A. J. Beyersdorf

Microbiome of the upper troposphere: Species composition and prevalence, effects of tropical storms, and atmospheric implications

The composition and prevalence of microorganisms in the middle-to-upper troposphere (8–15 km altitude) and their role in aerosol-cloud-precipitation interactions represent important, unresolved questions for biological and atmospheric science. In particular, airborne microorganisms above the oceans remain essentially uncharacterized, as most work to date is restricted to samples taken near the Earth’s surface. Here we report on the microbiome of low- and high-altitude air masses sampled onboard the National Aeronautics and Space Administration DC-8 platform during the 2010 Genesis and Rapid Intensification Processes campaign in the Caribbean Sea. The samples were collected in cloudy and cloud-free air masses before, during, and after two major tropical hurricanes, Earl and Karl. Quantitative PCR and microscopy revealed that viable bacterial cells represented on average around 20% of the total particles in the 0.25- to 1-μm diameter range and were at least an order of magnitude more abundant than fungal cells, suggesting that bacteria represent an important and underestimated fraction of micrometer-sized atmospheric aerosols. The samples from the two hurricanes were characterized by significantly different bacterial communities, revealing that hurricanes aerosolize a large amount of new cells. Nonetheless, 17 bacterial taxa, including taxa that are known to use C1–C4 carbon compounds present in the atmosphere, were found in all samples, indicating that these organisms possess traits that allow survival in the troposphere. The findings presented here suggest that the microbiome is a dynamic and underappreciated aspect of the upper troposphere with potentially important impacts on the hydrological cycle, clouds, and climate.

Atmospheric chemistry of an Antarctic volcanic plume

[1] We report measurements of the atmospheric plume emitted by Erebus volcano, Antarctica, renowned for its persistent lava lake. The observations were made in December 2005 both at source, with an infrared spectrometer sited on the crater rim, and up to 56 km downwind, using a Twin Otter aircraft; with the two different measurement platforms, plume ages were sampled ranging from <1 min to as long as 9 h. Three species (CO, carbonyl sulfide (OCS), and SO2) were measured from both air and ground. While CO and OCS were conserved in the plume, consistent with their long atmospheric lifetimes, the downwind measurements indicate a SO2/CO ratio about 20% of that observed at the crater rim, suggesting rapid chemical conversion of SO2. The aircraft measurements also identify volcanogenic H2SO4, HNO3 and, recognized for the first time in a volcanic plume, HO2NO2. We did not find NOx in the downwind plume despite previous detection of NO2 above the crater. This suggests that near-source NOx was quickly oxidized to HNO3 and HO2NO2, and probably NO3� (aq), possibly in tandem with the conversion of SO2 to sulfate. These fast processes may have been facilitated by ‘‘cloud processing’’ in the dense plume immediately downwind from the crater. A further striking observation was O3 depletion of up to � 35% in parts of the downwind plume. This is likely to be due to the presence of reactive halogens (BrO and ClO) formedthrough heterogeneous processes in the young plume. Our analysis adds to the growing evidence for the tropospheric reactivity of volcanic plumes and shows that Erebus volcano has a significant impact on Antarctic atmospheric chemistry, at least locally in the Southern Ross Sea area.

Mapping the Operation of the Miniature Combustion Aerosol Standard (Mini-CAST) Soot Generator

The Jing Ltd. miniature combustion aerosol standard (Mini-CAST) soot generator is a portable, commercially available burner that is widely used for laboratory measurements of soot processes. While many studies have used the Mini-CAST to generate soot with known size, concentration, and organic carbon fraction under a single or few conditions, there has been no systematic study of the burner operation over a wide range of operating conditions. Here, we present a comprehensive characterization of the microphysical, chemical, morphological, and hygroscopic properties of Mini-CAST soot over the full range of oxidation air and mixing N2 flow rates. Very fuel-rich and fuel-lean flame conditions are found to produce organic-dominated soot with mode diameters of 10–60 nm, and the highest particle number concentrations are produced under fuel-rich conditions. The lowest organic fraction and largest diameter soot (70–130 nm) occur under slightly fuel-lean conditions. Moving from fuel-rich to fuel-lean conditions also increases the O:C ratio of the soot coatings from ∼0.05 to ∼0.25, which causes a small fraction of the particles to act as cloud condensation nuclei near the Kelvin limit (κ ∼ 0–10−3). Comparison of these property ranges to those reported in the literature for aircraft and diesel engine soots indicates that the Mini-CAST soot is similar to real-world primary soot particles, which lends itself to a variety of process-based soot studies. The trends in soot properties uncovered here will guide selection of burner operating conditions to achieve optimum soot properties that are most relevant to such studies. Copyright 2014 American Association for Aerosol Research

