Aircraft And Satellites Research Articles

Observations of nonmethane organic compounds during ARCTAS − Part 1: Biomass burning emissions and plume enhancements

Abstract. Mixing ratios of a large number of nonmethane organic compounds (NMOCs) were observed by the Trace Organic Gas Analyzer (TOGA) on board the NASA DC-8 as part of the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) field campaign. Many of these NMOCs were observed concurrently by one or both of two other NMOC measurement techniques on board the DC-8: proton-transfer-reaction mass spectrometry (PTR-MS) and whole air canister sampling (WAS). A comparison of these measurements to the data from TOGA indicates good agreement for the majority of co-measured NMOCs. The ARCTAS study, which included both spring and summer deployments, provided opportunities to sample a large number of biomass burning (BB) plumes with origins in Asia, California and central Canada, ranging from very recent emissions to plumes aged one week or more. For this analysis, BB smoke interceptions were grouped by flight, source region and, in some cases, time of day, generating 40 identified BB plumes for analysis. Normalized excess mixing ratios (NEMRs) to CO were determined for each of the 40 plumes for up to 19 different NMOCs or NMOC groups. Although the majority of observed NEMRs for individual NMOCs or NMOC groups were in agreement with previously-reported values, the observed NEMRs to CO for ethanol, a rarely quantified gas-phase trace gas, ranged from values similar to those previously reported, to up to an order of magnitude greater. Notably, though variable between plumes, observed NEMRs of individual light alkanes are highly correlated within BB emissions, independent of estimated plume ages. BB emissions of oxygenated NMOC were also found to be often well-correlated. Using the NCAR Master Mechanism chemical box model initialized with concentrations based on two observed scenarios, fresh Canadian BB and fresh Californian BB, decreases are predicted for the low molecular weight carbonyls (i.e. formaldehyde, acetaldehyde, acetone and methyl ethyl ketone, MEK) and alcohols (i.e. methanol and ethanol) as the plumes evolve in time, i.e. the production of these compounds is less than the chemical loss. Comparisons of the modeled NEMRs to the observed NEMRs from BB plumes estimated to be three days in age or less indicate overall good agreement.

Accumulation-mode aerosol number concentrations in the Arctic during the ARCTAS aircraft campaign: Long-range transport of polluted and clean air from the Asian continent

[1] We evaluate the impact of transport from midlatitudes on aerosol number concentrations in the accumulation mode (light‐scattering particles (LSP) with diameters >180 nm) in the Arctic during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. We focus on transport from the Asian continent. We find marked contrasts in the number concentration (NLSP), transport efficiency (TEN_LSP, the fraction transported from sources to the Arctic), size distribution, and the chemical composition of aerosols between air parcels from anthropogenic sources in East Asia (Asian AN) and biomass burning sources in Russia and Kazakhstan (Russian BB). Asian AN air had lower NLSP and TEN_LSP (25 cm �3 and 18% in spring and 6.2 cm �3 and 3.0% in summer) than Russian BB air (280 cm �3 and 97% in spring and 36 cm �3 and 7.6% in summer) due to more efficient wet scavenging during transport from East Asia. Russian BB in this spring is the most important source of accumulation‐mode aerosols over the Arctic, and BB emissions are found to be the primary source of aerosols within all the data in spring during ARCTAS. On the other hand, the contribution of Asian AN transport had a negligible effect on the accumulation‐mode aerosol number concentration in the Arctic during ARCTAS. Compared with background air, NLSP was 2.3–4.7 times greater for Russian BB air but 2.4–2.6 times less for Asian AN air in both spring and summer. This result shows that the transport of Asian AN air decreases aerosol number concentrations in the Arctic, despite the large emissions of aerosols in East Asia. The very low aerosol number concentrations in Asian AN air were caused by wet removal during vertical transport in association with warm conveyor belts (WCBs). Therefore, this cleansing effect will be prominent for air transported via WCBs from other midlatitude regions and seasons. The inflow of clean midlatitude air can potentially have an important impact on accumulation‐mode aerosol number concentrations in the Arctic. Citation: Matsui, H., et al. (2011), Accumulation‐mode aerosol number concentrations in the Arctic during the ARCTAS aircraft campaign: Long‐range transport of polluted and clean air from the Asian continent, J. Geophys. Res., 116, D20217, doi:10.1029/2011JD016189.

