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Size distribution and scattering phase function of aerosol particles retrieved from sky brightness measurements

Ground-based measurements of the solar transmission and sky radiance in a horizontal plane through the Sun are taken in several geographical regions and aerosol types: dust in a desert transition zone in Israel, sulfate particles in Eastern and Western Europe, tropical aerosol in Brazil, and mixed continental/maritime aerosol in California. Stratospheric aerosol was introduced after the eruption of Mount Pinatubo in June 1991. Therefore measurements taken before the eruption are used to analyze the properties of tropospheric aerosol; measurements from 1992 are also used to detect the particle size and concentration of stratospheric aerosol. The measurements are used to retrieve the size distribution and the scattering phase function at large scattering angles of the undisturbed aerosol particles. The retrieved properties represent an average on the entire atmospheric column. A comparison between the retrieved phase function for a scattering angle of 120 deg, with phase function predicted from the retrieved size distribution, is used to test the assumption of particle homogeneity and sphericity in radiative transfer models (Mie theory). The effect was found to be small (20% +/- 15%). For the stratospheric aerosol (sulfates), as expected, the phase function was very well predicted using the Mie theory. A model with a power law distribution, based on the spectral dependence of the optical thickness, alpha, cannot estimate accurately the phase function (up to 50% error for lambda = 0.87 microns). Before the Pinatubo eruption the ratio between the volumes of sulfate and coarse particles was very well correlated with alpha. The Pinatubo stratospheric aerosol destroyed this correlation. The aerosol optical properties are compared with analysis of the size, shape, and composition of the individual particles by electron microscopy of in situ samples. The measured volume size distribution before the injection of stratospheric aerosol consistently show two modes, sulfate particles with r(sub m) less than 0.2 microns and coarse paritcles with r(sub m) greater than 0.7 microns. The 'window' in the tropospheric aerosol in this radius range was used to observe a stable stratospheric aerosol in 1992, with r(sub m) approximately 0.5 microns. A combination of such optical thickness and sky measurements can be used to assess the direct forcing and the climatic impact of aerosol. Systematic inversion for the key aerosol types (sulfates, smoke, dust, and maritime aerosol) of the size distribution and phase function can give the relationship between the aerosol physical and optical properties that can be used to compute the radiative forcing. This forcing can be validated in dedicated field experiments.

Kaufman, Y. J.↗

The THS Experiment: Simulating Titans Atmospheric Chemistry at Low Temperature (200K)

In Titan's atmosphere, composed mainly of N2 (95-98%) and CH4 (2-5%), a complex chemistry occurs at low temperature, and leads to the production of heavy organic molecules and subsequently solid aerosols. Here, we used the Titan Haze Simulation (THS) experiment, an experimental setup developed at the NASA Ames COSmIC simulation facility to study Titan's atmospheric chemistry at low temperature. In the THS, the chemistry is simulated by plasma in the stream of a supersonic expansion. With this unique design, the gas is cooled to Titan-like temperature ( approximately 150K) before inducing the chemistry by plasma, and remains at low temperature in the plasma discharge (approximately 200K). Different N2-CH4-based gas mixtures can be injected in the plasma, with or without the addition of heavier precursors present as trace elements on Titan, in order to monitor the evolution of the chemical growth. Both the gas- and solid phase products resulting from the plasma-induced chemistry can be monitored and analyzed using a combination of complementary in situ and ex situ diagnostics. A recent mass spectrometry[1] study of the gas phase has demonstrated that the THS is a unique tool to probe the first and intermediate steps of Titan's atmospheric chemistry at Titan-like temperature. In particular, the mass spectra obtained in a N2-CH4-C2H2-C6H6 mixture are relevant for comparison to Cassini's CAPS-IBS instrument. The results of a complementary study of the solid phase are consistent with the chemical growth evolution observed in the gas phase. Grains and aggregates form in the gas phase and can be jet deposited on various substrates for ex situ analysis. Scanning Electron Microscopy images show that more complex mixtures produce larger aggregates. A mass spectrometry analysis of the solid phase has detected the presence of aminoacetonitrile, a precursor of glycine, in the THS aerosols. X-ray Absorption Near Edge Structure (XANES) measurements also show the presence of imine and nitrile functional groups, showing evidence of nitrogen chemistry. These complementary studies show the high potential of THS to better understand Titan's chemistry and the origin of aerosol formation.

