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At least 757 records · Page 42

The Clumpy Absorber in the High-Mass X-Ray Binary Vela X-1

Bright and eclipsing, the high-mass X-ray binary Vela X-1 offers a unique opportunity to study accretion onto a neutron star from clumpy winds of O/B stars and to disentangle the complex accretion geometry of these systems. In Chandra-HETGS spectroscopy at orbital phase approximately 0.25, when our line of sight towards the source does not pass through the large-scale accretion structure such as the accretion wake, we observe changes in overall spectral shape on timescales of a few kiloseconds. This spectral variability is, at least in part, caused by changes in overall absorption and we show that such strongly variable absorption cannot be caused by unperturbed clumpy winds of O/B stars. We detect line features from high and low ionization species of silicon, magnesium, and neon whose strengths and presence depend on the overall level of absorption. These features imply a co-existence of cool and hot gas phases in the system, which we interpret as a highly variable, structured accretion flow close to the compact object such as has been recently seen in simulations of wind accretion in high-mass X-ray binaries.

Grinberg, V.↗

Evidence for interstellar H2O in the Orion molecular cloud

A search for interstellar gas phase H2O in the infrared spectrum of the BN object in Orion is reported. There is absorption (S/N = 2-4) at the position of the nu3 1(01)-2(02) line of H2O at 3801.42/cm, the strongest expected H2O line. Statistical analysis of the spectrum provides corroborating evidence for other H2O lines. With an assumed H2O excitation temperature of 150 K, N(H2O) of 2.3 x 10 to the 17th/sq cm or less toward the BN object is derived. The H2O column density implies abundance ratios of (H2O)/(CO) = 0.01-0.08 or less and (HDO)/(H2O) = 0.8-3.0 x 10 to the -3rd or more. The gas-to-ice ratio is (H2O gas)/(H2O ice) = 0.06 with an estimated uncertainty of a factor of 5.

Knacke, R. F.↗

Planetesimal Formation in the Outer Solar Nebula

A numerical investigation of the orbital trajectories of individual particles in the turbulent outer solar nebula has been performed. The (spherical) particle consists of an unchanging mm-sized 'dust' core surrounded by an H2O ice mantle; the density of both core and mantle is 0.5 g/cm(exp 3). The simulations include the effects of H2O condensation from the gas phase, H2O sublimation from the particle surface, and collisional growth via particle collisions with a background distribution of small H2O grains. The model nebula is an azimuthally symmetric minimum-mass nebula of solar composition with a vertical (and radial) temperature gradient. Particle evolution follows a pattern. A particle starting out in a cool region grows via condensation and collisional accretion until it is large enough (decimeter- to meter-sized) to decouple somewhat from the turbulence. (This growth occurs on a timescale of several thousand years at 10 AU; at 30 AU, the timescale is approx. 104 years.) The particle then moves rapidly inward toward the sun due to secular gas drag forces, sublimates much of its icy mantle, and slows its inward migration as it gets caught up in the turbulence again (due to its now-smaller size) at the 'sublimation boundary,' where the ambient gas temperature is approx. 150 K. Such a process could, on a short timescale (i.e., a timescale much shorter than the nebular gas lifetime of approx. 106 yr), generate a population of decimeter- to meter-sized bodies which would then collisionally accrete to form planetesimals.

Supulver, K. D.↗

Hot gas and the origin of the nebular continuum in novae

A featureless blue continuum (with constant f(sub nu)) is a defining feature of declining classical novae. The fact that f(sub nu) is constant into the infrared, and the absence of a Balmer jump, suggests that this continuum originates in hot tenous gas. The electron temperature and density of the hot gas phase of classical nova QU Vul 1984 are estimated from ground-based optical and IUE ultraviolet observations. This region has a temperature of 10(exp 5) - 10(exp 6), and a density in the range of 2 x 10(exp 4) to 3 x 10(exp 5)/cu cm. In addition, a colder, denser shell composed of many 'clumps' or condensations is present, and it is responsible for most of the optical-to-ultraviolet emission lines. The hot has, however, may be much more massive and could dominate the energetics of the ejecta. The total returned mass could be as high as 10(exp -4) and 4 x 10(exp -3) solar mass, depending on conditions in the hot gas. The large mass of the shell, in combination with the high metallicity found in this nova, supports the idea that novae may be an important contributor to the chemical enrichment of the interstellar medium.

