellite was compiled from the Mariner 9 ultraviolet spectrometer, Viking lander imaging, and ground-based photometric data. The probable surface composition of Phobos was deduced by comparing the obtained spectrum with the spectra of asteroids of known composition. The considered data show that the reflectivity of Phobos is flat from 1100 to 400 nm but decreases sharply in the ultraviolet to about 1 percent at 212 nm. The reflectance spectrum is similar to the spectra of asteroids Ceres and Pallas which were found to have surface compositions similar to that of carbonaceous chondrites. It is concluded that the surface composition of Phobos is also similar to that of carbonaceous chondrites. The results of the investigation point to different modes of origin for Mars and Phobos.

Pang, K. D.↗
NASA NTRS1978

Multicolor observations of Phobos with the Viking lander cameras - Evidence for a carbonaceous chondritic composition

The reflectivity of Phobos has been determined in the spectral region from 0.4 to 1.1 micrometers from images taken with a Viking lander camera. The reflectivity curve is flat in this spectral interval and the geometric albedo equals 0.05 + or - 0.01. These results, together with Phobos's reflectivity spectrum in the ultraviolet, are compared with laboratory spectra of carbonaceous chondrites and basalts. The spectra of carbonaceous chondrites are consistent with the observations, whereas the basalt spectra are not. These findings raise the possibility that Phobos may be a captured object rather than a natural satellite of Mars.

Pollack, J. B.↗
NASA NTRS1978

Textural evidence bearing on the origin of isolated olivine crystals in C2 carbonaceous chondrites

In some cases the mechanical competence of chondrules in carbonaceous chondrites has been reduced by alteration of their mesostasis glass to friable phyllosilicate, providing a mechanism by which euhedral olivines can be separated from chondrules. Morphological features of isolate olivine grains found in carbonaceous chondrites are similar to those of olivine phenocrysts in chondrules. These observations suggest that the isolated olivine grains formed in chondrules, by crystallization from a liquid, rather than by condensation from a vapor.

Richardson, S. M.↗
NASA NTRS1978

Carbonaceous chondritic material in the solar system

Carbonaceous chondritic matrix material (CCMM) appears to be an important planet-forming unit in the mid-solar system, from the orbits of Mars to that of Uranus. The type specimen for CCMM is the low-temperature (400-500 K) assemblage of clay minerals, organic polymer, magnetite, and Ni-rich iron sulfides which constitutes the black, fine-grained matrix of primitive carbonaceous chondrites. Solar-system objects which appear to be partly or wholly made of CCMM are the satellites of Mars, most asteroids, interplanetary dust, and, perhaps, comets, satellites of the outer planets and the rings of Uranus. CCMM constituents probably formed by low-temperature reactions of higher-temperature condensates with the ambient solar composition gas, or in the case of the organic polymer, by reactions of gaseous species catalyzed by solids.

Wilkening, L. L.↗
NASA NTRS1978

Rare-gas-rich separates from carbonaceous chondrites

This paper describes an analysis of carbon-rich separates prepared by demineralization of colloidal fractions after disaggregation of bulk samples of the type C2 meteorites Murray, Murchison, and Cold Bokkeveld, as well as a methanol colloid extracted from acid-resistant residues of the Allende meteorite (type C3V) obtained by dissolution of most of the minerals in HCl and HF acids. The carbonaceous separates, or lAlates (a coined word designating colloids prepared sometimes before and sometimes after acid treatment), are characterized incompletely and with difficulty. A stepwise heating experiment on a Murray lAlate is discussed which revealed bimodal release of all noble gases, with similar patterns for Ar, Kr, and Xe. Chemical reactions are suggested as the likely mechanism for gas release. The results are shown to support the concept of a carbonaceous gas carrier uniformly present in meteorites of various types.

