Search

This paper presents airborne measurements of multiple atmospheric trace constituents including greenhouse gases (such as CO2, CH4, O3) and biomass burning tracers (such as CO, CH3CN) downwind of an exceptionally large wildfire. In summer 2013, the Rim wildfire, ignited just west of the Yosemite National Park, California, and burned over 250,000 acres of the forest during the 2-month period (17 August to 24 October) before it was extinguished. The Rim wildfire plume was intercepted by flights carried out by the NASA Ames Alpha Jet Atmospheric eXperiment (AJAX) on 29 August and the NASA DC-8, as part of SEAC4RS (Studies of Emissions, Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys), on 26 and 27 August during its intense, primary burning period. AJAX revisited the wildfire on 10 September when the conditions were increasingly smoldering, with slower growth. The more extensive payload of the DC-8 helped to bridge key measurements that were not available as part of AJAX (e. g. CO). Data analyses are presented in terms of emission ratios (ER), emission factors (EF) and combustion efficiency and are compared with previous wildfire studies. ERs were 8.0 ppb CH4/(ppm CO2) on 26 August, 6.5 ppb CH4 (ppm CO2)1 on 29 August and 18.3 ppb CH4 (ppm CO2)1 on 10 September 2013. The increase in CH4 ER from 6.5 to 8.0 ppb CH4/(ppm CO2) during the primary burning period to 18.3 ppb CH4/(ppm CO2) during the fire's slower growth period likely indicates enhanced CH4 emissions from increased smoldering combustion relative to flaming combustion. Given the magnitude of the Rim wildfire, the impacts it had on regional air quality and the limited sampling of wildfire emissions in the western United States to date, this study provides a valuable dataset to support forestry and regional air quality management, including observations of ERs of a wide number of species from the Rim wildfire.

Aerosol and CCN number concentrations, and aerosol size distributions in and around the Korean Peninsula were measured onboard the NASA DC-8 research aircraft during the KORUS-AQ campaign in May and June of 2016. The average and standard deviation values of total aerosol number concentrations (diameter > 10 nm, NCN10) in the boundary layer (below 1 km altitude) over Seoul, the Korean Peninsula, the Yellow Sea, the East Sea, and the South Sea were 12,318±7808, 10,721±8636, 7599±8583, 5759±6051, and 4186±4777 cm−3, respectively. Corresponding values for CCN number concentration at 0.6% supersaturation (NCCN06) were 3358±1916, 3613±2242, 3422±1707, 2313±1039, and 1819±1328 cm−3, respectively. NCN10 was highly variable according to region and period. In contrast, NCCN06 was relatively invariant regardless of region and period. With the PMF analysis on the aircraft measured aerosol size distribution and NCCN06 data, it was found that aerosol size distributions were composed of several distinct modes and they were different depending on regions. The aerosol hygroscopicity parameter κ was also estimated based on the PMF analysis results. The estimated κ values over Seoul, the Korean Peninsula, and the Yellow Sea were 0.11, 0.11, and 0.36, respectively. Lastly, the CCN closure experiments indicated that CCN concentration could be successfully estimated with the aerosol size distribution data and the estimated κ information from the aircraft measurements. Overall, it was demonstrated that PMF analysis technique could be applied to extract valuable information from limited aircraft measurement dataset.

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 DC-8 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)2SO4. 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)2SO4 coagulated with dust to form (NH4)2Ca(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, 1σ = 0.10) compared to air masses that limited interaction with such pollution (average = 0.51, 1σ = 0.13).

Satellite data of atmospheric pollutants are becoming more widely used in the decision-making and environmental management activities of public, private sector and non-profit organizations. They are employed for estimating emissions, tracking pollutant plumes, supporting air quality forecasting activities, providing evidence for “exceptional event” declarations, monitoring regional long-term trends, and evaluating air quality model output. However, many air quality managers are not taking full advantage of the data for these applications nor has the full potential of satellite data for air quality applications been realized. A key barrier is the inherent difficulties associated with accessing, processing, and properly interpreting observational data. A degree of technical skill is required on the part of the data end-user, which is often problematic for air quality agencies with limited resources. Therefore, we 1) review the primary uses of satellite data for air quality applications, 2) provide some background information on satellite capabilities for measuring pollutants, 3) discuss the many resources available to the end-user for accessing, processing, and visualizing the data, and 4) provide answers to common questions in plain language.

