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NASA NTRS2019

Quantification of CO2 and CH4 emissions over Sacramento, California, based on divergence theorem using aircraft measurements

Emission estimates of carbon dioxide (CO2) and methane (CH4) and the meteorological factors affecting them are investigated over Sacramento, California, using an aircraft equipped with a cavity ring-down greenhouse gas sensor as part of the Alpha Jet Atmospheric eXperiment (AJAX) project. To better constrain the emission fluxes, we designed flights in a cylindrical pattern and computed the emission fluxes from two flights using a kriging method and Gauss’s divergence theorem. Differences in wind treatment and assumptions about background concentrations affect the emission estimates by a factor of 1.5 to 7. The uncertainty is also impacted by meteorological conditions and distance from the emission sources. The vertical layer averaging affects the flux estimate, but the choice of raw wind or mass-balanced wind is more important than the thickness of the vertical averaging for massbalanced wind for both urban and local scales. The importance of vertical mass transfer for flux estimates is examined, and the difference in the total emission estimate with and without vertical mass transfer is found to be small, especially at the local scale. The total flux estimates accounting for the entire circumference are larger than those based solely on measurements made in the downwind region. This indicates that a closed-shape flight profile can better contain total emissions relative to a one-sided curtain flight because most cities have more than one point source and wind direction can change with time and altitude. To reduce the uncertainty of the emission estimate, it is important that the sampling strategy account not only for known source locations but also possible unidentified sources around the city. Our results highlight that aircraft-based measurements using a closed-shape flight pattern are an efficient and useful strategy for identifying emission sources and estimating local- and city-scale greenhouse gas emission fluxes.

Ju-Mee Ryoo↗
NASA NTRS2020

The California Baseline Ozone Transport Study (CABOTS)

Ozone is one of the six “criteria” pollutants identified by the U.S. Clean Air Act Amendment of 1970 as particularly harmful to human health. Concentrations have decreased markedly across the United States over the past 50 years in response to regulatory efforts, but continuing research on its deleterious effects have spurred further reductions in the legal threshold. The South Coast and San Joaquin Valley Air Basins of California remain the only two “extreme” ozone nonattainment areas in the United States. Further reductions of ozone in the West are complicated by significant background concentrations whose relative importance increases as domestic anthropogenic contributions decline and the national standards continue to be lowered. These background concentrations derive largely from uncontrollable sources including stratospheric intrusions, wildfires, and intercontinental transport. Taken together the exogenous sources complicate regulatory strategies and necessitate a much more precise understanding of the timing and magnitude of their contributions to regional air pollution. The California Baseline Ozone Transport Study was a field campaign coordinated across Northern and Central California during spring and summer 2016 aimed at observing daily variations in the ozone columns crossing the North American coastline, as well as the modification of the ozone layering downwind across the mountainous topography of California to better understand the impacts of background ozone on surface air quality in complex terrain.

Ian C. Faloona↗
NASA NTRS2020

Influence of Cloud, Fog, and High Relative Humidity during Pollution Transport Events in South Korea: Aerosol Properties and PM2.5 Variability

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 addi-tional 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 mea-surements 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.

Aerosol↗
NASA NTRSDate not supplied

Particle Shape, Size, and Composition from Satellites

The MISR Research Aerosol (RA) retrieval algorithm produces (A) aerosol amount (optical depth – AOD), (B) an aerosol size constraint (Angstrom Exponent) (C) fraction of non-spherical particles, and (D) particle light-absorption (SSA). Near the Camp fire source region the particles tend to be large (low Angstrom Exponent) and non-spherical particles, probably from burning in the town of Paradise. Aerosols are smaller and more spherical downwind, probably as the plume mixes with smoke from burning forest.

aerosol↗
NASA NTRSDate not supplied

Remotely-Sensed Aerosol Optical Properties Retrieved from a High Spectral Resolution Lidar (HSRL) During the FIREX-AQ Field Campaign