Anthropogenic emissions during Arctas-A: mean transport characteristics and regional case studies

Abstract. 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.

CO source contribution analysis for California during ARCTAS-CARB

Abstract. Air pollution is of concern in many parts of California and is impacted by both local emissions and also by pollution inflow from the North Pacific Ocean. In this study, we use the regional chemical transport model WRF-Chem V3.2 together with the global Model for OZone and Related Chemical Tracers to examine the CO budget over California. We include model CO tracers for different emission sources in the models, which allow estimation of the relative importance of local sources versus pollution inflow on the distribution of CO at the surface and in the free troposphere. The focus of our study is on the 15 June–15 July 2008 time period, which coincides with the aircraft deployment of the NASA Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) mission over California. Model simulations are evaluated using these aircraft observations as well as satellite retrievals and surface observations of CO. Evaluation results show that the model overall predicts the observed CO fields well, but points towards an underestimate of CO from the fires in Northern California, which had a strong influence during the study period, and towards a slight overestimate of CO from pollution inflow and local anthropogenic sources. The analysis of the CO budget over California reveals that inflow of CO explains on average 99 ± 11 ppbV of surface CO during the study period, compared to 61 ± 95 ppbV for local anthropogenic direct emissions of CO and 84 ± 194 ppbV for fires. In the free troposphere, the average CO contributions are estimated as 96 ± 7 ppbV for CO inflow, 8 ± 9 ppbV for CO from local anthropogenic sources and 18 ± 13 ppbV for CO from fires. Accounting for the low bias in the CO fire emission inventory, the fire impact during the study period might have been up to a factor 4 higher than the given estimates.

Combined retrievals of boreal forest fire aerosol properties with a polarimeter and lidar

Abstract. Absorbing aerosols play an important, but uncertain, role in the global climate. Much of this uncertainty is due to a lack of adequate aerosol measurements. While great strides have been made in observational capability in the previous years and decades, it has become increasingly apparent that this development must continue. Scanning polarimeters have been designed to help resolve this issue by making accurate, multi-spectral, multi-angle polarized observations. This work involves the use of the Research Scanning Polarimeter (RSP). The RSP was designed as the airborne prototype for the Aerosol Polarimetery Sensor (APS), which was due to be launched as part of the (ultimately failed) NASA Glory mission. Field observations with the RSP, however, have established that simultaneous retrievals of aerosol absorption and vertical distribution over bright land surfaces are quite uncertain. We test a merger of RSP and High Spectral Resolution Lidar (HSRL) data with observations of boreal forest fire smoke, collected during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS). During ARCTAS, the RSP and HSRL instruments were mounted on the same aircraft, and validation data were provided by instruments on an aircraft flying a coordinated flight pattern. We found that the lidar data did indeed improve aerosol retrievals using an optimal estimation method, although not primarily because of the contraints imposed on the aerosol vertical distribution. The more useful piece of information from the HSRL was the total column aerosol optical depth, which was used to select the initial value (optimization starting point) of the aerosol number concentration. When ground based sun photometer network climatologies of number concentration were used as an initial value, we found that roughly half of the retrievals had unrealistic sizes and imaginary indices, even though the retrieved spectral optical depths agreed within uncertainties to independent observations. The convergence to an unrealistic local minimum by the optimal estimator is related to the relatively low sensitivity to particles smaller than 0.1 (μm) at large optical thicknesses. Thus, optimization algorithms used for operational aerosol retrievals of the fine mode size distribution, when the total optical depth is large, will require initial values generated from table look-ups that exclude unrealistic size/complex index mixtures. External constraints from lidar on initial values used in the optimal estimation methods will also be valuable in reducing the likelihood of obtaining spurious retrievals.