We measured and characterized semi-volatile chemical composition of particulate matter (PM) in aircraft engine exhaust plumes in a dedicated aircraft PM emission study (NASA's AAFEX 1 field measurement campaign). Mode-specific organic and sulfate components were observed with a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS). Nitrate components in both the nucleation and soot mode particles were negligible. The organic composition for the nucleation mode particles decreases with increasing engine power. For the soot mode, organic fraction initially decreases with increasing engine power but then slightly increases again above 45% engine thrust, probably due to the increasing contribution from lubrication oil emissions. These results show that an appreciable amount of semi-volatile PM can be generated in the exhaust plumes from a commercial aircraft engine. Thus, volatile PM must be studied as carefully as non-volatile soot emissions to fully address local air quality and human health impacts of aviation.

As part of the third NASA Aircraft Particle Emissions Experiment (APEX-3, November 2005), whole air samples were collected to determine the emission rates of volatile organic compounds (VOCs) from aircraft equipped with three different gas-turbine engines (an Allison Engine 3007-A1E, a Pratt–Whitney 4158, and a Rolls–Royce RB211-535E4B). Samples were collected 1 m behind the engine exhaust plane of the engines while they were operated at powers ranging from idle up to 30% of maximum rated thrust. Exhaust emission indices (mass emitted per kilogram of fuel used) for CO and non-methane hydrocarbons (NMHCs) were calculated based on enhancements over background relative to CO2. Emissions of all NMHCs were greatest at low power with values decreasing by an order of magnitude with increasing power. Previous studies have shown that scaling idle hydrocarbon emissions to formaldehyde or ethene (which are typically emitted at a ratio of 1-to-1 at idle) reduces variability amongst engine types. NMHC emissions were found to scale at low power, with alkenes contributing over 50% of measured NMHCs. However, as the power increases hydrocarbon emissions no longer scale to ethene, as the aromatics become the dominant species emitted. This may be due in part to a shift in combustion processes from thermal cracking (producing predominantly alkenes) to production of new molecules (producing proportionally more aromatics) as power increases. The formation of these aromatics is an intermediate step in the production of soot, which also increases with increasing power. The increase in aromatics relative to alkenes additionally results in a decrease in the hydroxyl radical reactivity and ozone formation potential of aircraft exhaust. Samples collected 30 m downwind of the engine were also analyzed for NMHCs and carbonyl compounds (acetone, 2-butanone and C1–C9 aldehydes). Formaldehyde was the predominant carbonyl emitted; however, the ratio of ethene-to-formaldehyde varied between the aircraft, possibly due to the sampling of transient emissions such as engine start-up and power changes. A large portion of the measured emissions (27–42% by mass) in the plume samples was made up of hazardous air pollutants (HAPs) with oxygenated compounds being most significant.

Multiyear (2000–2006) seasonal measurements of carbon monoxide, hydrocarbons, halogenated species, dimethyl sulfide, carbonyl sulfide and C 1 –C 4 alkyl nitrates at the South Pole are presented for the first time. At the South Pole, short-lived species (such as the alkenes) typically were not observed above their limits of detection because of long transit times from source regions. Peak mixing ratios of the longer lived species with anthropogenic sources were measured in late winter (August and September) with decreasing mixing ratios throughout the spring. In comparison, compounds with a strong oceanic source, such as bromoform and methyl iodide, had peak mixing ratios earlier in the winter (June and July) because of decreased oceanic production during the winter months. Dimethyl sulfide (DMS), which is also oceanically emitted but has a short lifetime, was rarely measured above 5 pptv. This is in contrast to high DMS mixing ratios at coastal locations and shows the importance of photochemical removal during transport to the pole. Alkyl nitrate mixing ratios peaked during April and then decreased throughout the winter. The dominant source of the alkyl nitrates in the region is believed to be oceanic emissions rather than photochemical production due to low alkane levels. Sampling of other tropospheric environments via a Twin Otter aircraft included the west coast of the Ross Sea and large stretches of the Antarctic Plateau. In the coastal atmosphere, a vertical gradient was found with the highest mixing ratios of marine emitted compounds at low altitudes. Conversely, for anthropogenically produced species the highest mixing ratios were measured at the highest altitudes, suggesting long-range transport to the continent. Flights flown through the plume of Mount Erebus, an active volcano, revealed that both carbon monoxide and carbonyl sulfide are emitted with an OCS/CO molar ratio of 3.3 × 10 −3 consistent with direct observations by other investigators within the crater rim.