Reynolds, J. H.↗
NASA NTRS1979

Are carbonaceous chondrites primitive or processed - A review

According to the results of the present analysis, carbonaceous chondrites are obviously not pristine samples of proto-solar-system condensates. In terms of chemistry, however, these chondrites may represent the most primitive solar system materials known. It appears that the alterations experienced by carbonaceous chondrites were isochemical, or nearly so, so that their bulk compositions have remained practically unchanged, provided that the analyses are representative of large portions of the meteorites.

Mcsween, H. Y., Jr.↗
NASA NTRS1979

Amino acids in the Yamato carbonaceous chrondrite from Antarctica

Evidence for the presence of amino acids of extraterrestrial origin in the Antarctic Yamato carbonaceous chrondrite is presented. Hydrolyzed and nonhydrolyzed water-extracted amino acid samples from exterior, middle and interior portions of the meteorite were analyzed by an amino acid analyzer and by gas chromatography of N-TFA-isopropyl amino acid derivatives. Nine protein and six nonprotein amino acids were detected in the meteorite at abundances between 34 and less than one nmole/g, with equal amounts in interior and exterior portions. Nearly equal abundances of the D and L enantiomers of alanine, aspartic acid and glutamic acid were found, indicating the abiotic, therefore extraterrestrial, origin of the amino acids. The Antarctic environment and the uniformity of protein amino acid abundances are discussed as evidence against the racemization of terrestrially acquired amino acids, and similarities between Yamato amino acid compositions and the amino acid compositions of the Murchison and Murray type II carbonaceous chrondrites are indicated.

Shimoyama, A.↗
NASA NTRS1979

Noble gas trapping and fractionation during synthesis of carbonaceous matter

An investigation of noble gas entrapment during synthesis of carbonaceous, macromolecular, and kerogen-like substances is presented. High molecular weight organic matter synthesized in aqueous condensation reactions contained little gas, and the composition was consistent with fractionation due to noble gas solubility in water; however, propane soot produced during a modified Miller-Urey experiment in an aritificial gas mixture contained high concentrations of trapped noble gases that displayed strong elemental fractionation from their reservoirs. It is concluded that theses experiemnts show that processes exist for synthesis of carbonaceous carriers that result in high noble gas concentrations and strong elemental fractionation at temperatures well above those required by absorption to achieve similar effects.

Frick, U.↗
NASA NTRS1982

The concentration and isotopic composition of hydrogen, carbon and nitrogen in carbonaceous meteorites

Stepwise pyrolysis was used to extract H2, N2 and C from powdered meteorites and from meteorite residues resulting from partial dissolution in aqueous HF or from reaction with HF-HCl solutions. Concentrations and isotopic compositions were determined for the cases of the carbonaceous chondrites Orgueil, Murray, Murchison, Renazzo and Cold Bokkeveld. Acidification of the meteorites removed the organic sources of H2, so that H2 in the HF-HCl acid residues came mostly from the insoluble organic matter making up 70-80% of the total carbon in carbonaceous meteorites. Good correlation is found between delta-D and the concentration of H2 in the acid residues, but no correlation exists between the delta-D, delta-C-13 and delta-N-15 in them. A model is proposed for both the high delta-D values and the relationship between those values and the H2 concentration.

Robert, F.↗
NASA NTRS1982

Electron microscopy of carbonaceous matter in Allende acid residues

On the basis of characteristic diffuse ring diffraction patterns, much of the carbonaceous matter in a large suite of Allende acid residues has been identified as a variety of turbostratic carbon. Crystallites of this phase contain randomly stacked sp(2) hybridized carbon layers and diffraction patterns resemble those from carbon black and glassy carbon. Carbynes are probably absent, and are certainly restricted to less than 0.5% of these acid residues. The work of Ott et al. (1981) provides a basis for the possibility that turbostratic carbon is a carrier of noble gases, but an additional component - amorphous carbon - may be necessary to explain the high release temperatures of noble gases as well as the glassy character of many of the carbonaceous particles. Carbynes are considered to be questionable as important carriers of noble gases in the Allende acid residues.

Lumpkin, G. R.↗