The NASA Langley Research Center’s High Spectral Resolution Lidar with Differential Absorption Lidar (HSRL-DIAL) instrument was flown on the NASA DC-8 aircraft during the Fire Influence on Region to Global Environments and Air Quality (FIREX-AQ; https://www.esrl.noaa.gov/csl/projects/firex-aq/) field campaign. The airborne HSRL-DIAL system retrieves aerosol backscatter and depolarization at 3 wavelengths (355, 532, and 1064 nm), aerosol extinction at 532 nm, and ozone concentration (differential at 290 and 300 nm). Additionally, the HSRL-DIAL system incorporates both a zenith and nadir telescope allowing for retrievals from in-smoke sampling to be integrated through the plume. During the first portion of the FIREX-AQ campaign, the DC8 aircraft sampled more than ten large-scale fires with varying fuels, combustion stages, and metrological conditions, with some fires being sampled multiple times across separate days. This presentation focuses on the retrievals of aerosol backscatter (at 532 and 1064 nm), aerosol depolarization (at 532 nm and 1064 nm), aerosol optical thickness (at 532 nm), lidar ratio, and color ratio to examine the changes in these properties in the smoke plume as they are advected downwind.

Taylor Shingler↗
NASA NTRSDate not supplied

In Situ Measurements of Ammonia In Plumes Emitted From Wildfires And Agricultural Fires in the US

Emissions of trace gases and particles from fires have a major impact on climate, visibility, air quality, and public health. Biomass burning emissions include reactive nitrogen gases, among which ammonia (NH3) plays a prominent role. NH3 is a short-lived gas that acts as precursor for secondary inorganic aerosols. This process is still poorly constrained in downwind fire plumes. In summer 2019, NASA and NOAA carried out the joint airborne FIREX-AQ (Fire Influence on Regional to global Environments and Air Quality) mission over the continental US to sample plumes from wildfires and agricultural fires. On board the NASA DC-8, we used a modified PTR-ToF-MS instrument for measuring NH3 in situ and at high time resolution. Over the course of the mission, we collected a large set of NH3 data in plumes emitted from fires differing in fuel type and burning stage. Herein, we will present the measured NH3 emissions ratios and factors, compare them with the literature, and investigate the dependence of NH3 emissions on fuel type and burning conditions.

ammonia↗
NASA NTRS2020

The Impacts of Fossil Fuel Emission Uncertainties and Accounting for 3-D Chemical CO2 Production on Inverse Natural Carbon Flux Estimates from Satellite and In Situ Data

Atmospheric carbon dioxide (CO2) inversions for estimating natural carbon fluxes typically do not allow for adjustment of fossil fuel CO2 emissions, despite significant uncertainties in emission inventories and inadequacies in the specification of international bunker emissions in inversions. Also, most inversions place CO2 release from fossil fuel combustion and biospheric sources entirely at the surface. However, a non-negligible portion of the emissions actually occurs in the form of reduced carbon species, which are eventually oxidized to CO2 downwind. Omission of this ‘chemical pump’ can result in a significant redistribution of the inferred total carbon fluxes among regions. We assess the impacts of different prescriptions of fossil fuel emissions and accounting for the chemical pump on flux estimation, with a novel aspect of conducting both satellite CO2 observation-based and surface in situ-based inversions. We apply 3-D carbon monoxide (CO) loss rates archived from a state-of-the-art GEOS chemistry and climate model simulation in a forward transport model run to simulate the distribution of CO2 originating from oxidation of carbon species. We also subtract amounts from the prior surface CO2 fluxes that are actually emitted in the form of fossil and biospheric CO, methane, and nonmethane volatile organic compounds (VOCs). We find that the posterior large-scale fluxes are generally insensitive to the finer-scale spatial differences between the ODIAC and CDIAC fossil fuel CO2 gridded datasets and assumptions about international bunker emissions. However, accounting for 3-D chemical CO2 production and the surface correction shifts the global carbon sink, e.g., from land to ocean and from the tropics to the north, with a magnitude and even direction that depend on assumptions about the surface correction. A GOSAT satellite-based inversion is more sensitive to the chemical pump than one using in situ observations, exhibiting substantial flux impacts of 0.28, 0.53, and -0.47 Pg C yr(exp -1) over tropical land, global land, and oceans, due to differences in the horizontal and vertical sampling of the wo observation types. Overall, the biases from neglecting the chemical pump appear to be minor relative to the flux estimate uncertainties and the differences between the in situ and GOSAT inversions, but their relative importance will grow in the future as observational coverage further increases and satellite retrieval biases decrease.