An investigation of methods for injecting emissions from boreal wildfires using WRF-Chem during ARCTAS

Abstract. The Weather Research and Forecasting Model (WRF) is considered a "next generation" mesoscale meteorology model. The inclusion of a chemistry module (WRF-Chem) allows transport simulations of chemical and aerosol species such as those observed during NASA's Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) in 2008. The ARCTAS summer deployment phase during June and July coincided with large boreal wildfires in Saskatchewan and Eastern Russia. One of the most important aspects of simulating wildfire plume transport is the height at which emissions are injected. WRF-Chem contains an integrated one-dimensional plume rise model to determine the appropriate injection layer. The plume rise model accounts for thermal buoyancy associated with fires and local atmospheric stability. This paper describes a case study of a 10 day period during the Spring phase of ARCTAS. It compares results from the plume model against those of two more traditional injection methods: Injecting within the planetary boundary layer, and in a layer 3–5 km above ground level. Fire locations are satellite derived from the GOES Wildfire Automated Biomass Burning Algorithm (WF_ABBA) and the MODIS thermal hotspot detection. Two methods for preprocessing these fire data are compared: The prep_chem_sources method included with WRF-Chem, and the Naval Research Laboratory's Fire Locating and Monitoring of Burning Emissions (FLAMBE). Results from the simulations are compared with satellite-derived products from the AIRS, MISR and CALIOP sensors. When FLAMBE provides input to the 1-D plume rise model, the resulting injection heights exhibit the best agreement with satellite-observed injection heights. The FLAMBE-derived heights are more realistic than those utilizing prep_chem_sources. Conversely, when the planetary boundary layer or the 3–5 km a.g.l. layer were filled with emissions, the resulting injection heights exhibit less agreement with observed plume heights. Results indicate that differences in injection heights produce different transport pathways. These differences are especially pronounced in area of strong vertical wind shear and when the integration period is long.

Global and regional effects of the photochemistry of CH<sub>3</sub>O<sub>2</sub>NO<sub>2</sub>: evidence from ARCTAS

Abstract. Using measurements from the NASA Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) experiment, we show that methyl peroxy nitrate (CH3O2NO2) is present in concentrations of ~5–15 pptv in the springtime arctic upper troposphere. We investigate the regional and global effects of CH3O2NO2 by including its chemistry in the GEOS-Chem 3-D global chemical transport model. We find that at temperatures below 240 K inclusion of CH3O2NO2 chemistry results in decreases of up to ~20 % in NOx, ~20 % in N2O5, ~5 % in HNO3, ~2 % in ozone, and increases in methyl hydrogen peroxide of up to ~14 %. Larger changes are observed in biomass burning plumes lofted to high altitude. Additionally, by sequestering NOx at low temperatures, CH3O2NO2 decreases the cycling of HO2 to OH, resulting in a larger upper tropospheric HO2 to OH ratio. These results may impact some estimates of lightning NOx sources as well as help explain differences between models and measurements of upper tropospheric composition.

Pollution transport efficiency toward the Arctic: Sensitivity to aerosol scavenging and source regions

The processes driving current changes in Arctic atmospheric composition and climate are still uncertain. In particular the relative contributions of major source regions from the midlatitudes remain a matter of debate in the literature. The objectives of this study are to better quantify the relative contributions of different processes governing the transport of pollution from the midlatitudes to the Arctic and the relative contributions of different geopolitical source regions. We use a suite of observational data sets (including the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaigns and the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) satellite instrument) to constrain a global aerosol simulation from the ECHAM5-HAMMOZ model. Preliminary comparison of model results with vertical profiles of sulfate and black carbon (BC) collected during the ARCTAS campaigns and with aerosol extinction time series retrieved from CALIOP indicates that the model underestimates export of aerosols from the planetary boundary layer to the free troposphere in the midlatitudes and long-range transport of aerosols from the midlatitudes toward the Arctic. In contrast, observed CO profiles are relatively well simulated, which points to a possible problem with wet scavenging. Decreasing the prescribed aerosol scavenging coefficients within the range of experimental data available in the literature significantly improves the agreement with observations. Sulfate and BC burdens in the Arctic increase by a factor 5-6. Annual global lifetimes of sulfate and BC increase from 3.1 to 4.6 days and from 4.4 to 5.9 days, respectively. Using the improved simulation, we find that 59% of sulfate in the Arctic troposphere comes from the oxidation of SO2 emitted in Siberia (19%), Europe (18%), Asia (13%), and North America (9%). Anthropogenic and biomass burning BC emitted in Siberia, Asia, Europe, and North America contributes 29, 27, 25, and 17%, respectively, to the Arctic BC burden. Emissions of aerosols (or precursors) from Siberia and Europe are more susceptible to be transported and subsequently deposited on the Arctic (about 7-12%) compared to those from North America and Asia (1-4%). Overall, the study shows that aerosol scavenging removal processes play a crucial role on the aerosol transport from the midlatitudes toward the Arctic and should be carefully characterized in aerosol models.

