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)−1 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)−1 during the primary burning period to 18.3 ppb CH4 (ppm CO2)−1 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.
•Airborne measurements of trace gases downwind of an exceptionally large wildfire.•Measurements during the Rim wildfire intense and smoldering burning phases.•Assessment of emission ratios, emission factors and combustion efficiency.•Dataset to support forestry and regional air quality management.
During the POLARCAT summer campaign in 2008, two episodes (2-5 July and 7-10 July 2008) occurred where low-pressure systems traveled from Siberia across the Arctic Ocean towards the North Pole. The ...two cyclones had extensive smoke plumes from Siberian forest fires and anthropogenic sources in East Asia embedded in their associated air masses, creating an excellent opportunity to use satellite and aircraft observations to validate the performance of atmospheric transport models in the Arctic, which is a challenging model domain due to numerical and other complications. Here we compare transport simulations of carbon monoxide (CO) from the Lagrangian transport model FLEXPART and the Eulerian chemical transport model TOMCAT with retrievals of total column CO from the IASI passive infrared sensor onboard the MetOp-A satellite. The main aspect of the comparison is how realistic horizontal and vertical structures are represented in the model simulations. Analysis of CALIPSO lidar curtains and in situ aircraft measurements provide further independent reference points to assess how reliable the model simulations are and what the main limitations are. The horizontal structure of mid-latitude pollution plumes agrees well between the IASI total column CO and the model simulations. However, finer-scale structures are too quickly diffused in the Eulerian model. Applying the IASI averaging kernels to the model data is essential for a meaningful comparison. Using aircraft data as a reference suggests that the satellite data are biased high, while TOMCAT is biased low. FLEXPART fits the aircraft data rather well, but due to added background concentrations the simulation is not independent from observations. The multi-data, multi-model approach allows separating the influences of meteorological fields, model realisation, and grid type on the plume structure. In addition to the very good agreement between simulated and observed total column CO fields, the results also highlight the difficulty to identify a data set that most realistically represents the actual pollution state of the Arctic atmosphere.
In the spring of 2008 NASA and NOAA funded the ARCTAS and ARCPAC field campaigns as contributions to POLARCAT, a core IPY activity. During the campaigns the NASA DC-8, P-3B and NOAA WP-3D aircraft ...conducted over 160 h of in-situ sampling between 0.1 and 12 km throughout the Western Arctic north of 55° N (i.e. Alaska to Greenland). All aircraft were equipped with multiple wavelength measurements of aerosol optics, trace gas and aerosol chemistry measurements, as well as direct measurements of the aerosol size distributions and black carbon mass. Late April of 2008 proved to be exceptional in terms of Asian biomass burning emissions transported to the Western Arctic. Though these smoke plumes account for only 11–14 % of the samples within the Western Arctic domain, they account for 42–47 % of the total burden of black carbon. Dust was also commonly observed but only contributes to 4–12 % and 3–8 % of total light absorption at 470 and 530 nm wavelengths above 6 km. Below 6 km, light absorption by carbonaceous aerosol derived from urban/industrial and biomass burning emissions account for 97–99 % of total light absorption by aerosol. Stratifying the data to reduce the influence of dust allows us to determine mass absorption efficiencies for black carbon of 11.2±0.8, 9.5±0.6 and 7.4±0.7 m2 g−1 at 470, 530 and 660 nm wavelengths. These estimates are consistent with 35–80 % enhancements in 530 nm absorption due to clear or slightly absorbing coatings of pure black carbon particulate. Assuming a 1/λ wavelength dependence for BC absorption, and assuming that refractory aerosol (420 °C, τ = 0.1 s) in low-dust samples is dominated by brown carbon, we derive mass absorption efficiencies for brown carbon of 0.83±0.15 and 0.27±0.08 m2 g−1 at 470 and 530 nm wavelengths. Estimates for the mass absorption efficiencies of Asian dust are 0.034 m2 g−1 and 0.017 m2 g−1. However the absorption efficiency estimates for dust are highly uncertain due to the limitations imposed by PSAP instrument noise. In-situ ARCTAS/ARCPAC measurements during the IPY provide valuable constraints for absorbing aerosol over the Western Arctic, species which are currently poorly simulated over a region that is critically under-sampled.