Between 1999 and 2005 a sampling campaign was conducted to identify and quantify the major species of atmospheric nonmethane hydrocarbons (NMHCs) in United States cities. Whole air canister samples were collected in 28 cities and analyzed for methane, carbon monoxide (CO) and NMHCs. Ambient mixing ratios exhibited high inter- and intra-city variability, often having standard deviations in excess of 50% of the mean value. For this reason, ratios of individual NMHC to CO, a combustion tracer, were examined to facilitate comparison between cities. Ratios were taken from correlation plots between the species of interest and CO, and most NMHCs were found to have correlation coefficients (r2) greater than 0.6, particularly ethene, ethyne and benzene, highlighting the influence of vehicular emissions on NMHC mixing ratios. Notable exceptions were the short-chain alkanes, which generally had poor correlations with CO. Ratios of NMHC vs. CO were also used to identify those cities with unique NMHC sources.

The first measurements of peroxy (HO2+RO2) and hydroxyl (OH) radicals above the arctic snowpack were collected during the summer 2003 campaign at Summit, Greenland. The median measured number densities for peroxy and hydroxyl radicals were 2.2×108 mol cm−3 and 6.4×106 mol cm−3, respectively. The observed peroxy radical values are in excellent agreement (R2=0.83, M/O=1.06) with highly constrained model predictions. However, calculated hydroxyl number densities are consistently more than a factor of 2 lower than the observed values. These results indicate that our current understanding of radical sources and sinks is in accord with our observations in this environment but that there may be a mechanism that is perturbing the (HO2+RO2)/OH ratio. This observed ratio was also found to depend on meteorological conditions especially during periods of high winds accompanied by blowing snow. Backward transport model simulations indicate that these periods of high winds were characterized by rapid transport (1–2 days) of marine boundary layer air to Summit. These data suggest that the boundary layer photochemistry at Summit may be periodically impacted by halogens.

Experiments were performed at Summit, Greenland (72°34′ N, 38°29′ W) to investigate hydroxyl mixing ratios in the sunlit surface snowpack (or firn). We added a carefully selected mixture of hydrocarbon gases (with a wide range of hydroxyl reactivities) to a UV and visible light transparent flow chamber containing undisturbed natural firn. The relative decrease in mixing ratios of these gases allowed estimation of the lower limit mixing ratio of hydroxyl radicals in the near-surface firn pore spaces. Hydroxyl mixing ratios in the firn air followed a diurnal cycle in summer 2003 (10–12 July), with peak values of more than 3.2×106 molecules cm−3 between 13:00 and 16:00 local time. The minimum value estimated was 1.1×106 molecules cm−3 at 20:00 local time. Results during spring of 2004 showed lower, but rapidly increasing, peak hydroxyl mixing ratios of 1.1×106 molecules cm−3 in the early afternoon on 15 April and 1.5×106 molecules cm−3 on 1 May. Our firn hydroxyl estimates were similar to directly measured above-snow ambient levels during the spring field season, but were only about 30% of ambient levels during summer.

Author(s): Dibb, JE; Albert, M; Anastasio, C; Atlas, E; Beyersdorf, AJ; Blake, NJ; Blake, DR; Bocquet, F; Burkhart, JF; Chen, G; Cohen, L; Conway, TJ; Courville, Z; Frey, MM; Friel, DK; Galbavy, ES; Hall, S; Hastings, MG; Helmig, D; Greg Huey, L; Hutterli, MA; Jarvis, JC; Lefer, BL; Meinardi, S; Neff, W; Oltmans, SJ; Sherwood Rowland, F; Sjostedt, SJ; Steig, EJ; Swanson, AL; Tanner, DJ