Airborne observation of aerosol optical depth during ARCTAS: vertical profiles, inter-comparison and fine-mode fraction

Abstract. We describe aerosol optical depth (AOD) measured during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) experiment, focusing on vertical profiles, inter-comparison with correlative observations and fine-mode fraction. Arctic haze observed in <2 km and 2–4 km over Alaska in April 2008 originated mainly from anthropogenic emission and biomass burning, respectively, according to aerosol mass spectrometry and black carbon incandescence measurements. The Ångström exponent for these air masses is 1.4 ± 0.3 and 1.7 ± 0.1, respectively, when derived at 499 nm from a second-order polynomial fit to the AOD spectra measured with the 14-channel Ames Airborne Tracking Sunphotometer (AATS-14) over 354–2139 nm. We examine 55 vertical profiles selected from all phases of the experiment. For two thirds of them, the AOD spectra are within 3% + 0.02 of the vertical integral of local visible-light scattering and absorption. The horizontal structure of smoke plumes from local biomass burning observed in central Canada in June and July 2008 explains most outliers. The differences in mid-visible Ångström exponent are <0.10 for 63% of the profiles with 499-nm AOD > 0.1. The retrieved fine-mode fraction of AOD is mostly between 0.7 and 1.0, and its root mean square difference (in both directions) from column-integral submicron fraction (measured with nephelometers, absorption photometers and an impactor) is 0.12. These AOD measurements from the NASA P-3 aircraft, after compensation for below-aircraft light attenuation by vertical extrapolation, mostly fall within ±0.02 of AERONET ground-based measurements between 340–1640 nm for five overpass events.

HFC-152a and HFC-134a emission estimates and characterization of CFCs, CFC replacements, and other halogenated solvents measured during the 2008 ARCTAS campaign (CARB phase) over the South Coast Air Basin of California

Abstract. This work presents results from the NASA Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) study. Whole air samples were obtained on board research flights that flew over California during June 2008 and analyzed for selected volatile organic compounds, including several halogenated species. Samples collected over the South Coast Air Basin of California (SoCAB), which includes much of Los Angeles (LA) County, were compared with samples from inflow air masses over the Pacific Ocean. The levels of many halocarbon species were enhanced significantly over the SoCAB, including compounds regulated by the Montreal Protocol and subsequent amendments. Emissions estimates of HFC-152a (1,1-difluoroethane, CH3CHF2; 0.82 ± 0.11 Gg) and HFC-134a (1,1,1,2-tetrafluoroethane, CH2FCF3; 1.16 ± 0.22 Gg) in LA County for 2008 were obtained using the observed HFC:carbon monoxide (CO) enhancement ratio. Emission rates also were calculated for the SoCAB (1.60 ± 0.22 Gg yr−1 for HFC-152a and 2.12 ± 0.28 Gg yr−1 for HFC-134a) and then extrapolated to the United States (32 ± 4 Gg yr−1 for HFC-152a and 43 ± 6 Gg yr−1 for HFC-134a) using population data. In addition, emission rates of the two HFCs in LA County and SoCAB were calculated by a second method that utilizes air quality modeling. Emissions estimates obtained using both methods differ by less than 25% for the LA County and less than 45% for the SoCAB.

Seasonal variation of the transport of black carbon aerosol from the Asian continent to the Arctic during the ARCTAS aircraft campaign

[1] Extensive measurements of black carbon (BC) aerosol were conducted in and near the North American Arctic during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) aircraft campaign in April and June–July 2008. We identify the pathways and mechanisms of transport of BC to the Arctic from the Asian continent using these data. The concentration, transport efficiency, and measured altitude of BC over the North American Arctic were highly dependent on season and origin of air parcels, e.g., biomass burning (BB) in Russia (Russian BB) and anthropogenic (AN) in East Asia (Asian AN). Russian BB air was mainly measured in the middle troposphere and caused maximum BC concentrations at this altitude in spring. The median BC concentration and transport efficiency of the Russian BB air were 270 ng m−3 (at STP) and 80% in spring and 20 ng m−3 and 4% in summer, respectively. Asian AN air was measured most frequently in the upper troposphere, with median values of 20 ng m−3 and 13% in spring and 5 ng m−3 and 0.8% in summer. These distinct differences are explained by differences in the transport mechanisms and accumulated precipitation along trajectories (APT), which is a measure of wet removal processes during transport. The transport of Russian BB air to the Arctic was nearly isentropic with slow ascent (low APT), while Asian AN air underwent strong uplift associated with warm conveyor belts (high APT). The APT values in summer were much larger than those in spring due to the increase in humidity in summer. These results show that the impact of BC emitted from AN sources in East Asia on the Arctic was very limited in both spring and summer. The BB emissions in Russia in spring are demonstrated to be the most important sources of BC transported to the North American Arctic.

