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Buseck, Peter R.

Publications and source records attributed to Buseck, Peter R..

At least 19 records

Structure and Bonding of Carbon in Clays from CI Carbonaceous Chondrites

Carbonaceous chondrites (CC) contain a diverse suite of C-rich materials. Acid dissolution of these meteorites leaves a C-rich residue with chemical and structural affinities to kerogen. This material has primarily been analyzed in bulk, and much information has been provided regarding functional groups and elemental and isotopic compositions. However, comparatively little work has been done on C in unprocessed meteorites. Studies of CCs suggest a spatial relationship of some C-rich materials with products of aqueous alteration. Recent studies revealed discrete submicronsized, C-rich particles in Tagish Lake and a range of CM2 meteorites. A challenge is to correlate the findings from the bulk acid-residue studies with those of high-spatial resolution-mineralogical and spectroscopic observations of unprocessed meteorites. Hence, the relationship between the C-rich materials in the acid residues and its form and locations in the unprocessed meteorite remains unclear. Here we provide information on the structure and bonding of C associated with clays in CI carbonaceous chondrites. Additional information is included in the original extended abstract.

Garview, Laurence a. J.↗

Polyhedral Serpentine Grains in CM Chondrites

CM chondrites are primitive rocks that experienced aqueous alteration in the early solar system. Their matrices and fine-grained rims (FGRs) sustained the effects of alteration, and the minerals within them hold clues to the aqueous reactions. Sheet silicates are an important product of alteration, and those of the serpentine group are abundant in the CM2 chondrites. Here we expand on our previous efforts to characterize the structure and chemistry of serpentines in CM chondrites and report results on a polyhedral form that is structurally similar to polygonal serpentine. Polygonal serpentine consists of tetrahedral (T) sheets joined to M(2+)-centered octahedral (O) sheets (where (M2+) is primarily Mg(2+) and Fe(2+)), which give rise to a 1:1 (TO) layered structure with a 0.7-nm layer periodicity. The structure is similar to chrysotile in that it consists of concentric lizardite layers wrapped around the fiber axis. However, unlike the rolled-up chrysotile, the tetrahedral sheets of the lizardite layers are periodically inverted and kinked, producing sectors. The relative angles between sectors result in 15- and 30-sided polygons in terrestrial samples.

Zega, Thomas J.↗

Electron Tomography of Nanoparticle Clusters: Implications for Atmospheric Lifetimes and Radiative Forcing of Soot

Nanoparticles are ubiquitous in nature. Their large surface areas and consequent chemical reactivity typically result in their aggregation into clusters. Their chemical and physical properties depend on cluster shapes, which are commonly complex and unknown. This is the first application of electron tomography with a transmission electron microscope to quantitatively determine the three-dimensional (3D) shapes, volumes, and surface areas of nanoparticle clusters. We use soot (black carbon, BC) nanoparticles as an example because it is a major contributor to environmental degradation and global climate change. To the extent that our samples are representative, we find that quantitative measurements of soot surface areas and volumes derived from electron tomograms differ from geometrically derived values by, respectively, almost one and two orders of magnitude. Global sensitivity studies suggest that the global burden and direct radiative forcing of fractal BC are only about 60% of the value if it is assumed that BC has a spherical shape.

vanPoppel, Laura H.↗

Serpentine Nanotubes in CM Chondrites

The CM chondrites are primitive meteorites that formed during the early solar system. Although they retain much of their original physical character, their matrices and fine-grained rims (FGRs) sustained aqueous alteration early in their histories [1- 3]. Serpentine-group minerals are abundant products of such alteration, and information regarding their structures, compositions, and spatial relationships is important for determining the reactions that produced them and the conditions under which they formed. Our recent work on FGRs and matrices of the CM chondrites has revealed new information on the structures and compositions of serpentine-group minerals [4,5] and has provided insights into the evolution of these primitive meteorites. Here we report on serpentine nanotubes from the Mighei and Murchison CM chondrites [6].

Zega, Thomas J.↗

Cosmochemistry and Mineralogy of Primitive Meteorites

We have produced significant research results during the grant period. These have been reported in five papers published in Geochimica et Cosmochimica Acta and Meteoritics and Hanetary Science and several others are in review. We also presented 17 abstracted talks at professional meetings. The citations are given in 2, and abstracts of the papers are provided in $3. The full papers are available on request.

Buseck, Peter R.↗

TEM Study of SAFARI-2000 Aerosols

The aim of our research was to obtain data on the chemical and physical properties of individual aerosol particles from biomass smoke plume s in southern Africa and from air masses in the region that are affec ted by the smoke. We used analytical transmission electron microscopy (ATEM), including energy-dispersive X-ray spectrometry (EDS) and ele ctron energy-loss spectroscopy (EELS), and field-emission electron microscopy (FESEM) to study aerosol particles from several smoke and haz e samples and from a set of cloud samples.