Saizar, Pedro↗

Laser velocimetry in turbulent flow fields - Particle response

Measurements of the particle response in a decelerating flow and a highly turbulent two-phase flow were obtained. Simultaneous measurements of the particle size and velocity served to quantify the particle response to the prevailing flow field. In the case of a flow incident upon a cylinder, the particle lag for a range of size classes was recorded. Results were also obtained in the flow generated by an atomizer operating on the leeward side of a flat disk bluff body in a coflowing air stream. Measurements of the mean axial, mean radial, and rms velocities and angles of trajectories were obtained for representative particle size classes. The air velocity and turbulence intensity were inferred from the seed particles on the order of one micrometer in diameter. Particles 9 micrometers and larger showed significant differences with respect to the gas phase mean velocity and turbulence intensity even at low velocities. In two-phase flows, reliable measurements of the continuous phase velocity and turbulence parameters requires the simultaneous measurement of particle size as a means for rejecting readings from large particles from the velocity pdf's.

Bachalo, W. D.↗

Near-Limit Flamelet Phenomena in Buoyant Low Stretch Diffusion Flames Beneath a Solid Fuel

A unique near-limit low stretch multidimensional stable flamelet phenomena has been observed for the first time which extends the material flammability limit beyond the one-dimensional low stretch flammability limit to lower burning rates and higher relative heat losses than is possible with uniform flame coverage. During low stretch experiments burning the underside of very large radii (greater than or = 75 cm stretch rate less than or = 3/s) cylindrical cast PMMA samples, multidimensional flamelets were observed, in contrast with a one-dimensional flame that was found to blanket the surface for smaller radii samples ( higher stretch rate). Flamelets were observed by decreasing the stretch rate or by increasing the conductive heat loss from the flame. Flamelets are defined as flames that cover only part of the burning sample at any given time, but persist for many minutes. Flamelet phenomena is viewed as the flame's method of enhancing oxygen flow to the flame, through oxygen transport into the edges of the flamelet. Flamelets form as heat losses (surface radiation and solid-phase conduction) become large relative to the weakened heat release of the low stretch flame. While heat loss rates remain fairly constant, the limiting factor in the heat release of the flame is hypothesized to be the oxygen transport to the flame in this low stretch (low convective) environment. Flamelet extinction is frequently caused by encroachment of an adjacent flamelet. Large-scale whole-body flamelet oscillations at 1.2 - 1.95 Hz are noted prior to extinction of a flamelet. This oscillation is believed to be due a repeated process of excess fuel leakage through the dark channels between the flamelets, fuel premixing with slow incoming oxidizer, and subsequent rapid flame spread and retreat of the flamelet through the premixed layer. The oscillation frequency is driven by gas-phase diffusive time scales.

Olson, S. L.↗

Global Simulation of Atmospheric Mercury Concentrations and Deposition Fluxes

Results from a numerical model of the global emissions, transport, chemistry, and deposition of mercury (Hg) in the atmosphere are presented. Hg (in the form of Hg(O) and Hg(II)) is emitted into the atmosphere from natural and anthropogenic sources (estimated to be 4000 and 2100 Mg/ yr, respectively). It is distributed between gaseous, aqueous and particulate phases. Removal of Hg from the atmosphere occurs via dry deposition and wet deposition, which are calculated by the model to be 3300 and 2800 Mg/ yr, respectively. Deposition on land surfaces accounts for 47% of total global deposition. The simulated Hg ambient surface concentrations and deposition fluxes to the Earth's surface are consistent with available observations. Observed spatial and seasonal trends are reproduced by the model, although larger spatial variations are observed in Hg(O) surface concentrations than are predicted by the model. The calculated atmospheric residence time of Hg is -1.7 years. Chemical transformations between Hg(O) and HG(II) have a strong influence on Hg deposition patterns because HG(II) is removed faster than Hg(O). Oxidation of Hg(O) to HG(II) occurs primarily in the gas phase, whereas HG(II) reduction to Hg(O) occurs solely in the aqueous phase. Our model results indicated that in the absence of the aqueous reactions the atmospheric residence time of Hg is reduced to 1.2 from 1.7 years and the Hg surface concentration is -25% lower because of the absence of the HG(II) reduction pathway. This result suggests that aqueous chemistry is an essential component of the atmospheric cycling of Hg.

