Laboratory Evaluation of Black Carbon Deposition onto Snow and Transport via Snowmelt

Black carbon (BC) is an aerosol material produced by incomplete combustion of fossil fuels and biomass. BC has been shown to be the second most important anthropogenic climate warming agent after carbon dioxide due to its ability to absorb solar radiation, influence cloud behavior, and accelerate snow melt. BC in otherwise clean snow can significantly reduce its reflectivity. In order to learn about the significance of BC contamination in snow, we explored the deposition of BC onto snow and the transport of BC in snow during snowmelt. A Single Particle Soot Photometer (SP2), was used to measure the concentration and size distribution of BC in an airstream drawn through snow to determine the rate at which the snow trapped BC. BC concentration in meltwater was measured to determine if the BC was left in the snow or was removed during melting. SP2 testing showed a significant drop in BC aerosol concentration after contact with the snow. This implies that naturally occurring snow is a highly efficient absorber of BC from the atmosphere. Meltwater samples had a lower BC concentration than the snow, suggesting that the majority of the BC is left behind in snow during partial melting. This accumulation of BC could potentially cause a positive feedback to the rate of snowmelt. Better understanding the behavior of BC in snow will help scientists describe the impact of BC on climate and help policymakers predict the benefits of reducing BC emissions

Evolution of brown carbon in wildfire plumes

Particulate brown carbon (BrC) in the atmosphere absorbs light at subvisible wavelengths and has poorly constrained but potentially large climate forcing impacts. BrC from biomass burning has virtually unknown lifecycle and atmospheric stability. Here, BrC emitted from intense wildfires was measured in plumes transported over 2 days from two main fires, during the 2013 NASA SEAC4RS mission. Concurrent measurements of organic aerosol (OA) and black carbon (BC) mass concentration, BC coating thickness, absorption Ångström exponent, and OA oxidation state reveal that the initial BrC emitted from the fires was largely unstable. Using back trajectories to estimate the transport time indicates that BrC aerosol light absorption decayed in the plumes with a half-life of 9 to 15 h, measured over day and night. Although most BrC was lost within a day, possibly through chemical loss and/or evaporation, the remaining persistent fraction likely determines the background BrC levels most relevant for climate forcing

Global Budget and Radiative Forcing of Black Carbon Aerosol: Constraints from Pole-to-Pole (HIPPO) Observations across the Pacific

We use a global chemical transport model (GEOS-Chem) to interpret aircraft curtain observations of black carbon (BC) aerosol over the Pacific from 85°N to 67°S during the 2009–2011 HIAPER (High-Performance Instrumented Airborne Platform for Environmental Research) Pole-to-Pole Observations (HIPPO) campaigns. Observed concentrations are very low, implying much more efficient scavenging than is usually implemented in models. Our simulation with a global source of $6.5 Tg a^{−1}$ and mean tropospheric lifetime of 4.2 days (versus 6.8 ± 1.8 days for the Aerosol Comparisons between Observations and Models (AeroCom) models) successfully simulates BC concentrations in source regions and continental outflow and captures the principal features of the HIPPO data but is still higher by a factor of 2 (1.48 for column loads) over the Pacific. It underestimates BC absorbing aerosol optical depths (AAODs) from the Aerosol Robotic Network by 32% on a global basis. Only 8.7% of global BC loading in GEOS-Chem is above 5 km, versus 21 ± 11% for the AeroCom models, with important implications for radiative forcing estimates. Our simulation yields a global BC burden of 77 Gg, a global mean BC AAOD of 0.0017, and a top-of-atmosphere direct radiative forcing (TOA DRF) of $0.19 W m^{−2}$, with a range of $0.17–0.31 W m^{−2}$ based on uncertainties in the BC atmospheric distribution. Our TOA DRF is lower than previous estimates $(0.27 \pm 0.06 W m^{−2}$ in AeroCom, $0.65–0.9 W m^{−2}$ in more recent studies). We argue that these previous estimates are biased high because of excessive BC concentrations over the oceans and in the free troposphere.Engineering and Applied Science