James S Wang↗
NASA NTRS2020

The Evolution of Icelandic Volcano Emissions, as Observed From Space in the Era of NASA's Earth Observing System (EOS)

Volcanoes are natural phenomena that have global environmental impacts. Satellite remote sensing can help classify volcanic eruptions and track the dispersion of emissions. We assess multiple volcanic eruptions in Iceland (Eyjafjallajökull 2010, Grímsvötn 2011 and Holuhraun 2014-2015), using space-borne observations to infer information about the geological dynamics of each volcano and the properties and evolution of plume particles. We derive qualitative constraints on plume particle size, shape and light-absorption characteristics from Multi-angle Imaging SpectroRadiometer (MISR) space-borne imagery. With the MISR Research Algorithm (RA), we distinguish sulfate/water-dominated volcanic plumes from Holuhraun and ash-dominated plumes from Eyjafjallajökull and Grímsvötn, and even identify subtler changes in ash particle size and light-absorption within plumes. Additionally, plume heights are retrieved geometrically from MISR. These are combined with surface thermal anomalies from the MODerate resolution Imaging Spectroradiometer (MODIS) and SO2 concentrations derived from the Ozone Monitoring Instrument (OMI) to synthesize eruption remote-sensing chronologies. Signals related to differences in particle properties are identified and linked to evolving magma composition at Eyjafjallajökull. The results illustrate the potential to distinguish qualitative differences in eruptive magma composition based on particle light absorption and plume profile from remote-sensing. For the sulfate-rich Holuhraun plumes, the influence of aerosol hygroscopic growth during transport is inferred from such data. Three processes appear to dominate plume evolution in Iceland: downwind aerosol formation; particle hydration; and particle deposition. This work demonstrates enhanced MISR capabilities, and more generally, remote-sensing analysis that can be applied globally, especially where suborbital volcano observations are limited or entirely absent.

remote sensting↗
NASA NTRS2020

High Ice Water Content in Tropical Cyclones during NASA/FAA Radar Flight Campaigns with Comparison to Numerical Simulations

Results from two recent flight campaigns into High Ice Water Content (HIWC) are summarized. HIWC was detected with airborne radar and measured via microphysical probes mounted on NASA’s DC-8. Results from the campaign demonstrate detectability of HIWC using airborne radar. In the cases examined, tropical storms are more proficient at producing large areas of HIWC than hurricanes. Three-dimensional, numerical simulations of tropical cyclones encountered during the campaign are also presented and are compared to measurements in order to understand conditions associated with HIWC. Within Hurricane Lane (2018), the highest ice water contents were found in regenerating thermal plumes located in the eye wall and in feeder bands. Within Tropical Storm Danny (2015), large areas of ice water content greater than 1 g m-3 were fed by broad-areas of convection occurring downwind from the center of circulation.

Aviation hazards↗
NASA NTRSDate not supplied

Understanding Land-Atmosphere Interactions in Agricultural Areas through Improved Modeling and Monitoring of Irrigation

Irrigation increases soil moisture and evapotranspiration, often leading to cooler and more humid conditions over and downwind of irrigated areas. These changes can affect the evolution of the planetary boundary layer and ultimately influence the development of clouds and precipitation. It is for this reason that there has been a push to include irrigation processes in weather and climate models. This presentation will discuss recent efforts to model irrigation impacts in NASA’s land surface and coupled models, via both improved parameterizations and the incorporation of satellite data from platforms such as SMAP, MODIS, and ECOSTRESS. This work underscores the need to consider human water management impacts when analyzing or predicting components of the water and energy cycles, and the critical roles that NASA observations and models play in this assessment.