Shia, Run-Lie↗

Laboratory Studies of Fischer-Tropsch-Type Reactions and Their Implications for Organics in Asteroids and Comets

We have been studying Fischer-Tropsch type (FTT) reactions as a source for organic materials both in the gas phase of the solar nebula and incorporated into primitive comets and asteroids for almost 10 years, and over this time our concept has evolved greatly from the standard "catalytic" model to a much more robust chemical scenario. Our simulations have been conducted at temperatures that are much higher than we like, primarily for practical reasons such as the timescale of individual reactions, and we are just starting a series of measurements to allow us to measure reaction rates at temperatures from 873K down to as low as 373K. We have preliminary data on the carbon (d13C = -50) & nitrogen (d15N = +9.5) isotopic fractionation at 873K, but not on materials produced at lower temperature. Isotope values are on the VPDB scale for carbon and vs. Air for nitrogen. We have also investigated the noble gas trapping efficiency of the FTT process by adding a small amount of a noble gas mix to our standard synthesis mix. The noble gas ratio is 49:49:1:1::Ne:Ar:Kr:Xe. Xe and Kr are trapped at 873K and are more efficiently trapped at 673K with no isotopic fractionation at either temperature. Ar trapping is detected at 673K, but not at 873K. Ne has not yet been observed in our samples. The solar nebula was an extremely complex system, mixing materials from the innermost regions out to well into the zones where comets formed and thus mixing highly processed nebular materials with grains and coatings formed before the nebula began to collapse. Laboratory studies may provide the means to separate such diverse components based on carbon or nitrogen isotopic fractionation or the quantities of noble gases trapped in grain coatings and their thermal release patterns, among other observables. The ultimate goal of laboratory synthesis of nebular analogs is to provide the means to identifY the conditions under which natural samples were formed and the signatures of subsequent metamorphic events.

Nuth, Joseph↗

Ignition and subsequent flame spread over a thin cellulosic material

Both ignition and flame spread on solid fuels are processes that not only are of considerable scientific interest but that also have important fire safety applications. Both types of processes, ignition and flame spread, are complicated by strong coupling between chemical reactions and transport processes, not only in the gas phase but also in the condensed phase. In most previous studies, ignition and flame spread were studied separately with the result that there has been little understanding of the transition from ignition to flame spread. In fire safety applications this transition is crucial to determine whether a fire will be limited to a localized, temporary burn or will transition into a growth mode with a potential to become a large fire. In order to understand this transition, the transient mechanisms of ignition and subsequent flame spread must be studied. However, there have been no definitive experimental or modeling studies, because of the complexity of the flow motion generated by buoyancy near the heated sample surface. One must solve the full Navier-Stokes equations over an extended region to represent accurately the highly unstable buoyant plume and entrainment of surrounding gas from far away. In order to avoid the complicated nature of the starting plume problem under normal gravity, previous detailed radiative ignition models were assumed to be one-dimensional or were applied at a stagnation point. Thus, these models cannot be extended to include the transition to flame spread. The mismatch between experimental and calculated geometries means that theories cannot be compared directly with experimental results in normal gravity. To overcome the above difficulty, theoretical results obtained without buoyancy can be directly compared with experimental data measured in a microgravity environment. Thus, the objective of this study is to develop a theoretical model for ignition and the transition to flame spread and to make predictions using the thermal and chemical characteristics of a cellulosic material which are measured in normal gravity.

Nakabe, Kazuyoshi↗

X-ray emission from clusters and groups of galaxies

Recent major advances in x-ray imaging and spectroscopy of clusters have allowed the determination of their mass and mass profile out to approximately 1/2 the virial radius. In rich clusters, most of the baryonic mass is in the gas phase, and the ratio of mass in gas/stars varies by a factor of 2-4. The baryonic fractions vary by a factor of approximately 3 from cluster to cluster and almost always exceed 0.09 h50-[3/2] and thus are in fundamental conflict with the assumption of Omega = 1 and the results of big bang nucleosynthesis. The derived Fe abundances are 0.2-0.45 solar, and the abundances of O and Si for low redshift systems are 0.6-1.0 solar. This distribution is consistent with an origin in pure type II supernova. The amount of light and energy produced by these supernovae is very large, indicating their importance in influencing the formation of clusters and galaxies. The lack of evolution of Fe to a redshift of z approximately 0.4 argues for very early enrichment of the cluster gas. Groups show a wide range of abundances, 0.1-0.5 solar. The results of an x-ray survey indicate that the contribution of groups to the mass density of the universe is likely to be larger than 0.1 h50-2. Many of the very poor groups have large x-ray halos and are filled with small galaxies whose velocity dispersion is a good match to the x-ray temperatures.