Agricultural fires in the southeastern U.S. during SEAC4RS: Emissions of trace gases and particles and evolution of ozone, reactive nitrogen, and organic aerosol

Emissions from 15 agricultural fires in the southeastern U.S. were measured from the NASA DC-8 research aircraft during the summer 2013 Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC^4RS) campaign. This study reports a detailed set of emission factors (EFs) for 25 trace gases and 6 fine particle species. The chemical evolution of the primary emissions in seven plumes was examined in detail for ~1.2 h. A Lagrangian plume cross-section model was used to simulate the evolution of ozone (O_3), reactive nitrogen species, and organic aerosol (OA). Observed EFs are generally consistent with previous measurements of crop residue burning, but the fires studied here emitted high amounts of SO_2 and fine particles, especially primary OA and chloride. Filter-based measurements of aerosol light absorption implied that brown carbon (BrC) was ubiquitous in the plumes. In aged plumes, rapid production of O_3, peroxyacetyl nitrate (PAN), and nitrate was observed with ΔO_3/ΔCO, ΔPAN/ΔNO_y, and Δnitrate/ΔNO_y reaching ~0.1, ~0.3, and ~0.3. For five selected cases, the model reasonably simulated O_3 formation but underestimated PAN formation. No significant evolution of OA mass or BrC absorption was observed. However, a consistent increase in oxygen-to-carbon (O/C) ratios of OA indicated that OA oxidation in the agricultural fire plumes was much faster than in urban and forest fire plumes. Finally, total annual SO_2, NO_x, and CO emissions from agricultural fires in Arkansas, Louisiana, Mississippi, and Missouri were estimated (within a factor of ~2) to be equivalent to ~2% SO_2 from coal combustion and ~1% NO_x and ~9% CO from mobile sources.

Biofuel blending reduces particle emissions from aircraft engines at cruise conditions

Aviation-related aerosol emissions contribute to the formation of contrail cirrus clouds that can alter upper tropospheric radiation and water budgets, and therefore climate. The magnitude of air-traffic-related aerosol–cloud interactions and the ways in which these interactions might change in the future remain uncertain. Modelling studies of the present and future effects of aviation on climate require detailed information about the number of aerosol particles emitted per kilogram of fuel burned and the microphysical properties of those aerosols that are relevant for cloud formation. However, previous observational data at cruise altitudes are sparse for engines burning conventional fuels, and no data have previously been reported for biofuel use in-flight. Here we report observations from research aircraft that sampled the exhaust of engines onboard a NASA DC‐8 aircraft as they burned conventional Jet A fuel and a 50:50 (by volume) blend of Jet A fuel and a biofuel derived from Camelina oil. We show that, compared to using conventional fuels, biofuel blending reduces particle number and mass emissions immediately behind the aircraft by 50 to 70 per cent. Our observations quantify the impact of biofuel blending on aerosol emissions at cruise conditions and provide key microphysical parameters, which will be useful to assess the potential of biofuel use in aviation as a viable strategy to mitigate climate change.