Laboratory↗

In Situ Observation of Carbonaceous Material in the Matrices of CV and CM Carbonaceous Chondrites: Preliminary Results from Energy Filtered Transmission Electron Microscopy

Energy filtered transmission electron microscopy shows that organic matter can be detected in situ in the matrices of carbonaceous chondrites at a spatial resolution of at least 1 nm. In CM chondrites, carbon is often associated with sulfide particles. Additional information is contained in the original extended abstract.

Brearley, A. J.↗

The interaction of small particles and thin films of metals with gases. I - A brief review of the early stages of oxide formation

Existing work on gas-solid reactions making use of thin film technologies is reviewed. The discussion concentrates on two major areas of gas-metal interactions: chemisorption and the early stages of oxidation of metals (characterized by a non-volatile reaction product) and catalytic surface reactions (featuring volatile reaction products). A brief survey of oxide formation on metals is presented. Here it is of importance to distinguish between reactions on continuous thin film substrates and reactions on particulate deposits. Small particle-gas interactions also affect the nucleation, growth and sintering processes of thin films. It is shown that various combinations of UHV and high resolution electron microscopy techniques, which include in situ experimentation, can provide the appropriate tools for studying angstrom particle chemistry.

Poppa, H.↗

Characterization of Cosmic Grain Analogs Formed at Low Temperature from Small Hydrocarbon Precursors in the NASA Ames COSmIC Facility

Here, we present the results of the first solid-phase ex situ analysis of cosmic grain analogs produced at low temperature (<200 K) in the NASA Ames COsmic SImulation Chamber (COSmIC) from small hydrocarbon precursors, methane (CH4) and acetylene (C2H2), seeded in an argon supersonic jet expansion and submitted to a plasma discharge. The plasma-induced chemical reactions, initiated between the precursor molecules and their atomic and molecular fragments, radicals and ions, produce larger molecules and eventually solid particles that are collected in situ under controlled conditions. Scanning electron microscopy (SEM) imaging was used to provide insight on the morphology and growth structure of the grains produced in COSmIC, and to investigate how the precursors used to produce the grains affect these parameters. This SEM study has shown that under identical experimental conditions with fixed physical and chemical parameters (precursor density, temperature, energy, and reaction time), heavier precursors in the initial mixture produce larger grains and in larger quantity, most likely as a result of a more complex chemistry: most of the grains produced in the Ar/CH4 (95:5) gas mixture ranged from 15 to 385 nm in diameter with an average density of 2.1 grains per sq.μm, while the grains produced in the Ar/C2H2 (95:5) gas mixture ranged from 40 to 650 nm with a density of 3.5 grains per sq.μm. Changes in the morphology were also observed, with grains produced from acetylene (C2H2) precursors tending to be more spherical than grains produced from methane (CH4) precursors. This change in morphology could be associated with different stages of growth formation at low temperature from a more "planar" growth at first, followed by coagulation into more spherical particles. This study demonstrates that the COSmIC experimental setup can be used to investigate carbon grain formation from small gas-phase molecular precursors at low temperature (<200 K), i.e., under a temperature regime that is representative of the dust condensation zone and outer region of circumstellar envelopes.

Ella Sciamma-O'Brien↗

Preparation and analysis of particulate metal deposits

Small particles and clusters of palladium were grown by deposition from the vapor phase under ultrahigh vacuum conditions. Amorphous and crystalline support films of Al2O3 and ultrathin amorphous carbon films were used as substrate materials. The growth of the metal deposit was monitored in situ by scanning transmission diffraction of energy-filtered 100 kV electrons and high resolution transmission electron microscopy (TEM) analysis was performed in a separate instrument. It was established by in situ TEM, however, that the transfer of specimens in this case did not unduly affect the size and distribution of deposit particles. It was found that the cleanness, stoichiometry, crystallinity and structural perfection of the support surface play an essential role in determining the crystalline perfection and structure of the particles. The smallest palladium clusters reproducibly prepared contained not more than six atoms but size determinations below 1 nm average particle diameter are very problematic with conventional TEM. Palladium particles grown on carbon supports feature an impurity-stabilized mosaic structure.