Patricia Lawston Parker↗
NASA NTRS2020

Inconsistencies in Sulphur Dioxide Emissions from the Canadian Oil Sands and Potential Implications

Satellite-derived and reported sulfur dioxide (SO2) emissions from the Canadian oil sands are shown to have been consistent up to 2013. Post-2013, these sources of emissions data diverged, with reported emissions dropping by a factor of two, while satellite-derived emissions for the region remained relatively constant, with the discrepancy (satellite-derived emissions minus reported emissions) peaking at 50 kt(SO2) yr−1 around 2016. The 2013–2014 period corresponds to when new flue-gas desulfurization units came on-line. Previous work has established a high level of consistency between at-stack SO2 emissions observations and satellite estimates, and surface monitoring network SO2 concentrations over the same multi-year period show similar trends as the satellite data, with a slight increase in concentrations post-2013. No clear explanation for this discrepancy currently exists. The implications of the discrepancy towards estimated total sulfur deposition to downwind ecosystems were estimated relative to 2013 emissions levels, with the satellite-derived values leaving the area of regional critical load exceedances of aquatic ecosystems largely unchanged from 2013 values, 335 000 km2, and reported values potentially decreasing this area to 185,000 km2.

Sulphur dioxide (SO2) emissions↗
NASA NTRS2020

Assessment of Natural and Anthropogenic Aerosol Air Pollution In the Middle East Using MERRA-2, CAMS Data Assimilation Products, and High-Resolution WRF-Chem Model Simulations

Modern-Era Retrospective analysis for Research and Applications v.2 (MERRA-2), Copernicus Atmosphere Monitoring Service Operational Analysis (CAMS-OA), and a high-resolution regional Weather Research and Forecasting model coupled with chemistry (WRF-Chem) were used to evaluate natural and anthropogenic particulate matter (PM) air pollution in the Middle East (ME) during 2015–2016. Two Moderate Resolution Imaging Spectrometer (MODIS) retrievals – combined product Deep Blue and Deep Target (MODIS-DB&DT) and Multi-Angle Implementation of Atmospheric Correction (MAIAC) – and Aerosol Robotic Network (AERONET) aerosol optical depth (AOD) observations as well as in situ PM measurements for 2016 were used for validation of the WRF-Chem output and both assimilation products. MERRA-2 and CAMS-OA assimilate AOD observations. WRF-Chem is a free-running model, but dust emission in WRF-Chem is tuned to fit AOD and aerosol volume size distributions obtained from AERONET. MERRA-2 was used to construct WRF-Chem initial and boundary conditions both for meteorology and chemical and aerosol species. SO2 emissions in WRF-Chem are based on the novel OMI-HTAP SO2 emission dataset. The correlation with the AERONET AOD is highest for MERRA-2 (0.72–0.91), MAIAC (0.63–0.96), and CAMSOA (0.65–0.87), followed by MODIS-DB&DT (0.56–0.84) and WRF-Chem (0.43–0.85). However, CAMS-OA has a relatively high positive mean bias with respect to AERONET AOD. The spatial distributions of seasonally averaged AODs from WRF-Chem, assimilation products, and MAIAC are well correlated with MODIS-DB&DT AOD product. MAIAC has the highest correlation (R = 0.8), followed by MERRA-2 (R = 0.66), CAMS-OA (R = 0.65), and WRF-Chem (R = 0.61). WRF-Chem, MERRA-2, and MAIAC underestimate and CAMS-OA overestimates MODIS-DB&DT AOD. The simulated and observed PM concentrations might differ by a factor of 2 because it is more challenging for the model and the assimilation products to reproduce PM concentration measured within the city. Although aerosol fields in WRF-Chem and assimilation products are entirely consistent, WRF-Chem is preferable for analysis of regional air quality over the ME due to its higher spatial resolution and better SO2 emissions. The WRF-Chem’s PM background concentrations exceed the World Health Organization (WHO) guidelines over the entire ME. Mineral dust is the major contributor to PM (≈ 75%–95%) compared to other aerosol types. Near and downwind from the SO2 emission sources, non-dust aerosols (primarily sulfate) contribute up to 30% to PM(sub 2.5). The contribution of sea salt to PM in coastal regions can reach 5%. The contributions of organic matter, black carbon and organic carbon to PM over the Middle East are insignificant. In the major cities over the Arabian Peninsula, the 90th percentile of PM(sub 10) and PM(sub 2.5) (particles with diameters less than 10 and 2.5 μm, respectively) daily mean surface concentrations exceed the corresponding Kingdom of Saudi Arabia air quality limits. The contribution of the non-dust component to PM(sub 2.5) is < 25%, which limits the emission control effect on air quality. The mitigation of the dust effect on air quality requires the development of environment-based approaches like growing tree belts around the cities and enhancing in-city vegetation cover. The WRF-Chem configuration presented in this study could be a prototype of a future air quality forecast system that warns the population against air pollution hazards.