One‐second in situ measurements of CO and CO2 mole fractions were made aboard the National Aeronautics and Space Administration DC‐8 aircraft during the 2016 KORUS‐AQ joint air quality and ...atmospheric chemistry field campaign in South Korea. The ratio of CO to CO2 enhancement is used to characterize regional combustion source signatures. Calculations of the ∆CO/∆CO2 ratio were made with a short duration rolling window (60 s), filtered by the coefficient of determination (R2), and plotted as distributions to characterize air masses measured from the aircraft during the campaign. The KORUS‐AQ sampling domain was divided into analysis regions to facilitate the analysis. Over Seoul, the boundary layer shows a low‐ratio signature in the ∆CO/∆CO2 ratios, with more than 50% of the correlated slopes in the boundary layer falling below 1% ∆CO/∆CO2, and 80% of the slopes between 0% and 2% ∆CO/∆CO2. However, this behavior changes to a larger ratio distribution at higher altitudes. The West Sea receptor region was divided into three analysis sectors, by meteorological regime, and used in conjunction with measurements collected over China during the KORUS‐AQ campaign time period to characterize the Chinese ∆CO/∆CO2 ratio signature. Chinese‐type emissions have a slope distribution that is shifted to higher ratios and broadened compared to measurements over Seoul, with the bulk of the measurements between 2% and 4% ∆CO/∆CO2, with few negative slopes. The measured ratio trends over South Korea are consistent with inventoried CO and CO2 emissions.
Plain Language Summary
Measurements of carbon monoxide (CO) and carbon dioxide (CO2) were made over South Korea in May and June of 2016. The ratio of CO to CO2 provides information about the combustion sources in a region, as most of the CO measured in the atmosphere is sourced from combustion, such as open air fires or engines. Using a 1‐s data set, the short‐term slopes of CO to CO2 enhancement were calculated by making a measurement of the CO to CO2 slope at every observation using the data in the surrounding minute. Plotting the distributions of the short‐term slopes with correlated values in the calculation window reveals whether the air masses have mostly low ratios of CO/CO2, which indicates high‐efficiency combustion, or mostly high ratios of CO/CO2, from low‐efficiency combustion. The slope distributions over the Seoul megacity show low‐ratio distributions, but at high altitudes the ratios move to higher values, showing that the combustion sources change with altitude and have a less efficient combustion signature. Meanwhile, the ratios that were measured over the West Sea show that the air coming to South Korea from China has higher CO/CO2 ratios than the air that is measured over South Korea.
Key Points
Short‐term ∆CO/∆CO2 ratios characterized air masses measured by aircraft over South Korea during the 2016 KORUS‐AQ field campaign
The air mass combustion efficiency signature can be assessed with the distribution of the correlated short‐term CO to CO2 slopes
Differences were found between Chinese influenced and South Korea influenced air masses, which reflect the known sources in each country
High‐frequency (20 Hz) aircraft measurements of tropical tropopause layer (TTL) cirrus and humidity are used to examine recent homogeneous freezing ice nucleation events. Several localized regions ...with peak ice concentrations greater than 10 cm−3 are documented. These high ice concentrations are almost certainly generated by homogeneous freezing of aqueous aerosols. The high‐frequency data reveals considerable structure in the cloud properties and humidity at along‐track scales as short as 8.5 m. Simulations of vapor depletion by growing ice crystals are used to assess the time since nucleation in these high ice concentration patches. Comparisons between observed and simulated dependence of supersaturation on ice concentration indicate the nucleation events occurred within minutes (sometimes only a few minutes) of the aircraft sampling. The infrequency and short ages of the events suggest that the high ice concentrations do not persist for long times, but they may still be important for TTL cirrus microphysical properties by providing a source of ice crystals that can lead to extensive, persistent clouds with lower ice concentrations. We have also used the extensive TTL measurements provided by the high‐altitude aircraft campaigns to evaluate the threshold supersaturation for homogeneous freezing. Peak supersaturations observed are consistent with recent laboratory experiments indicating that ice saturation ratios of about 1.75–1.95 are required for homogeneous freezing of aqueous aerosols at temperatures of 185–200 K.
Plain Language Summary
High‐frequency aircraft measurements of cirrus clouds and humidity in the cold, tropical upper troposphere are used to examine recent ice crystal formation events. Several localized regions with very large numbers of small ice crystals are documented. The numerous ice crystals are almost certainly generated by spontaneous freezing of abundant liquid aerosol particles. The high‐frequency data reveals considerable fine‐scale structure in the cloud properties and humidity. Comparisons with calculations of water vapor depletion by growing ice crystals indicate the formation events occurred within minutes (sometimes only a few minutes) of the aircraft sampling. The infrequency and short ages of the events suggest that the high ice number densities do not persist for long times, but they may still be important for cirrus physical properties by providing a source of ice crystals that can lead to extensive, persistent clouds with lower ice numbers. We have also used the extensive measurements provided by the high‐altitude aircraft campaigns to evaluate the threshold conditions for spontaneous freezing of liquid aerosol particles. The threshold conditions are consistent with recent laboratory experiments indicating that substantial super‐cooling must occur before the liquid aerosol particles can freeze.
