K. L. Thornhill

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 Angstrom 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.

Brown carbon in the continental troposphere

Little is known about the optical significance of light absorbing particulate organic compounds (i.e., brown carbon, BrC), including the importance relative to black carbon (BC) and influence on direct radiative forcing by aerosols. The vertical profile of BrC affects its radiative forcing, yet the distribution of BrC in the free troposphere is largely unknown. In this study, BrC absorption was directly measured in solvent extracts of particulate filters obtained from aircraft sampling over the continental USA. Excluding biomass burning plumes, BrC was observed throughout the tropospheric column (<13 km), and its prevalence increased relative to BC with increasing altitude, indicating contributions from secondary sources. Closure analysis showed good agreement between light absorption from BC plus BrC relative to measured total aerosol absorption. A radiative transfer model indicated that BrC absorption reduced top of atmosphere aerosol forcing by ~20%, suggesting that it is an important component of direct aerosol radiative forcing.

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.

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.

Observational evidence for the convective transport of dust over the central United States

Bulk aerosol composition and aerosol size distributions measured aboard the DC-8 aircraft during the Deep Convective Clouds and Chemistry Experiment mission in May/June 2012 were used to investigate the transport of mineral dust through nine storms encountered over Colorado and Oklahoma. Measurements made at low altitudes (  9 km MSL). Storm mean outflow Ca2+ mass concentrations and total coarse (1 µm   50 µm) ice particle number concentrations was not evident; thus, the influence of ice shatter on these measurements was assumed small. Mean inflow aerosol number concentrations calculated over a diameter range (0.5 µm < diameter < 5.0 µm) relevant for proxy ice nuclei (NPIN) were ~15–300 times higher than ice particle concentrations for all storms. Ratios of predicted interstitial NPIN (calculated as the difference between inflow NPIN and ice particle concentrations) and inflow NPIN were consistent with those calculated for Ca2+ and Vc and indicated that on average less than 10% of the ingested NPIN were activated as ice nuclei during anvil formation. Deep convection may therefore represent an efficient transport mechanism for dust to the upper troposphere where these particles can function as ice nuclei cirrus forming in situ.

Near-global aerosol mapping in the upper troposphere and lowermost stratosphere with data from the CARIBIC project

This study extrapolates aerosol data of the CARIBIC project from 1997 until June 2008 in along trajectories to compose large-scale maps and vertical profiles of submicrometre particle concentrations in the upper troposphere and lowermost stratosphere (UT/LMS). The extrapolation was validated by comparing extrapolated values with CARIBIC data measured near the respective trajectory position and by comparing extrapolated CARIBIC data to measurements by other experiments near the respective trajectory positions. Best agreement between extrapolated and measured data is achieved with particle lifetimes longer than the maximum length of used trajectories. The derived maps reveal regions of strong and frequent new particle formation, namely the Tropical Central and Western Africa with the adjacent Atlantic, South America, the Caribbean and Southeast Asia. These regions of particle formation coincide with those of frequent deep convective clouds. Vertical particle concentration profiles for the troposphere and the stratosphere confirm statistically previous results indicating frequent new particle formation in the tropopause region. There was no statistically significant increase in Aitken mode particle concentration between the first period of CARIBIC operation, 1997–2002, and the second period, 2004–2009. However, a significant increase in concentration occurred within the latter period when considering it in isolation.

Hygrosopicity measurements of aerosol particles in the San Joaquin Valley, CA, Baltimore, MD, and Golden, CO

Aerosol hygroscopicity was investigated using a novel dryer-humidifier system, coupled to a TSI-3563 nephelometer, to obtain the light scattering coefficient (σscat) as a function of relative humidity (RH) in hydration and dehydration modes. The measurements were performed in Porterville, CA (10 January to 6 February 2013), Baltimore, MD (3–30 July 2013), and Golden, CO (12 July to 10 August 2014). Observations in Porterville and Golden were part of the NASA-sponsored Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality project. The measured σscat under varying RH in the three sites was combined with ground aerosol extinction, PM2.5 mass concentrations, and particle composition measurements and compared with airborne observations performed during campaigns. The enhancement factor, f(RH), defined as the ratio of σscat(RH) at a certain RH divided by σscat at a dry value, was used to evaluate the aerosol hygroscopicity. Particles in Porterville showed low average f(RH = 80%) (1.42) which was attributed to the high carbonaceous loading in the region where residential biomass burning and traffic emissions contribute heavily to air pollution. In Baltimore, the high average f(RH = 80%) (2.06) was attributed to the large contribution of SO42− in the region. The lowest water uptake was observed in Golden, with an average f(RH = 80%) = 1.24 where organic carbon dominated the particle loading. Different empirical fits were evaluated using the f(RH) data. The widely used Kasten (gamma) model was found least satisfactory, as it overestimates f(RH) for RH < 75%. A better empirical fit with two power law curve fitting parameters c and k was found to replicate f(RH) accurately from the three sites. The relationship between the organic carbon mass and the species that are affected by RH and f(RH) was also studied and categorized.

Surface Dimming by the 2013 Rim Fire Simulated by a Sectional Aerosol Model

Abstract The Rim Fire of 2013, the third largest area burned by fire recorded in California history, is simulated by a climate model coupled with a size‐resolved aerosol model. Modeled aerosol mass, number, and particle size distribution are within variability of data obtained from multiple‐airborne in situ measurements. Simulations suggest that Rim Fire smoke may block 4–6% of sunlight energy reaching the surface, with a dimming efficiency around 120–150 W m−2 per unit aerosol optical depth in the midvisible at 13:00–15:00 local time. Underestimation of simulated smoke single scattering albedo at midvisible by 0.04 suggests that the model overestimates either the particle size or the absorption due to black carbon. This study shows that exceptional events like the 2013 Rim Fire can be simulated by a climate model with 1° resolution with overall good skill, although that resolution is still not sufficient to resolve the smoke peak near the source region.