Buseck, Peter R.↗

Characterization of Individual Aerosol Particles Associated with Clouds (CRYSTAL-FACE)

The aim of our research was to obtain data on the chemical and physical properties of individual aerosol particles from near the bottoms and tops of the deep convective systems that lead to the generation of tropical cirrus clouds and to provide insights into the particles that serve as CCN or IN. We used analytical transmission electron microscopy (ATEM), including energy-dispersive X-ray spectrometry (EDS) and electron energy-loss spectroscopy (EELS), and field-emission electron microscopy (FESEM) to compare the compositions, concentrations, size distributions, shapes, surface coatings, and degrees of aggregation of individual particles from cloud bases and the anvils near the tropopause. Aggregates of sea salt and mineral dust, ammonium sulfate, and soot particles are abundant in in-cloud samples. Cirrus samples contain many H2SO4 droplets, but acidic sulfate particles are rare at the cloud bases. H2SO4 probably formed at higher altitudes through oxidation of SO2 in cloud droplets. The relatively high extent of ammoniation in the upper troposphere in-cloud samples appears to have resulted from vertical transport by strong convection. The morphology of H2SO4 droplets indicates that they had been at least yartiy ammoniated at the time of collection. They are internally mixed with organic materials, metal sulfates, and solid particles of various compositions. Ammoniation and internal mixing of result in freezing at higher temperature than in pure H2SO4 aerosols. K- and S-bearing organic particles and Si-Al-rich particles are common throughout. Sea salt and mineral dust were incorporated into the convective systems from the cloud bases and worked as ice nuclei while being vertically transported. The nonsulfate particles originated from the lower troposphere and were transported to the upper troposphere and lower stratosphere.

Buseck, Peter R.↗

Atmospheric Tar Balls: Particles from Biomass and Biofuel Burning

Tar balls are amorphous, carbonaceous spherules that occur in the tropospheric aerosol as a result of biomass and biofuel burning. They form a distinct group of particles with diameters typically between 30 and 500 nm and readily identifiable with electron microscopy. Their lack of a turbostratic microstructure distinguishes them from soot, and their morphology and composition (approximately 90 mol% carbon) renders them distinct from other carbonaceous particles. Tar balls are particularly abundant in slightly aged (minutes to hours old) biomass smoke, indicating that they likely form by gas-to-particle conversion within smoke plumes. The material of tar balls is initially hygroscopic; however, the particles become largely insoluble as a result of free radical polymerization of their organic molecules. Consequently, tar balls are primarily externally mixed with other particle types, and they do not appreciably increase in size during aging. When tar balls coagulate with water-bearing particles, their material may partly dissolve and no longer be recognizable as distinct particles. Tar balls may contain organic compounds that absorb sunlight. They are an important, previously unrecognized type of carbonaceous (organic) atmospheric particle.

Posfai, Mihaly↗

Individual Aerosol Particles from Biomass Burning in Southern Africa: Compositions and Size Distributions of Carbonaceous Particles - 1

Individual aerosol particles in smoke plumes from biomass fires and in regional hazes in southern Africa were studied using analytical transmission electron microscopy (TEM), which allowed detailed characterization of carbonaceous particle types in smoke and determination of changes in particle properties and concentrations during smoke aging. Based on composition, morphology, and microstructure, three distinct types of carbonaceous particles were present in the smoke: organic particles with inorganic (K-salt) inclusions, tar ball particles, and soot. The relative number concentrations of organic particles were largest in young smoke, whereas tar balls were dominant in a slightly aged (1 hour) smoke from a smoldering fire. Flaming fires emitted relatively more soot particles than smoldering fires, but soot was a minor constituent of all studied plumes. Further aging caused the accumulation of sulfate on organic and soot particles, as indicated by the large number of internally mixed organic/sulfate and soot/sulfate particles in the regional haze. Externally mixed ammonium sulfate particles dominated in the boundary layer hazes, whereas organic/sulfate particles were the most abundant type in the upper hazes. Apparently, elevated haze layers were more strongly affected by biomass smoke than those within the boundary layer. Based on size distributions and the observed patterns of internal mixing, we hypothesize that organic and soot particles are the cloud-nucleating constituents of biomass smoke aerosols. Sea-salt particles dominated in the samples taken in stratus clouds over the Atlantic Ocean, off the coast of Namibia, whereas a distinct haze layer above the clouds consisted of aged biomass smoke particles.

Posfai, Mihaly↗

Individual Aerosol Particles from Biomass Burning in Southern Africa Compositions and Aging of Inorganic Particles: Compositions and Aging of Inorganic Particles - 2

Individual aerosol particles collected over southern Africa during the SAFARI 2000 field study were studied using transmission electron microscopy and field-emission scanning electron microscopy. The sizes, shapes, compositions, mixing states, surface coatings, and relative abundances of aerosol particles from biomass burning, in boundary layer hazes, and in the free troposphere were compared, with emphasis on aging and reactions of inorganic smoke particles. Potassium salts and organic particles were the predominant species in the smoke, and most were internally mixed. More KCl particles occur in young smoke, whereas more K2SO4 and KNO3 particles were present in aged smoke. This change indicates that with the aging of the smoke, KCl particles from the fires were converted to K2SO4 and KNO3 through reactions with sulfur- and nitrogen- bearing species from biomass burning as well as other sources. More soot was present in smoke from flaming grass fires than bush and wood fires, probably due to the predominance of flaming combustion in grass fires. The high abundance of organic particles and soluble salts can affect the hygroscopic properties of biomass-burning aerosols and therefore influence their role as cloud condensation nuclei. Particles from biomass burning were important constituents of the regional hazes.