Key Points
High‐frequency airborne cloud and humidity measurements are used to examine high ice concentration events in the tropical tropopause layer
The supersaturation in some of these events indicates that ice nucleation occurred less than 12 min prior to the aircraft sampling
Peak supersaturation measurements indicate a higher threshold for homogeneous freezing than previously assumed in models
An instrumented NASA P-3B aircraft was used for airborne sampling of trace gases in a plume that had emanated from a small forest understory fire in Georgia, USA. The plume was sampled at its origin ...to derive emission factors and followed ∼ 13.6 km downwind to observe chemical changes during the first hour of atmospheric aging. The P-3B payload included a proton-transfer-reaction time-of-flight mass spectrometer (PTR-ToF-MS), which measured non-methane organic gases (NMOGs) at unprecedented spatiotemporal resolution (10 m spatial/0.1 s temporal). Quantitative emission data are reported for CO2, CO, NO, NO2, HONO, NH3, and 16 NMOGs (formaldehyde, methanol, acetonitrile, propene, acetaldehyde, formic acid, acetone plus its isomer propanal, acetic acid plus its isomer glycolaldehyde, furan, isoprene plus isomeric pentadienes and cyclopentene, methyl vinyl ketone plus its isomers crotonaldehyde and methacrolein, methylglyoxal, hydroxy acetone plus its isomers methyl acetate and propionic acid, benzene, 2,3-butanedione, and 2-furfural) with molar emission ratios relative to CO larger than 1 ppbV ppmV−1. Formaldehyde, acetaldehyde, 2-furfural, and methanol dominated NMOG emissions. No NMOGs with more than 10 carbon atoms were observed at mixing ratios larger than 50 pptV ppmV−1 CO. Downwind plume chemistry was investigated using the observations and a 0-D photochemical box model simulation. The model was run on a nearly explicit chemical mechanism (MCM v3.3) and initialized with measured emission data. Ozone formation during the first hour of atmospheric aging was well captured by the model, with carbonyls (formaldehyde, acetaldehyde, 2,3-butanedione, methylglyoxal, 2-furfural) in addition to CO and CH4 being the main drivers of peroxy radical chemistry. The model also accurately reproduced the sequestration of NOx into peroxyacetyl nitrate (PAN) and the OH-initiated degradation of furan and 2-furfural at an average OH concentration of 7.45 ± 1.07 × 106 cm−3 in the plume. Formaldehyde, acetone/propanal, acetic acid/glycolaldehyde, and maleic acid/maleic anhydride (tentatively identified) were found to be the main NMOGs to increase during 1 h of atmospheric plume processing, with the model being unable to capture the observed increase. A mass balance analysis suggests that about 50 % of the aerosol mass formed in the downwind plume is organic in nature.
In this paper, we provide a detailed comparison between carbon monoxide (CO) data measured by the Infrared Atmospheric Sounding Interferometer (IASI)/MetOp and aircraft observations over the Arctic. ...The CO measurements were obtained during North American (NASA ARCTAS and NOAA ARCPAC) and European campaigns (POLARCAT-France, POLARCAT-GRACE and YAK-AEROSIB) as part of the International Polar Year (IPY) POLARCAT activity in spring and summer 2008. During the campaigns different air masses were sampled including clean air, polluted plumes originating from anthropogenic sources in Europe, Asia and North America, and forest fire plumes originating from Siberia and Canada. The paper illustrates that CO-rich plumes following different transport pathways were well captured by the IASI instrument, in particular due to the high spatial coverage of IASI. The comparison between IASI CO total columns, 0-5 km partial columns and profiles with collocated aircraft data was achieved by taking into account the different sensitivity and geometry of the sounding instruments. A detailed analysis is provided and the agreement is discussed in terms of information content and surface properties at the location of the observations. For profiles, the data were found to be in good agreement in spring with differences lower than 17%, whereas in summer the difference can reach 20% for IASI profiles below 8 km for polluted cases. For total columns the correlation coefficients ranged from 0.15 to 0.74 (from 0.47 to 0.77 for partial columns) in spring and from 0.26 to 0.84 (from 0.66 to 0.88 for partial columns) in summer. A better agreement is seen over the sea in spring (0.73 for total column and 0.78 for partial column) and over the land in summer (0.69 for total columns and 0.81 for partial columns). The IASI vertical sensitivity was better over land than over sea, and better over land than over sea ice and snow allowing a higher potential to detect CO vertical distribution during summer.