Alexander Ukhov↗
NASA NTRS2020

Influence of Synoptic-Dynamic Meteorology on the Long-Range Transport of Indochina Biomass Burning Aerosols

Impacts of long-range transported biomass burning aerosols from northern Indochina on regional air quality, atmospheric visibility, and climate effects have been discussed extensively in the literature over the past decade. However, the mechanism between aerosol transport and the low-level jet (LLJ) in synoptic meteorology dynamics (e.g., the frontal system) is still not fully understood. In this study, we present results of aerosol-LLJ interaction based on the National Aeronautics and Space Administration/Modern Era Retrospective-analysis for Research and Application version 2 (NASA/MERRA-2) dataset simultaneous to field campaigns in spring 2013–2015 over Southeast Asia. For linking the atmospheric circulation to aerosol transport, a general meteorological condition favorable for aerosol transport is demonstrated. Biomass burning aerosol accumulation over the source region (i.e., northern Indochina) coincided with weak westerly system over the northern South China Sea, and as the synoptic weather system evolved, the aerosols were transported to downwind regions (i.e., Taiwan and West Pacific) by a cold front and LLJ dynamics. The MERRA-2 reanalysis data show the postcold front accompanied a LLJ stream at approximately 700 hPa (3 km) and accelerated the haze plume transport eastward with a life cycle of approximately 3–5 days, an event that reoccurred multiple times from March to April. Our results indicate that coexistence of LLJ and a South China Sea anticyclone at 700 hPa, which primarily could drive the mechanism behind these transport events. Furthermore, more observational data from Southeast Asia would greatly benefit studies of aerosol-meteorology interactions in the region.

Hsiang-Yu Huang↗
NASA NTRS2020

VolKilau: Volcano Rapid Response Balloon Campaign During the 2018 Kilauea Eruption

After nearly 35 years of stable activity, the Kilauea volcanic system in Hawaiʽi, went through sudden changes in May 2018 with the emergence of 20 volcanic fissures along the Lower Eastern Rift Zone(LERZ) destroying 700 homes in Leilani Estates and forcing more than 2000 people to evacuate. Volcanic emissions lasted for several months between June and September 2018 leading to low visibility and poor air quality in Hawaiʽi and across the Western Pacific. The NASA-funded VolKilau mission was rapidly mounted and conducted between 11-18 June 2018 to: i) Profile volcanic emissions with SO2and aerosol measurements, ii) Validate satellite observations and iii) Be prepared for the next large volcanic eruption. Through a series of balloon-borne measurements with tethered and free released launches, we measured SO2 concentration, aerosol concentration and optical properties 60 to 80km downwind from the volcanic fissures using gas sensors, optical particle counters, backscatter sondes, and an aerosol impactor. While most of measurements made during the Kilauea eruption were ground-based, the VolKilau mission represented a unique opportunity to characterize plume properties, constrain emission profiles, study early chemistry involving the conversion of SO2 into sulfuric acid and understand the influence of water clouds in the removal of SO2. Our team continues to be better prepared for deploying in the event of a major volcanic eruption