Atmospheric chemistry results from the ANTCI 2005 Antarctic plateau airborne study

One of the major goals of the 2005 Antarctic Tropospheric Chemistry Investigation (ANTCI) was to bridge the information gap between current knowledge of South Pole (SP) chemistry and that of the plateau. The former has been extensively studied, but its geographical position on the edge of the plateau makes extrapolating these findings across the plateau problematic. The airborne observations reported here demonstrate that, as at SP, elevated levels of nitric oxide (NO) are a common summertime feature of the plateau. As in earlier studies, planetary boundary layer (PBL) variations were a contributing factor leading to NO fluctuations. Thus, extensive use was made of in situ measurements and models to characterize PBL depths along each flight path and over broader areas of the plateau. Consistent with earlier SP studies that revealed photolysis of nitrate in surface snow as the source of NO x , large vertical gradients in NO were observed over most plateau areas sampled. Similar gradients were also found for the nitrogen species HNO3 and HO2NO2 and for O3. Thus, a common meteorological-chemical feature found was shallow PBLs associated with nitrogen species concentrations that exceeded free tropospheric levels. Collectively, these new results greatly extend the geographical sampling footprint defined by earlier SP studies. In particular, they suggest that previous assessments of the plateau as simply a chemical depository need updating. Although the evidence supporting this position comes in many forms, the fact that net photochemical production of ozone occurs during summer months over extensive areas of the plateau is pivotal.

Airborne characterization of subsaturated aerosol hygroscopicity and dry refractive index from the surface to 6.5 km during the SEAC4RS campaign

In situ aerosol particle measurements were conducted during 21 NASA DC-8 flights in the Studies of Emissions and Atmospheric Composition, Clouds, and Climate Coupling by Regional Surveys field campaign over the United States, Canada, Pacific Ocean, and Gulf of Mexico. For the first time, this study reports rapid, size-resolved hygroscopic growth and real refractive index (RI at 532 nm) data between the surface and upper troposphere in a variety of air masses including wildfires, agricultural fires, biogenic, marine, and urban outflow. The Differential Aerosol Sizing and Hygroscopicity Spectrometer Probe (DASH-SP) quantified size-resolved diameter growth factors (GF = Dp,wet/Dp,dry) that are used to infer the hygroscopicity parameter κ. Thermokinetic simulations were conducted to estimate the impact of partial particle volatilization within the DASH-SP across a range of sampling conditions. Analyses of GF and RI data as a function of air mass origin, dry size, and altitude are reported, in addition to κ values for the inorganic and organic fractions of aerosol. Average RI values are found to be fairly constant (1.52–1.54) for all air mass categories. An algorithm is used to compare size-resolved DASH-SP GF with bulk scattering f(RH = 80%) data obtained from a pair of nephelometers, and the results show that the two can only be reconciled if GF is assumed to decrease with increasing dry size above 400 nm (i.e., beyond the upper bound of DASH-SP measurements). Individual case studies illustrate variations of hygroscopicity as a function of dry size, environmental conditions, altitude, and composition.

Determination of the emissions from an aircraft auxiliary power unit (APU) during the Alternative Aviation Fuel Experiment (AAFEX)

The emissions from a Garrett-AiResearch (now Honeywell) Model GTCP85–98CK auxiliary power unit (APU) were determined as part of the National Aeronautics and Space Administrations (NASAs) Alternative Aviation Fuel Experiment (AAFEX) using both JP-8 and a coal-derived Fischer Tropsch fuel (FT-2). Measurements were conducted by multiple research organizations for sulfur dioxide (SO2), total hydrocarbons (THC), carbon monoxide (CO), carbon dioxide (CO2), nitrogen oxides (NOx), speciated gas-phase emissions, particulate matter (PM) mass and number, black carbon, and speciated PM. In addition, particle size distribution (PSD), number-based geometric mean particle diameter (GMD), and smoke number were also determined from the data collected. The results of the research showed PM mass emission indices (EIs) in the range of 20 to 700 mg/kg fuel and PM number EIs ranging from 0.5 × 1015 to 5 × 1015 particles/kg fuel depending on engine load and fuel type. In addition, significant reductions in both the SO2 and PM EIs were observed for the use of the FT fuel. These reductions were on the order of ∼90% for SO2 and particle mass EIs and ∼60% for the particle number EI, with similar decreases observed for black carbon. Also, the size of the particles generated by JP-8 combustion are noticeably larger than those emitted by the APU burning the FT fuel with the geometric mean diameters ranging from 20 to 50 nm depending on engine load and fuel type. Finally, both particle-bound sulfate and organics were reduced during FT-2 combustion. The PM sulfate was reduced by nearly 100% due to lack of sulfur in the fuel, with the PM organics reduced by a factor of ∼5 as compared with JP-8. Implications: The results of this research show that APUs can be, depending on the level of fuel usage, an important source of air pollutant emissions at major airports in urban areas. Substantial decreases in emissions can also be achieved through the use of Fischer Tropsch (FT) fuel. Based on these results, the use of FT fuel could be a viable future control strategy for both gas- and particle-phase air pollutants. Supplemental Data: Supplemental data is available for this article. Go to the publishers online edition of the Journal of the Air & Waste Management Association for information on the test participants, description of the APU, fuel composition, sampling probes and instrumentation, test matrix, benzene to formaldehyde ratios, and speciated emissions by particle size.