Li, Jia↗

Electron Energy-Loss Spectroscopy (EELS) of Fe-bearing Sheet Silicates in CM Chondrites

The primitive character and hydrated mineralogy of the CM chondrites offers insight into some of the earliest reactions between solids and water. Such reactions profoundly affected the matrices and fine-grained rims (FGRs) [1-4], two of the most significant components of these meteorites [5]. We are using EELS combined with a transmission electron microscope (TEM) to investigate the compositions of Fe-bearing minerals, with emphasis on determining oxidation states and quantification of oxidation-state ratios. Iron is among the most abundant elements in the solar system and it can occur naturally in three oxidation states: Fe0, Fe2+, and Fe3+. Determination of oxidation- state ratios is useful because they can be used to infer the redox conditions under which the minerals formed or were last equilibrated [6, 7]. We are particularly interested in understanding how the oxidation state of Fe was affected by the aqueous reactions of the CM chondrites.

Zega, Thomas J.↗

Cosmochemistry and Mineralogy of Primitive Meteorites

We have produced significant research results during the grant period. These have been reported in five papers published in Geochimica et Cosmochimica Acta and Meteoritics and Planetary Science and several others are in review. We also presented 17 abstracted talks at professional meetings. The citations are given in section 2, and abstracts of the papers are provided in section 3. The full papers are available on request.

Buseck, Peter R.↗

Cobalt-rich, nickel-poor metal (wairauite) in the Ningqiang carbonaceous chondrite

A structurally ordered cubic metal grain containing approximately 39 wt% Co, 61 wt% Fe, and less than 0.6 wt% Ni (approximately Fe3Co2) was found associated with troilite and pentlandite in the matrix of the Ningqiang carbonaceous chondrite. This mineral is similar to terrestrial wairauite. Experimental data in the Fe-Co system indicate that this CsCl-type Co-rich metal is stable below 700 C. Phase relations in the Fe-Co-Ni system show that Co cannot fractionate from Ni above 500 C. The dominant opaque minerals of awaruite, magnetite, and pentlandite in Ningqiang suggest relatively oxidizing conditions.

Xin, Hua↗

Matrices of carbonaceous chondrite meteorites

The morphology, classification, and chemistry of the matrices of carbonaceous chondrite (CC) meteorites is reviewed based on recent research results. The various kinds of CCs are examined in terms of their matrix mineralogy. Alteration processes in CCs are discussed.

Buseck, Peter R.↗

Calcic micas in the Allende meteorite - Evidence for hydration reactions in the early solar nebula

Two calcic micas, clintonite and margarite, have been identified in alteration products in a calcium- and aluminum-rich inclusion (CAI) in the Allende meteorite. Clintonite replaces grossular in alteration veins, and margarite occurs as lamellae in anorthite. Their occurrence suggests that, in addition to undergoing high-temperature alteration by a volatile and iron-rich vapor that produced the grossular and anorthite, some CAIs underwent alteration at moderate temperatures (400 K or less). Petrographic evidence suggests that the calcic micas formed before accretion but after the formation of the layered rim sequences that surround the CAI. These calcic micas provide strong evidence that, contrary to theoretical calculations, some hydration reactions occurred in the early solar nebula.

Keller, Lindsay P.↗

Aqueous alteration in the Kaba CV3 carbonaceous chondrite

Results from TEM and SEM examinations of the Kaba CV3 carbonaceous chondrite are presented, showing that the chondrules and the matrix of Kaba have undergone pervasive low-temperature aqueous alteration, resulting in the formation of Fe-bearing saponite from glass and enstatite in chondrules, and from anhydrous silicates in matrix. The alteration products in Kaba were found to resemble those in other aqueously altered carbonaceous chondrites such as the Mokoia CV3 and in Orgueil CI chondrites and Y-82162 chondrites. However, Kaba lacks the abundant high-Al phyllosilicates, reported for CAIs from Mokoia, and the serpentine and ferrihydrite, found in Orgueil.

Keller, Lindsay P.↗

Phyllosilicates in the Mokoia CV carbonaceous chondrite - Evidence for aqueous alteration in an oxidizing environment

Most CV chondrites contain little if any phyllosilicate mineralization. A petrographic and transmission electron microscopy study of the Mokoia CV carbonaceous chondrite shows that the matrix, chondrules, aggregates, and inclusions all contain considerable amounts of phyllosilicates. The mineralogy and occurrence of phyllosilicates in Mokoia differ from those in the CI and CM chondrites. The differences suggests that aqueous alteration of the three meteorite groups probably occurred under a variety of conditions.

Tomeoka, Kazushige↗