The largest share in the climate impact of aviation results from contrail cirrus clouds. Here, the dependence of microphysical contrail ice properties and extinction on temperature and humidity is investigated. Contrail measurements were performed at various altitudes during the 2018 ECLIF II/NDMAX campaign with the NASA DC‐8 chasing the DLR A320. Ice number concentrations and contrail extinction coefficients are largest at altitudes near 9.5 km, typical for short‐ and medium‐range air traffic. At higher altitudes near 11.5 km, low ambient water vapor concentrations lead to smaller contrail particle sizes and lower extinction coefficients. In addition, contrails were detected below 8.2 km near the Schmidt‐Appleman contrail formation threshold temperature. Here, only a small fraction (<15%) of the emitted soot particles were activated into ice. Our observations enhance the understanding of contrail formation near the formation threshold and give a glimpse on the altitude dependence of climate‐relevant contrail properties.

Accurate fire emissions inventories are crucial to predict the impacts of wildland fires on air quality and atmospheric composition. Two traditional approaches are widely used to calculate fire emissions: a satellite-based top-down approach and a fuels-based bottom-up approach. However, these methods often considerably disagree on the amount of particulate mass emitted from fires. Previously available observational datasets tended to be sparse, and lacked the statistics needed to resolve these methodological discrepancies. Here, we leverage the extensive and comprehensive airborne in situ and remote sensing measurements of smoke plumes from the recent Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) campaign to statistically assess the skill of the two traditional approaches. We use detailed campaign observations to calculate and compare emission rates at an exceptionally high-resolution using three separate approaches: top-down, bottom-up, and a novel approach based entirely on integrated airborne in situ measurements. We then compute the daily average of these high-resolution estimates and compare with estimates from lower resolution, global top-down and bottom-up inventories. We uncover strong, linear relationships between all of the high-resolution emission rate estimates in aggregate, however no single approach is capable of capturing the emission characteristics of every fire. Global inventory emission rate estimates exhibited weaker correlations with the high-resolution approaches and displayed evidence of systematic bias. The disparity between the low-resolution global inventories and the high-resolution approaches is likely caused by high levels of uncertainty in essential variables used in bottom-up inventories and imperfect assumptions in top-down inventories.

This investigation examines aerosol dynamics during major fine mode aerosol transboundary pollution events in South Korea primarily during the KORUS-AQ campaign from May 1 – June 10, 2016, particularly when cloud fraction was high and/or fog was present to quantify the change in aerosol characteristics due to near-cloud or fog interaction. We analyze the new AERONET Version 3 data that have significant changes to cloud screening algorithms, allowing many more fine-mode observations in the near vicinity of clouds or fog. Case studies for detailed investigation include May 25–26, 2016 when cloud fraction was high over much of the peninsula, associated with a weak frontal passage and advection of pollution from China. These cloud-influenced Chinese transport dates also had the highest aerosol optical depth (AOD), surface PM2.5 concentrations and fine mode particle sizes of the entire campaign. Another likewise cloud/high relative humidity (RH) case is June 9 and 10, 2016 when fog was present over the Yellow Sea that appears to have affected aerosol properties well downwind over the Korean peninsula. In comparison we also investigated aerosol properties on air stagnation days with very low cloud cover and relatively low RH (May 17 & 18, 2016), when local Korean emissions dominated. Aerosol volume size distributions show marked differences between the transport days (with high RH and cloud influences) and the local pollution stagnation days, with total column-integrated particle fine mode volume being an order of magnitude greater on the pollution transport dates. The PM2.5 over central Seoul were significantly greater than for coastal sites on the transboundary transport days yet not on stagnation days, suggesting additional particle formation from gaseous urban emissions in cloud/fog droplets and/or in the high RH humidified aerosol environment. Many days had KORUS-AQ research aircraft flights that provided observations of aerosol absorption, particle chemistry and vertical profiles of extinction. AERONET retrievals and aircraft in situ measurements both showed high single scattering albedo (weak absorption) on the cloudy or cloud influenced days, plus aircraft profile in situ measurements showed large AOD enhancements (versus dried aerosol) at ambient relative humidity (RH) on the pollution transport days, consistent with the significantly larger fine mode particle radii and weak absorption.