J-P Vernier↗
NASA NTRS2020

Estimating Wildfire-Generated Ozone Over North America Using Ozonesonde Profiles and a Differential Back Trajectory Technique

An objective method, employing HYSPLIT back-trajectories and Moderate Resolution Imaging Spectroradiometer (MODIS) fire observations, is developed to estimate ozone enhancement in air transported from regions of active forest fires at 18 ozone sounding sites located across North America. The Differential Back Trajectory (DBT) method compares mean differences between ozone concentrations associated with fire-affected and fire-unaffected parcels. It is applied to more than 1100 ozonesonde profiles collected from these sites during the summer months June to August, 2006, 2008, 2010 and 2011. Layers of high ozone associated with low humidity were first removed from the ozonesonde profiles to minimize the potential effects of stratospheric intrusions on the calculations. No significant influence on average ozone levels by North American fires was found for stations located at Arctic latitudes. The ozone enhancement for stations nearer large fires, such as Trinidad Head and Bratt’s Lake, was up to 324.8% of the TTOC (Total Tropospheric Ozone Column). Fire ozone accounted for up to 8.3% of TTOC at downwind sites such as Yarmouth, Sable Island, Narragansett, and Walsingham. The results are consistent with other studies that have reported an increase in ozone production with the age of the smoke plume.

Moderate Resolution Imaging Spectroradiometer (MOD↗
NASA NTRS2021

Evaluation of Novel NASA MODIS and VIIRS Aerosol Products and Assessment of Smoke Height Boundary Layer Ratio During Extreme Smoke Events in the Western U.S.

We analyze new aerosol products from NASA satellite retrievals over the western U.S. during August 2013, with special attention to locally generated wildfire smoke and downwind plume structures. Aerosol optical depth (AOD) at 550 nm from MODIS (Terra and Aqua Collections 6 and 6.1) and VIIRS Deep Blue (DB) and MODIS (Terra and Aqua) Multi‐Angle Implementation of Atmospheric Correction (MAIAC) retrievals are evaluated against ground‐based AErosol RObotic NETwork (AERONET) observations. We find a significant improvement in correlation with AERONET and other metrics in the latest DB AOD (MODIS C6.1 r^2=0.75, VIIRS r^2=0.79) compared to MODIS C6 (r2=0.62). In general, MAIAC (r^2=0.84) and DB (MODIS C6.1 and VIIRS) present similar statistical evaluation metrics for the western U.S. and are useful tools to characterize aerosol loading associated with wildfire smoke. We also evaluate three novel NASA MODIS plume injection height (PIH) products, one from MAIAC and two from the Aerosol Single scattering albedo and layer Height Estimation (ASHE) (MODIS and VIIRS) algorithm. Both Terra and Aqua MAIAC PIHs statistically agree with ground‐based and satellite lidar observations near the fire source, as do ASHE, although the latter is sensitive to assumptions about aerosol absorption properties. We introduce a first‐order approximation Smoke Height Boundary Layer Ratio (SHBLR) to qualitatively distinguish between aerosol pollution within the planetary boundary layer and the free troposphere. We summarize the scope, limitations, and suggestions for scientific applications of surface level aerosol concentrations specific to wildfire emissions and smoke plumes using these novel NASA MODIS and VIIRS aerosol products.