Characteristics of brown carbon in Western United States wildfires

Brown carbon (BrC) associated with aerosol particles in western United States wildfires was measured between Jul. and Aug. 2019 onboard the NASA DC-8 research aircraft during the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) study. Two BrC measurement methods are investigated; highly spectrally-resolved light absorption in solvent (water and methanol) extracts of particles collected on filters and in-situ bulk aerosol particle light absorption measured at three wavelengths (405, 532, 664 nm) with a photo acoustic spectrometer (PAS). A light absorption closure analysis for wavelengths between 300 and 700 nm was performed. The combined light absorption of particle pure black carbon material, including enhancements due to internally mixed materials, plus soluble BrC and a Mie-predicted factor for conversion of soluble BrC to aerosol particle BrC, was compared to absorption spectra from a power law fit to the three PAS wavelengths. For the various parameters used, at a wavelength of roughly 400 nm they agreed, at lower wavelengths the individual component-predicted particle light absorption significantly exceeded the PAS and at higher wavelengths the PAS absorption was consistently higher, but more variable. Limitations with extrapolation of PAS data to wavelengths below 405 nm and missing BrC species of low solubility that more strongly absorb at higher wavelengths may account for the differences. Based on measurements closest to fires, the emission ratio of PAS measured BrC at 405 nm relative to carbon monoxide (CO) was on average 0.13 Mm−1 ppbv−1, emission ratios for soluble BrC are also provided. As the smoke moved away from the burning regions the evolution over time of BrC was observed to be highly complex; BrC enhancement, depletion, or constant levels with age were all observed in the first 8 hours after emission in different plumes. Within 8 hours following emissions, 4-nitrocatechol, a well characterized BrC chromophore commonly found in smoke particles, was largely depleted relative to the bulk BrC. In a descending plume where temperature increased by 15 K, 4-nitrocatechol dropped possibly due to temperature-driven evaporation, but bulk BrC remained largely unchanged. Evidence was found for reactions with ozone, or related species, as a pathway for secondary formation of BrC under both low and high oxides of nitrogen (NOx) conditions, while BrC was also observed to be bleached in regions of higher ozone and low NOx, consistent with complex behaviors of BrC observed in laboratory studies. Although the evolution of smoke in the first hours following emission is highly variable, a limited number of measurements of more aged smoke (15 to 30 hours) indicate a net loss of BrC. It is yet to be determined how the near-field BrC evolution in smoke affects the characteristics of smoke over longer time and spatial scales, where its environmental impacts are likely to be greater

Global measurements of brown carbon and estimated direct radiative effects

Brown carbon (BrC) is an organic aerosol material that preferentially absorbs light of shorter wavelengths. Global-scale radiative impacts of BrC have been difficult to assess due to the lack of BrC observational data. To address this, aerosol filters were continuously collected with near pole-to-pole latitudinal coverage over the Pacific and Atlantic basins in three seasons as part of the Atmospheric Tomography Mission. BrC chromophores in filter extracts were measured. We find that globally, BrC was highly spatially heterogeneous, mostly detected in air masses that had been transported from regions of extensive biomass burning. We calculate the average direct radiative effect due to BrC absorption accounted for approximately 7% to 48% of the top of the atmosphere clear-sky instantaneous forcing by all absorbing carbonaceous aerosols in the remote atmosphere, indicating that BrC from biomass burning is an important component of the global radiative balance

Seiberg-Witten Description of the Deconstructed 6D (0,2) Theory

It has recently been suggested that, in a large N limit, a particular four dimensional gauge theory is indistinguishable from the six dimensional CFT with (0,2) supersymmetry compactified on a torus. We give further evidence for this correspondence by studying the Seiberg-Witten curve for the "deconstructed" theory and demonstrating that along the reduced Coulomb branch of moduli space (on the intersection of the Higgs and Coulomb branches) it describes the low energy physics on a stack of M5-branes on a torus, which is the (0,2) theory on a torus as claimed. The M-theory construction helps to clarify the enhancement of supersymmetry in the deconstructed theory at low energies, and demonstrates its stability to radiative and instanton corrections. We demonstrate the role of the theta vacuum in the deconstructed theory. We point out that by varying the theta parameters and gauge couplings in the deconstructed theory, the complex structure of the torus can be chosen arbitrarily, and the torus is not metrically S^1 x S^1 in general.Comment: 13 pages, 2 figure

Ambient aerosol properties in the remote atmosphere from global-scale in-situ measurements

In situ measurements of aerosol microphysical, chemical, and optical properties were made during global-scale flights from 2016–2018 as part of the Atmospheric Tomography Mission (ATom). The NASA DC-8 aircraft flew from ∼ 84∘ N to ∼ 86∘ S latitude over the Pacific, Atlantic, Arctic, and Southern oceans while profiling nearly continuously between altitudes of ∼ 160 m and ∼ 12 km. These global circuits were made once each season. Particle size distributions measured in the aircraft cabin at dry conditions and with an underwing probe at ambient conditions were combined with bulk and single-particle composition observations and measurements of water vapor, pressure, and temperature to estimate aerosol hygroscopicity and hygroscopic growth factors and calculate size distributions at ambient relative humidity. These reconstructed, composition-resolved ambient size distributions were used to estimate intensive and extensive aerosol properties, including single-scatter albedo, the asymmetry parameter, extinction, absorption, Ångström exponents, and aerosol optical depth (AOD) at several wavelengths, as well as cloud condensation nuclei (CCN) concentrations at fixed supersaturations and lognormal fits to four modes. Dry extinction and absorption were compared with direct in situ measurements, and AOD derived from the extinction profiles was compared with remotely sensed AOD measurements from the ground-based Aerosol Robotic Network (AERONET); this comparison showed no substantial bias. The purpose of this work is to describe the methodology by which ambient aerosol properties are estimated from the in situ measurements, provide statistical descriptions of the aerosol characteristics of different remote air mass types, examine the contributions to AOD from different aerosol types in different air masses, and provide an entry point to the ATom aerosol database. The contributions of different aerosol types (dust, sea salt, biomass burning, etc.) to AOD generally align with expectations based on location of the profiles relative to continental sources of aerosols, with sea salt and aerosol water dominating the column extinction in most remote environments and dust and biomass burning (BB) particles contributing substantially to AOD, especially downwind of the African continent. Contributions of dust and BB aerosols to AOD were also significant in the free troposphere over the North Pacific. Comparisons of lognormally fitted size distribution parameters to values in the Optical Properties of Aerosols and Clouds (OPAC) database commonly used in global models show significant differences in the mean diameters and standard deviations for accumulation-mode particles and coarse-mode dust. In contrast, comparisons of lognormal parameters derived from the ATom data with previously published shipborne measurements in the remote marine boundary layer show general agreement. The dataset resulting from this work can be used to improve global-scale representation of climate-relevant aerosol properties in remote air masses through comparison with output from global models and assumptions used in retrievals of aerosol properties from both ground-based and satellite remote sensing