Evolution, Planetary↗

Extinction of the Stagnation Point Diffusion Flame: Effect of Conductive Heat Loss into Solid Interior

The planned microgravity experiment Growth and Extinction Limit (GEL) is designed to study the material flammability and extinction of thermally thick solid with an emphasis to quantify the effect of conductive heat loss into the solid interior by measuring the in-depth temperature profile. To obtain a more detailed understanding of the extinction phenomena, a previously developed one-dimensional axisymmetric stagnation-point diffusion flame model is expanded to account for the excessive heat loss into the solid beyond the steady burning state. This is important because for thick solids, this is important because the burning period can have a long and slow solid transient with a quasi-steady gas -phase. A non-dimensional excessive conductive heat loss parameter Ψ is defined in the paper and extensive numerical computations have been performed to determine the extinction boundary and the characteristics of near-limit flames. The classical U-shaped flammability boundary in the oxygen vs. stretch rate plot now becomes a series of U-shaped boundaries as a function of Ψ. For a given oxygen ambient, extinction boundary is a function of Ψ. The boundary consists of a blowoff branch and a radiative quenching branch. This is similar to the steady burning flammability boundary (Ψ =0) in the oxygen vs stretch rate plot. Extensive computed data including flame and pyrolysis temperatures, burning rate, flame standoff distance, and reaction rate are presented along the extinction boundaries. In particular, we note that the non-dimensional gas reaction rate is the ratio of diffusion reaction time to the reaction diffusion time, so it has the classical Damhkoler number character. By examining the maximum non-dimensional reaction rates, we observe that along the extinction boundaries, they are approximate constant across the entire range of stretch rates (from quenching to blow-off). These critical values are of the order unity but may vary in different oxygen ambient. The implication will be discussed in the presentation together with the near-limit flame structures.

Chengyao Li↗

Mechanisms of microgravity flame spread over a thin solid fuel - Oxygen and opposed flow effects

Microgravity tests varying oxygen concentration and forced flow velocity have examined the importance of transport processes on flame spread over very thin solid fuels. Flame spread rates, solid phase temperature profiles and flame appearance for these tests are measured. A flame spread map is presented which indicates three distinct regions where different mechanisms control the flame spread process. In the near-quenching region (very low characteristic relative velocities) a new controlling mechanism for flame spread - oxidizer transport-limited chemical reaction - is proposed. In the near-limit, blowoff region, high opposed flow velocities impose residence time limitations on the flame spread process. A critical characteristic relative velocity line between the two near-limit regions defines conditions which result in maximum flammability both in terms of a peak flame spread rate and minimum oxygen concentration for steady burning. In the third region, away from both near-limit regions, the flame spread behavior, which can accurately be described by a thermal theory, is controlled by gas-phase conduction.

Olson, S. L.↗

Solubility of HOBr in Acidic Solution and Implications for Liberation of Halogens Via Aerosol Processing

Halogen species are known to catalytically destroy ozone in several regions of the atmosphere. In addition to direct catalytic losses, bromine compounds can indirectly enhance ozone loss through coupling to other radical families. Hypobromous acid (HOBr) is a key species in the linkage of BrOx to ClOx and HOx. The aqueous- phase coupling reaction HOBr + HCI (right arrow) BrCl + H2O may provide a pathway for chlorine activation on sulfate aerosols at temperatures warmer than those required for polar stratospheric cloud formation. We have measured t h e solubility of HOBr in 45 - 70 wt% sulfuric acid solutions. Over the temperature range 201 - 252 K, HOBr is quite soluble in sulfuric acid, H* = 10(exp 4) - 10(exp 7) mol dm(exp -3) atm(exp -1). The expected inverse dependence of H* on temperature was observed, but only a weak dependence on acidity was found. The solubility of HOBr is comparable to that of HBr, indicating that equilibrium concentrations of HOBr could equal or exceed those of HBr in upper tropospheric and lower stratospheric aerosols. Despite the high solubility of HOBr, aerosol volumes are not large enough to sequester a significant fraction of inorganic bromine from the gas phase. Our measurements of HOBr uptake in aqueous sulfuric acid in the presence of other brominated gases show the evolution of gaseous products including Br2O and Br2.