The air quality of South Korea was the focus of the NASA/NIER KORean -United States Air Quality (KORUS-AQ) mission of 2016. KORUS-AQ was planned for the period after the spring peak in outbreaks of Asian dust. Regardless of this strategic planning, quantifiable dust was still observed via instrumentation on the NASA DC8 in early May. A novel analysis of supermicron dust and associated supermicron ionic relationships was completed using two size dependent instruments. This supermicron dust provided surface area for heterogeneous chemistry between CaCO3, the gases HNO3, NO2, and SO2, and particulate (NH4)(2)SO4. Uptake of the pollutant gases is greatly enhanced by formation of an aqueous layer on the surface of the dust particles. More water is attracted to particles where uptake of HNO3 has replaced surface CaCO3 with Ca(NO3)(2) generating a dynamic aqueous layer on the dust particle. We propose that particulate (NH4)(2)SO4 coagulated with dust to form (NH4)(2)Ca(SO4)(2) on the particle surface, which rapidly formed CaSO4 and NH4+ in a Ca(NO3)(2) facilitated aqueous layer. A conceptual model is proposed to explain these dust uptake chemical processes. We define the nanoequivalent concentration of supermicron SO42- plus NO3 over the nanoequivalent concentration of supermicron NH4+ plus Ca2+ as the Dust Pollution Index (DPI), used to quantify the extent to which carbonate dust has been modified. DPI values range from 0 (pure dust) to 1 (completely reacted); thus, it represents the conversion of CaCO3 into secondary salts. This mechanism should be used to better predict chemical dynamics in atmospheric models while also helping to further explain the importance of dust and secondary coating on cloud formation processes and dust optical properties. Air masses containing dust that traversed industrial China while mixing with polluted southern air had significantly higher DPI values (average = 0.82, 1s = 0.10) compared to air masses that limited interaction with such pollution (average = 0.51, 1s = 0.13).

We describe results of in situ observations of a 1‐ to 2‐min‐old contrail in the vortex phase generated from soot‐rich exhaust (>1015 emitted soot particles per kilogram of fuel burned). Simultaneous measurements of soot (EIsoot) and apparent ice (AEIice) particle number emission indices show a pronounced anticorrelation in the vertical contrail profile. AEIice decrease by about 75% with increasing distance below the contrail‐producing aircraft, while EIsoot increase by an equivalent relative fraction, therefore strongly suggesting ice particle formation to be soot‐controlled and losses to be caused by sublimation. Quantifying these losses in measurements helps to validate and improve contrail parameterizations used to estimate the climate impact of contrails and contrail cirrus. Our study further demonstrates the challenges in the performance and interpretation of particle measurements in young contrails and lends itself to suggestions for improving contrail data evaluation.

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 (<5 km mean sea level (MSL)) in the storm inflow region were compared to those made in cirrus anvils (altitude > 9 km MSL). Storm mean outflow Ca2+ mass concentrations and total coarse (1 µm < diameter < 5 µm) aerosol volume (Vc) were comparable to mean inflow values as demonstrated by average outflow/inflow ratios greater than 0.5. A positive relationship between Ca2+, Vc, ice water content, and large (diameter > 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.

Abstract Under the Federal Aviation Administration’s (FAA) Aviation Climate Change Research Initiative (ACCRI), non-CO2 climatic impacts of commercial aviation are assessed for current (2006) and for future (2050) baseline and mitigation scenarios. The effects of the non-CO2 aircraft emissions are examined using a number of advanced climate and atmospheric chemistry transport models. Radiative forcing (RF) estimates for individual forcing effects are provided as a range for comparison against those published in the literature. Preliminary results for selected RF components for 2050 scenarios indicate that a 2% increase in fuel efficiency and a decrease in NOx emissions due to advanced aircraft technologies and operational procedures, as well as the introduction of renewable alternative fuels, will significantly decrease future aviation climate impacts. In particular, the use of renewable fuels will further decrease RF associated with sulfate aerosol and black carbon. While this focused ACCRI program effort has yielded significant new knowledge, fundamental uncertainties remain in our understanding of aviation climate impacts. These include several chemical and physical processes associated with NOx–O3–CH4 interactions and the formation of aviation-produced contrails and the effects of aviation soot aerosols on cirrus clouds as well as on deriving a measure of change in temperature from RF for aviation non-CO2 climate impacts—an important metric that informs decision-making.