Plume injection height↗
NASA NTRS2021

Ozone Production and Precursor Emission from Wildfires in Africa

Tropospheric ozone (O3) negatively impacts human health and is also a greenhouse gas. It is formed photochemically by reactions of nitrogen oxides (NOx) and volatile organic compounds (VOCs), of which wildfires are an important source. This study presents data from research flights sampling wildfires in West and Central African savannah regions, both close to the fires and after the emissions had been transported several days over the tropical North Atlantic Ocean. Emission factors (EFs) in g kg-1 for NOx (as NO), six VOCs and formaldehyde were calculated from enhancement to mole fractions in data taken close to the fires. For NOx, the emission factor was calculated as 2.05±0.43 g kg-1 for Senegal and 1.20±0.28 g kg-1 for Uganda, both higher than the average value of 1.13±0.6 g kg-1 for previous studies of African savannah regions. For most VOCs (except acetylene), EFs in Uganda were lower by factors of 20-50% compared to Senegal, with almost all the values below those in the literature. O3 enhancement in the fire plumes was investigated by examining the ΔO3/ΔCO enhancement ratio, with values ranging from 0.07 - 0.14 close to the fires up to 0.25 for measurements taken over the Atlantic Ocean up to 200 hours downwind. In addition, measurements of O3 and its precursors were compared to the output of a global chemistry transport model (GEOS-CF) for the flights over the Atlantic Ocean. Normalised mean bias (NMB) comparison between the measured and modelled data was good outside of the fire plumes, with CO showing a model under-prediction of 4.6% and O3 a slight over-prediction of 0.7% (both within the standard deviation of the data). For NOx the agreement was poorer, with an under-prediction of 9.9% across all flights. Inside the fire plumes the agreement between modelled and measured values is worse, with the model being biased significantly lower for all three species. In total across all flights, there was an under-prediction of 29.4%, 16.5% and 37.5% for CO, O3 and NOx respectively. Finally, the measured ΔO3/ΔCO enhancement ratios were compared those in the model for the equivalent flight data, with the model showing a lower value of 0.17±0.03 compared to an observed value of 0.29±0.05. The results detailed here show that the O3 burden to the North Atlantic Ocean from African wildfires may be underestimated and that further study is required to better study the O3 precursor emissions and chemistry.

James D Lee↗
NASA NTRS2021

Airborne and Ground-Based Measurements of Aerosol Optical Depth of Freshly Emitted Anthropogenic Plumes in the Athabasca Oil Sands Region

In this work we report the airborne aerosol optical depth (AOD) from measurements within freshly emitted anthropogenic plumes arising from mining and processing operations in the Athabasca Oil Sands Region (AOSR) in the context of ground-based AERONET climatological daily averaged AODs at Fort McMurray (Alberta, Canada). During two flights on 9 and 18 June 2018, the NASA airborne 4STAR (Spectrometers for Sky-Scanning, Sun-Tracking Atmospheric Research) Sun photometer registered high fine-mode (FM, <1 µm) in-plume AODs of up to 0.4 and 0.9, respectively, in the vicinity of the plume source (<20 km). Particle composition shows that the plumes were associated with elevated concentrations of sulfates and ammonium. These high AODs significantly exceed climatological averages for June and were not captured by the nearby AERONET instrument (mean daily AODs of 0.10±0.01 and 0.07±0.02, maximum AOD of 0.12) due possibly to horizontal inhomogeneity of the plumes, plume dilution and winds which in certain cases were carrying the plume away from the ground-based instrument. The average 4STAR out-of-plume (background) AODs deviated only marginally from AERONET daily averaged values. While 4STAR AOD peaks were generally well correlated in time with peaks in the in situ-measured particle concentrations, we show that differences in particle size are the dominant factor in determining the 4STAR-derived AOD. During the two flights of 24 June and 5 July 2018 when plumes likely travelled distances of 60 km or more, the average 4STAR FM AOD increased by 0.01–0.02 over ∼50 km of downwind particle evolution, which was supported by the increases in layer AODs calculated from the in situ extinction measurements. Based on these observations as well as the increases in organic mass, we attribute the observed AOD increase, at least in part, to secondary organic aerosol formation. The in-plume and out-of-plume AODs for this second pair of flights, in contrast to clear differences in in situ optical and other measurements, were practically indistinguishable and compared favourably to AERONET within 0.01–0.02 AOD. This means that AERONET was generally successful in capturing the background AODs, but missed some of the spatially constrained high-AOD plumes with sources as close as 30–50 km, which is important to note since the AERONET measurements are generally thought to be representative of the regional AOD loading. The fact that industrial plumes can be associated with significantly higher AODs in the vicinity of the emission sources than previously reported from AERONET can potentially have an effect on estimating the AOSR radiative impact.

AERONET↗