Iraci, Laura T.↗

An Ensemble Investigation of the Causes for Regional Air-Quality Model Critical Load Exceedances Prediction Variability in European and North American Domains Using Diagnostics From Phase 4 of the Air Quality Model Evaluation International Initiative

We summarize tentative findings from multi air quality model ensembles for the years 2009 and 2010 in Europe (EU), and 2010 and 2016 in North America (NA), under AQMEII-4. The model predictions of sulphur and nitrogen deposition were used to estimate exceedances of critical loads for acidification and eutrophication, to show the extent to which the ensemble members agree in the magnitude and the trend of ecologically meaningful impacts. Model exceedance variability was analyzed using AQMEII-4 diagnostics. Evaluation against concentration and wet deposition observations, coupled with these diagnostics, identified specific process representations as the causes for variability between model predictions and for reduced model performance. All models predicted reductions in ecosystem acidification impacts in North America between the years 2010 and 2016, in accord with SO2 emissions reduction legislation which started in 2010 (SO2 SIP) However, all models in EU and NA domains had net negative biases for wet deposition of sulphur and nitrogen relative to observations. The wet S deposition average mean bias for the NA ensemble was -0.17 eq ha-1 d-1, and for the EU ensemble -1.15 eq ha-1 d-1. The NA daily wet deposition average mean bias for NH4+ was -0.37 eq ha-1d-1; EU -1.19 eq ha-1 d-1. The daily NA wet NO3- deposition average mean bias was -0.24 eq ha-1d-1; EU -0.69 eq ha-1 d-1. The members of the ensemble diverged (factor of 10) in their North American predictions for Ndep and consequently their eutrophication exceedances. The models with the highest eutrophication predictions also predicted the highest levels of gas-phase ammonia dry deposition (standard deviation of ammonia dry deposition flux across ensemble members was larger than the ensemble average). These models also had negative biases of predicted ammonia concentrations; average mean biases of -0.63 (satellite NH3) and -0.85 ppbv (surface NH3) compared to ensemble averages of -0.30 and -0.34 ppbv. Diagnostics showed that these differences resulted from the manner in which bidirectional ammonia fluxes were parameterized within these models. The second largest source of NA eutrophication prediction variability were models with positive biases in particulate ammonium and nitrate concentrations, and higher particle nitrogen deposition levels ( particle ammonium concentration bias +0.35 ug m-3; ensemble bias +0.15 ug m-3). We believe two factors may have led to these latter overestimates: higher levels of fine mode particle nitrate formation compared to other models (due to the use of an inorganic heterogeneous chemistry algorithm which did not take base cation chemistry into account), and updates to particle dry deposition velocities carried out in the absence of concurrent updates to wet scavenging algorithms. The relative importance of dry gas, dry particulate, and wet deposition towards total sulphur and nitrogen deposition totals differed between EU and North American domains, though all models had negative biases in wet deposition as noted above. Parallel and subsequent work suggests that multiphase hydrometeor scavenging may improve model wet deposition performance. An increased research focus is recommended for four model processes: multiphase hydrometeor scavenging, ammonia bidirectional fluxes, base cation chemistry and emissions, and particle dry deposition.

regional air-quality model↗

Adsorption processes in spacecraft environmental control and life support systems

The environmental control and life support system on a spacecraft maintains a safe and comfortable environment in which the crew can live and work by supplying oxygen and water and by removing carbon dioxide, water vapor, and trace contaminants from cabin air. Although open-loop systems have been used successfully in the past for short-duration missions, the economics of current and future long-duration missions in space will make nearly complete recycling of air and water imperative. A variety of operations will be necessary to achieve the goal of nearly complete recycling. These include separation and reduction of carbon dioxide, removal of trace gas-phase contaminants, recovery and purification of humidity condensate, purification and polishing of wastewater streams, and others. Several of these can be performed totally or in part by adsorption processes. These processes are good candidates to perform separations and purifications in space due to their gravity independence, high reliability, relative high energy efficiency, design flexibility, technological maturity, and regenerative nature. For these reasons, adsorption has historically played a key role in life support on U.S. and Russian piloted spacecraft. Among the life support applications that can be achieved through use of adsorption technology are removal of trace contaminants and carbon dioxide from cabin air and recovery of potable water from waste streams. In each of these cases adsorption technology has been selected for use onboard the International Space Station. The requirements, science, and hardware for these applications are discussed. Human space exploration may eventually lead to construction of planetary habitats. These habitats may provide additional opportunities for use of adsorption processes, such as control of greenhouse gas composition, and may have different resources available to them, such as gases present in the planetary atmosphere. Separation and purification processes based on adsorption can be expected to continue to fulfill environmental control and life support needs on future missions.