Poppa, H.↗

Deep UV Native Fluorescence Imaging of Antarctic Cryptoendolithic Communities

An interdisciplinary team at the Jet Propulsion Laboratory Center for Life Detection has embarked on a project to provide in situ chemical and morphological characterization of Antarctic cryptoendolithic microbial communities. We present here in situ deep ultraviolet (UV) native fluorescence and environmental scanning electron microscopy images transiting 8.5 mm into a sandstone sample from the Antarctic Dry Valleys. The deep ultraviolet imaging system employs 224.3, 248.6, and 325 nm lasers to elicit differential fluorescence and resonance Raman responses from biomolecules and minerals. The 224.3 and 248.6 nm lasers elicit a fluorescence response from the aromatic amino and nucleic acids. Excitation at 325 nm may elicit activity from a variety of biomolecules, but is more likely to elicit mineral fluorescence. The resultant fluorescence images provide in situ chemical and morphological maps of microorganisms and the associated organic matrix. Visible broadband reflectance images provide orientation against the mineral background. Environmental scanning electron micrographs provided detailed morphological information. The technique has made possible the construction of detailed fluorescent maps extending from the surface of an Antarctic sandstone sample to a depth of 8.5 mm. The images detect no evidence of microbial life in the superficial 0.2 mm crustal layer. The black lichen component between 0.3 and 0.5 mm deep absorbs all wavelengths of both laser and broadband illumination. Filamentous deep ultraviolet native fluorescent activity dominates in the white layer between 0.6 mm and 5.0 mm from the surface. These filamentous forms are fungi that continue into the red (iron-rich) region of the sample extending from 5.0 to 8.5 mm. Using differential image subtraction techniques it is possible to identify fungal nuclei. The ultraviolet response is markedly attenuated in this region, apparently from the absorption of ultraviolet light by iron-rich particles coating the filaments. Below 8.5 mm the filamentous morphology of the upper layers gives way to punctate 1-2 micron particles evidencing fluorescent activity following excitation at both deep ultraviolet wavelengths.

Storrie-Lombardi, M. C.↗

Quantitative Characterization of Structural and Mechanical Properties of Boron Nitride Nanotubes in High Temperature Environments

The structural stability and mechanical integrity of boron nitride nanotubes (BNNTs) in high temperature environments are of importance in pursuit of their applications that are involved with extreme thermal processing and/or working conditions, but remain not well understood. In this paper, we perform an extensive study of the impacts of high temperature exposure on the structural and mechanical properties of BNNTs with a full structural size spectrum from nano- to micro- to macro-scale by using a variety of in situ and ex situ material characterization techniques. Atomic force microscopy (AFM) and high resolution transmission electron microscopy measurements reveal that the structures of individual BNNTs can survive at up to 850 °C in air and capture the signs of their structural degradation at 900 °C or above. In situ Raman spectroscopy measurements reveal that the BN bonds in BNNT micro-fibrils undergo substantial softening at elevated temperatures of up to 900 °C. The AFM-based nanomechanical compression measurements demonstrate that the mechanical integrity of individual BNNTs remain intact after being thermally baked at up to 850 °C in air. The studies reveal that BNNTs are structurally and mechanically stable materials in high temperature environments, which enables their usages in high temperature applications.

Chen, Xiaoming↗

Australian Red Dune Sand: A Potential Martian Regolith Analog

To demonstrate the potential scientific and technical merits of in situ microscopy on Mars, we analyzed a possible Martian regolith analog - an acolian red dune sand from the central Australian desert (near Mt. Olga). This sand was chosen for its ubiquitous red coating and the desert environment in which is it found. Grains of this sand were analyzed using a variety of microanalytical techniques. A database of detailed studies of such terrestrial analogs would assist the study of geological and astrobiological specimens in future missions to Mars. Potential instrument concepts for in situ deployment on Mars include local electrode atom probe nanoanalysis (LEAP), vertical scanning white light interferometry (VSWLI), scanning electron microscopies, energy dispersive x-ray microanalysis (EDX), atomic force microscopy (AFM) and X-ray diffraction (XRD). While in situ deployment of these techniques is many years away, ground-based studies using these analytical techniques extend our understanding of the data obtained from instruments to be flown in the near future.