Identifying chemical aerosol signatures using optical suborbital observations: how much can optical properties tell us about aerosol composition

Improvements in air quality and Earth\u27s 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 aerosol composition measurements from ground-based networks 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). 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, an airborne field campaign carried out over the US during the summer of 2013). We find distinct optical signatures for AMTs such as biomass burning (from agricultural or wildfires), biogenic and polluted dust. We find that all four AMTs, studied when prescribed using mostly airborne in situ gas measurements, can be successfully extracted from a few combinations of airborne in situ aerosol optical properties (e.g., extinction Ångström exponent, absorption Ångström exponent and real refractive index). However, we find that the optically based classifications for biomass burning from agricultural fires and polluted dust include a large percentage of misclassifications that limit the usefulness of results related 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 dataset 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 Aerosols, Cloud, Convection and Precipitation (ACCP) designated observables)

In situ measurements of water uptake by black carbon-containing aerosol in wildfire plumes

Water uptake by black carbon (BC)-containing aerosol was quantified in North American wildfire plumes of varying age (1 to ~40 h old) sampled during the SEAC4RS mission (2013). A Humidified Dual SP2 (HD-SP2) is used to optically size BC-containing particles under dry and humid conditions from which we extract the hygroscopicity parameter, κ, of materials internally mixed with BC. Instrumental variability and the uncertainty of the technique are briefly discussed. An ensemble average κ of 0.04 is found for the set of plumes sampled, consistent with previous estimates of bulk aerosol hygroscopicity from biomass burning sources. The temporal evolution of κ in the Yosemite Rim Fire plume is explored to constrain the rate of conversion of BC-containing aerosol from hydrophobic to more hydrophilic modes in these emissions. A BC-specific κ increase of ~0.06 over 40 h is found, fit well with an exponential curve corresponding to a transition from a κ of 0 to a κ of ~0.09 with an e-folding time of 29 h. Although only a few percent of wildfire particles contain BC, a similar κ increase is estimated for bulk aerosol and the measured aerosol composition is used to infer that the observed κ change is driven by a combination of incorporation of ammonium sulfate and oxidation of existing organic materials. Finally, a substantial fraction of wildfire-generated BC-containing aerosol is calculated to be active as cloud condensation nuclei shortly after emission likely indicating efficient wet removal. These results can constrain model treatment of BC from wildfire sources

Fine Ash-Bearing Particles as a Major Aerosol Component in Biomass Burning Smoke

Biomass burning (BB) events are occurring globally with increasing frequency, and their emissions are having more impacts on human health and climate. Large ash particles are recognized as a BB product with major influences on soil and water environments. However, fine-ash particles, which have diameters smaller than several microns and characteristic morphologies and compositions (mainly Ca and Mg carbonates), have not yet been explicitly considered as a major BB aerosol component either in field observations or climate models. This study measured BB aerosol samples using transmission electron microscopy (TEM) and ion chromatography during the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) campaign. We show that significant amounts of fine ash-bearing particles are transported \u3e100 km from their fire sources. Our environmental chamber experiments suggest that they can act as cloud condensation and ice nuclei. We also found considerable amounts of fine ash-bearing particles in the TEM samples collected during previous campaigns (Biomass Burning Observation Project and Megacity Initiative: Local and Global Research Observations). These ash particles are commonly mixed with organic matter and make up ∼8% and 5% of BB smoke by number and mass, respectively, in samples collected during the FIREX-AQ campaign. The measured ash-mass concentrations are approximately five times and six times greater than those of BB black carbon and potassium, respectively, scaling to an estimated global emission of 11.6 Tg yr−1 with a range of 8.8–16.3 Tg yr−1. Better characterization and constraints on these fine ash-bearing particles will improve BB aerosol measurements and strengthen assessments of BB impacts on human health and climate