Review, Tutorial↗

On the Use of Fourier Transform Infrared (FT-IR) Spectroscopy and Synthetic Calibration Spectra to Quantify Gas Concentrations in a Fischer-Tropsch Catalyst System

One possible origin of prebiotic organic material is that these compounds were formed via Fischer-Tropsch-type (FTT) reactions of carbon monoxide and hydrogen on silicate and oxide grains in the warm, inner-solar nebula. To investigate this possibility, an experimental system has been built in which the catalytic efficiency of different grain-analog materials can be tested. During such runs, the gas phase above these grain analogs is sampled using Fourier transform infrared (FT-IR) spectroscopy. To provide quantitative estimates of the concentration of these gases, a technique in which high-resolution spectra of the gases are calculated using the high-resolution transmission molecular absorption (HITRAN) database is used. Next, these spectra are processed via a method that mimics the processes giving rise to the instrumental line shape of the FT-IR spectrometer, including apodization, self-apodization, and broadening due to the finite resolution. The result is a very close match between the measured and computed spectra. This technique was tested using four major gases found in the FTT reactions: carbon monoxide, methane, carbon dioxide, and water. For the ranges typical of the FTT reactions, the carbon monoxide results were found to be accurate to within 5% and the remaining gases accurate to within 10%. These spectra can then be used to generate synthetic calibration data, allowing the rapid computation of the gas concentrations in the FTT experiments.

Infrared Spectroscopy↗

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↗

Identifying Chemical Aerosol Signatures Using Optical Suborbital Observations: How Much Can Optical Properties Tell us about Aerosol Composition?

Improvements in air quality and Earth’s climate predictions require improvements of the aerosol speciation in chemical transport models, using observational constraints. Aerosol speciation (e.g., organic aerosols, black carbon, sulfate, nitrate, ammonium, dust or sea salt) is typically determined using in situ instrumentation. Continuous, routine surface network aerosol composition measurements are not uniformly widespread over the globe. Satellites, on the other hand, can provide a maximum coverage of the horizontal and vertical atmosphere but observe aerosol optical properties (and not aerosol speciation) based on remote sensing instrumentation. Combinations of satellite-derived aerosol optical properties can inform on air mass aerosol types (AMTs e.g., clean marine, dust, polluted continental). However, these AMTs are subjectively defined, might often be misclassified and are hard to relate to the critical parameters that need to be refined in models. In this paper, we derive AMTs that are more directly related to sources and hence to speciation. They are defined, characterized, and derived using simultaneous in situ gas-phase, chemical and optical instruments on the same aircraft during the Study of Emissions and Atmospheric Composition, Clouds, and Climate Coupling by Regional Surveys (SEAC4RS, US, summer of 2013). First, we prescribe well-informed AMTs that display distinct aerosol chemical and optical signatures to act as a training AMT dataset. These in situ observations reduce the errors and ambiguities in the selection of the AMT training dataset. We also investigate the relative skill of various combinations of aerosol optical properties to define AMTs and how much these optical properties can capture dominant aerosol speciation. We find distinct optical signatures for biomass burning (from agricultural or wildfires), biogenic and dust-influence AMTs. Useful aerosol optical properties to characterize these signatures are the extinction angstrom exponent (EAE), the single scattering albedo, the difference of single scattering albedo in two wavelengths, the absorption coefficient, the absorption angstrom exponent (AAE), and the real part of the refractive index (RRI). We find that all four AMTs studied when prescribed using mostly airborne in situ gas measurements, can be successfully extracted from at least three combinations of airborne in situ aerosol optical properties (e.g., EAE, AAE and RRI) over the US during SEAC4RS. However, we find that the optically based classifications for BB from agricultural fires and polluted dust include a large percentage of misclassifications that limit the usefulness of results relating to those classes. The technique and results presented in this study are suitable to develop a representative, robust and diverse source-based AMT database. This database could then be used for widespread retrievals of AMTs using existing and future remote sensing suborbital instruments/networks. Ultimately, it has the potential to provide a much broader observational aerosol data set to evaluate chemical transport and air quality models than is currently available by direct in situ measurements. This study illustrates how essential it is to explore existing airborne datasets to bridge chemical and optical signatures of different AMTs, before the implementation of future spaceborne missions (e.g., the next generation of Earth Observing System (EOS) satellites addressing Aerosol, Cloud, Convection and Precipitation (ACCP) designated observables).

Meloe S F Kacenelenbogen↗