Kuhlman, K. R.↗

In Situ Location and Characterization of Carbon-bearing Phases in Carbonaceous Chondrites: Insights from Yamato 791198, a Weakly-altered CM2 Chondrite

Intense studies of carbonaceous chondrites have provided remarkable insights into the behavior of carbon during the earliest stages of our solar system. This research has demonstrated that carbonaceous meteorites contain a diverse array of organic compounds, whose origins are probably the result of multiple processes that occurred in different locations including interstellar space, the solar nebula and asteroidal parent bodies [1-3]. The most abundant organic carbon component in CI1 and CM2 carbonaceous chondrites is so-called macromolecular carbon, a high molecular weight material that has some affinities to terrestrial kerogen and constitutes approximately 60-70% of the organic material in these meteorites. Although recent studies e.g. [3] have radically improved our understanding of the structural and compositional characteristics of this material, a number of key questions remain to be addressed. In particular, our knowledge of where this macromolecular material is distributed at the fine-scale within carbonaceous chondrites is scant. [4] have shown that organic material is associated with phyllosilicate-rich matrix in CM chondrites, but the detailed mineralogical associations are not well-known. Over the past 2 years, we have begun to address this question by using energy filtered transmission electron microscopy (EFTEM) to locate carbon-bearing materials in situ, focusing specifically on the CM2s. To date we have reported data on the Murchison CM2 chondrite [5], a meteorite that has experienced a modest degree of aqueous alteration. To extend our observations to other CM2 chondrites, we have examined the occurrence of carbon-bearing phases in Yamato 791198. Our recent studies [5] have shown that Y-791198 is among the most weakly-altered CM chondrite currently known and hence is likely to preserve a quite primitive distribution of carbonaceous material. In this study, we present initial observations on the distribution of these materials in one fine-grained rim and compare them with our results from Murchison. Such information may provide important insights into the origins of the carbonaceous material and how it was distributed in nebular and perhaps presolar dust.

Brearley, Adrian J.↗

In situ fatigue loading stage inside scanning electron microscope

A fatigue loading stage inside a scanning electron microscopy (SEM) was developed. The stage allows dynamic and static high-magnification and high-resolution viewing of the fatigue crack initiation and crack propagation processes. The loading stage is controlled by a closed-loop servohydraulic system. Maximum load is 1000 lb (4450 N) with test frequencies ranging up to 30 Hz. The stage accommodates specimens up to 2 inches (50 mm) in length and tolerates substantial specimen translation to view the propagating crack. At room temperature, acceptable working resolution is obtainable for magnifications ranging up to 10,000X. The system is equipped with a high-temperature setup designed for temperatures up to 2000 F (1100 C). The signal can be videotaped for further analysis of the pertinent fatigue damage mechanisms. The design allows for quick and easy interchange and conversion of the SEM from a loading stage configuration to its normal operational configuration and vice versa. Tests are performed entirely in the in-situ mode. In contrast to other designs, the NASA design has greatly extended the life of the loading stage by not exposing the bellows to cyclic loading. The loading stage was used to investigate the fatigue crack growth mechanisms in the (100)-oriented PWA 1480 single-crystal, nickel-based supperalloy. The high-magnification observations revealed the details of the crack growth processes.

Telesman, Jack↗

Growth and characterization of GaAs layers on Si substrates by migration-enhanced molecular beam epitaxy

Migration-enhanced molecular beam epitaxial (MEMBE) growth and characterization of the GaAs layer on Si substrates (GaAs/Si) are reported. The MEMBE growth method is described, and material properties are compared with those of normal two-step MBE-grown or in situ annealed layers. Micrographs of cross-section view transmission electron microscopy and scanning surface electron microscopy of MEMBE-grown GaAs/Si showed dislocation densities of 10 to the 7th/sq cm. AlGaAs/GaAs double heterostructures have been successfully grown on MEMBE GaAs/Si by both metalorganic chemical vapor deposition and liquid phase epitaxy.