We present a climatology of O3, CO, and H2O for the upper troposphere and lower stratosphere (UTLS), based on a large collection of high‐resolution research aircraft data taken between 1995 and 2008. ...To group aircraft observations with sparse horizontal coverage, the UTLS is divided into three regimes: the tropics, subtropics, and the polar region. These regimes are defined using a set of simple criteria based on tropopause height and multiple tropopause conditions. Tropopause‐referenced tracer profiles and tracer‐tracer correlations show distinct characteristics for each regime, which reflect the underlying transport processes. The UTLS climatology derived here shows many features of earlier climatologies. In addition, mixed air masses in the subtropics, identified by O3‐CO correlations, show two characteristic modes in the tracer‐tracer space that are a result of mixed air masses in layers above and below the tropopause (TP). A thin layer of mixed air (1–2 km around the tropopause) is identified for all regions and seasons, where tracer gradients across the TP are largest. The most pronounced influence of mixing between the tropical transition layer and the subtropics was found in spring and summer in the region above 380 K potential temperature. The vertical extent of mixed air masses between UT and LS reaches up to 5 km above the TP. The tracer correlations and distributions in the UTLS derived here can serve as a reference for model and satellite data evaluation.
Acquiring accurate measurements of water vapor at the low mixing ratios (< 10 ppm) encountered in the upper troposphere and lower stratosphere (UT/LS) has proven to be a significant analytical ...challenge evidenced by persistent disagreements between high‐precision hygrometers. These disagreements have caused uncertainties in the description of the physical processes controlling dehydration of air in the tropical tropopause layer and entry of water into the stratosphere and have hindered validation of satellite water vapor retrievals. A 2011 airborne intercomparison of a large group of in situ hygrometers onboard the NASA WB‐57F high‐altitude research aircraft and balloons has provided an excellent opportunity to evaluate progress in the scientific community toward improved measurement agreement. In this work we intercompare the measurements from the Midlatitude Airborne Cirrus Properties Experiment (MACPEX) and discuss the quality of agreement. Differences between values reported by the instruments were reduced in comparison to some prior campaigns but were nonnegligible and on the order of 20% (0.8 ppm). Our analysis suggests that unrecognized errors in the quantification of instrumental background for some or all of the hygrometers are a likely cause. Until these errors are understood, differences at this level will continue to somewhat limit our understanding of cirrus microphysical processes and dehydration in the tropical tropopause layer.
Key Points
Agreement among in situ measurements of UT/LS water vapor is improved
Scientifically significant disagreements between instruments still exist
The National Aeronautics and Space Administration (NASA) conducted the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) mission during 2008 as a part of the ...International Polar Year (IPY). The purpose of ARCTAS was to study the factors responsible for changes in the Arctic's atmospheric composition and climate. A major emphasis was to investigate Arctic haze, which is most pronounced during winter and early spring. This study focuses on the spring phase of ARCTAS (ARCTAS-A) that was based in Alaska during April 2008. Although anthropogenic emissions historically have been associated with Arctic haze, biomass burning emissions dominated the ARCTAS-A period and have been the focus of many ARCTAS related studies. This study determines mean transport characteristics of anthropogenic emissions during ARCTAS-A. Trajectories are initiated each day from three significant regions of anthropogenic emissions (Asia, North America, and Europe). The fifteen day forward trajectories are calculated using data from the Weather Research and Forecasting (WRF) model at 45 km horizontal resolution. The trajectory calculations indicate: origins of emissions that reach the Arctic (defined as north of 70° N) within fifteen days, pathways of these emissions, Arctic entry locations, and altitudes at which the trajectories enter the Arctic. Three cases during the ARCTAS-A period (one for each of the regions above) are examined using backward trajectories and chemical fingerprinting based on in situ data sampled from the NASA DC-8. The fingerprinting utilizes volatile organic compounds that represent pure anthropogenic tracers, Asian anthropogenic pollution, incomplete combustion, and natural gas emissions. We determine flight legs containing anthropogenic emissions and the pathways travelled by these emissions. Results show that the DC-8 sampled anthropogenic emissions from Asia, North America, and Europe during the spring phase of ARCTAS. The pathways travelled by these emissions agree with our derived transport characteristics and previous studies of Arctic transport. Meteorological analysis and trajectory calculations indicate that middle latitude cyclones and their associated warm conveyor belts play an important role in lofting the surface based emissions to their sampling altitude in all three cases.
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