Gaseous and Particulate Emissions Results of the NASA Alternative Aviation Fuel Experiment (AAFEX)

The Aircraft Alternative Fuels Emissions experiment (AAFEX) was conducted at National Aeronautic and Space Administration (NASA) Dryden Flight Research Center (DFRC) Aircraft Operations Facility (DAOF) in Palmdale, California, during January and February 2009. The purpose was to systematically investigate the effect of alternative fuels on both gas-phase and particle emissions from a CFM56-2C1 engine on NASA’s DC-8 aircraft parked on the ground as functions of engine power, fuel composition, and exhaust plume age. Emissions parameters were measured at 6 engine power settings, ranging from idle to maximum thrust, in samples collected at 1, 30, and 145 meters (m) downstream of the exhaust plane as the aircraft burned three pure fuels and two fuel blends. The fuels included JP-8, two fuels produced using the Fischer-Tropsch process and 50/50 blends by volume of the F-T fuels with JP-8. The 1 m sampling rakes contained multiple gas and particle inlet probes and could also be traversed in order to measure the spatial variation of emissions across the engine exhaust plane. The #2 inboard engine on the left side always burned JP-8 while the #3 inboard right side engine was fueled with the various fuels and fuel blends. In addition, emissions from the Auxiliary Power Unit (APU) were also evaluated with both JP-8 and one pure F-T fuel. Both gaseous and particulate emissions are presented. Results show that the synthetic fuels reduced pollutant emissions while having relatively little effect on engine operation or performance.Copyright

Intercomparison of aerosol single‐scattering albedo derived from AERONET surface radiometers and LARGE in situ aircraft profiles during the 2011 DRAGON‐MD and DISCOVER‐AQ experiments

Single-scattering albedo (SSA) retrievals obtained with CIMEL Sun-sky radiometers from the Aerosol Robotic Network (AERONET) aerosol monitoring network were used to make comparisons with simultaneous in situ sampling from aircraft profiles carried out by the NASA Langley Aerosol Group Experiment (LARGE) team in the summer of 2011 during the coincident DRAGON-MD (Distributed Regional Aerosol Gridded Observational Network-Maryland) and DISCOVER-AQ (Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality) experiments. The single-scattering albedos (interpolated to 550 nm) derived from AERONET measurements for aerosol optical depth (AOD) at 440 nm ≥ 0.4 (mean SSA: 0.979) were on average 0.011 lower than the values derived from the LARGE profile measurements (mean SSA: 0.99). The maximum difference observed was 0.023 with all the observed differences within the combined uncertainty for the stated SSA accuracy (0.03 for AERONET; 0.02 for LARGE). Single-scattering albedo averages were also analyzed for lower aerosol loading conditions (AOD ≥ 0.2) and a dependence on aerosol optical depth was noted with significantly lower single-scattering albedos observed for lower AOD in both AERONET and LARGE data sets. Various explanations for the SSA trend were explored based on other retrieval products including volume median radius and imaginary refractive index as well as column water vapor measurements. Additionally, these SSA trends with AOD were evaluated for one of the DRAGON-MD study sites, Goddard Space Flight Center, and two other Mid-Atlantic AERONET sites over the long-term record dating to 1999.