Kim, Jae-Hoon↗

Microbiological Methodology in Astrobiology

Searching for life in astromaterials to be delivered from the future missions to extraterrestrial bodies is undoubtedly related to studies of the properties and signatures of living microbial cells and microfossils on Earth. As model terrestrial analogs of Martian polar subsurface layers are often regarded the Antarctic glacier and Earth permafrost habitats where alive microbial cells preserved viability for millennia years due to entering the anabiotic state. For the future findings of viable microorganisms in samples from extraterrestrial objects, it is important to use a combined methodology that includes classical microbiological methods, plating onto nutrient media, direct epifluorescence and electron microscopy examinations, detection of the elemental composition of cells, radiolabeling techniques, PCR and FISH methods. Of great importance is to ensure authenticity of microorganisms (if any in studied samples) and to standardize the protocols used to minimize a risk of external contamination. Although the convincing evidence of extraterrestrial microbial life will may come from the discovery of living cells in astromaterials, biomorphs and microfossils must also be regarded as a target in search of life evidence bearing in mind a scenario that alive microorganisms had not be preserved and underwent mineralization. Under the laboratory conditions, processes that accompanied fossilization of cyanobacteria were reconstructed, and artificially produced cyanobacterial stromatolites resembles by their morphological properties those found in natural Earth habitats. Regarding the vital importance of distinguishing between biogenic and abiogenic signatures and between living and fossil microorganisms in analyzed samples, it is worthwhile to use some previously developed approaches based on electron microscopy examinations and analysis of elemental composition of biomorphs in situ and comparison with the analogous data obtained for laboratory microbial cultures and fossilized microorganisms. This communication will be focused on the analysis of our experience in working with ancient microorganisms and fossils and discussion of some issues that are crucial for development of the program for future finding of extraterrestrial life and its evidence.

Abyzov, S. S.↗

Experimental approaches to well controlled studies of thin-film nucleation and growth.

Particular features and the performance of two experimental systems are described for quantitative studies of thin-film nucleation and growth processes including epitaxial depositions. System I consists of a modified LEED-Auger instrument combined with high-resolution electron microscopy. System II is a UHV electron microscope adapted for in-situ deposition studies. The two systems complement each other ideally, and the combined use of both can result in a comprehensive investigation of vapor deposition processes not obtainable with any other known method.

Poppa, H.↗

Ballistic electron emission microscopy and spectroscopy of Au/GaAs interfaces

This paper presents the first Schottky barrier results for the Au/GaAs(100) interface prepared completely in situ on GaAs grown by molecular-beam epitaxy. The resulting interface displays unexpected properties which can be interpreted in terms of enhanced electrode interdiffusion. In addition, the capability of molecular-beam epitaxy for in situ processing enables the stabilization of this interface against diffusion and allows the formation of a Au/GaAs system with nearly ideal properties. Newly developed ballistic electron spectroscopy and imaging techniques demonstrate that the heterogeneity present at the interface of Au/GaAs(100) fabricated on chemically treated GaAs substrates is removed.

Kaiser, W. J.↗

In situ oxidation studies on /001/ copper-nickel alloy thin films

High-resolution transmission electron microscopy studies are reported of (001)-oriented single crystalline thin films of Cu-3%Ni, Cu-4.6%Ni, and Cu-50%Ni alloy which were prepared by vapor deposition onto (001) NaCl substrates and subsequently annealed at around 1100 K and oxidized at 725 K at low oxygen partial pressure. At all alloy concentrations, Cu2O and NiO nucleated and grew independently without the formation of mixed oxides. The shape and growth rates of Cu2O nuclei were similar to rates found earlier. For low-nickel alloy concentrations, the NiO nuclei were larger and the number density of NiO was less than that of Cu-50%Ni films for which the shape and growth rates of NiO were identical to those for pure nickel films. Phenomena involving a reduced induction period, surface precipitation, and through-thickness growth are also described. The results are consistent with previously established oxidation mechanisms for pure copper and pure nickel films.

Heinemann, K.↗

Physical and Optical/Radiative Properties of Arctic Aerosols: Potential Effects on Arctic Climate

We have determined the abundance of light-scattering sulfuric acid (H2SO4/H2O) and light-absorbing black carbon aerosol (BCA) in Spring 1992 in the Arctic atmosphere by airborne in situ sampling with impactors, and measured particle sizes and morphologies by scanning electron microscopy. The mass of BCA in the Arctic troposphere is one percent of the total aerosol, reduced to one part in 104 in the stratosphere. A Mie algorithm permits the calculation of the optical properties of the various aerosol components, and an algorithm developed by Ackerman and Toon and modified to serve our needs lets us calculate the optical effects of the black carbon aerosol that is mixed internally with the sulfuric acid aerosol. It follows that the effect of internally-mixed BCA on the aerosol scattering and absorption properties depends on its location within the droplet. BCA concentrated near the droplet surface has a greater effect on absorption of solar radiation than does the same amount of BCA located near its center. Single scatter albedos of the combined system are omega(sub 0)=1.0 in the post-Pinatubo Arctic stratosphere, and as low as 0.94 in the troposphere. The aerosol has the potential to regionally warm the Arctic earth-atmosphere system, because of the high surface albedo of the snow-covered Arctic.

Pueschel, R. F.↗