Characterizing summertime chemical boundary conditions for airmasses entering the US West Coast

Abstract. The objective of this study is to analyze the pollution inflow into California during summertime and how it impacts surface air quality through combined analysis of a suite of observations and global and regional models. The focus is on the transpacific pollution transport investigated by the NASA Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) mission in June 2008. Additional observations include satellite retrievals of carbon monoxide and ozone by the EOS Aura Tropospheric Emissions Spectrometer (TES), aircraft measurements from the MOZAIC program and ozonesondes. We compare chemical boundary conditions (BC) from the MOZART-4 global model, which are commonly used in regional simulations, with measured concentrations to quantify both the accuracy of the model results and the variability in pollution inflow. Both observations and model reflect a large variability in pollution inflow on temporal and spatial scales, but the global model captures only about half of the observed free tropospheric variability. Model tracer contributions show a large contribution from Asian emissions in the inflow. Recirculation of local US pollution can impact chemical BC, emphasizing the importance of consistency between the global model simulations used for BC and the regional model in terms of emissions, chemistry and transport. Aircraft measurements in the free troposphere over California show similar concentration ranges, variability and source contributions as free tropospheric air masses over ocean, but caution has to be taken that local pollution aloft is not misinterpreted as inflow. A flight route specifically designed to sample boundary conditions during ARCTAS-CARB showed a prevalence of plumes transported from Asia and thus may not be fully representative for average inflow conditions. Sensitivity simulations with a regional model with altered BCs show that the temporal variability in the pollution inflow does impact modeled surface concentrations in California. We suggest that time and space varying chemical boundary conditions from global models provide useful input to regional models, but likely still lead to an underestimate of peak surface concentrations and the variability associated with long-range pollution transport.

Validation of northern latitude Tropospheric Emission Spectrometer stare ozone profiles with ARC-IONS sondes during ARCTAS: sensitivity, bias and error analysis

Abstract. We compare Tropospheric Emission Spectrometer (TES) versions 3 and 4, V003 and V004, respectively, nadir-stare ozone profiles with ozonesonde profiles from the Arctic Intensive Ozonesonde Network Study (ARCIONS, http://croc.gsfc.nasa.gov/arcions/ during the Arctic Research on the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) field mission. The ozonesonde data are from launches timed to match Aura's overpass, where 11 coincidences spanned 44° N to 71° N from April to July 2008. Using the TES "stare" observation mode, 32 observations are taken over each coincidental ozonesonde launch. By effectively sampling the same air mass 32 times, comparisons are made between the empirically-calculated random errors to the expected random errors from measurement noise, temperature and interfering species, such as water. This study represents the first validation of high latitude (>70°) TES ozone. We find that the calculated errors are consistent with the actual errors with a similar vertical distribution that varies between 5% and 20% for V003 and V004 TES data. In general, TES ozone profiles are positively biased (by less than 15%) from the surface to the upper-troposphere (~1000 to 100 hPa) and negatively biased (by less than 20%) from the upper-troposphere to the lower-stratosphere (100 to 30 hPa) when compared to the ozonesonde data. Lastly, for V003 and V004 TES data between 44° N and 71° N there is variability in the mean biases (from −14 to +15%), mean theoretical errors (from 6 to 13%), and mean random errors (from 9 to 19%).

Bromine measurements in ozone depleted air over the Arctic Ocean

Abstract. In situ measurements of ozone, photochemically active bromine compounds, and other trace gases over the Arctic Ocean in April 2008 are used to examine the chemistry and geographical extent of ozone depletion in the arctic marine boundary layer (MBL). Data were obtained from the NOAA WP-3D aircraft during the Aerosol, Radiation, and Cloud Processes affecting Arctic Climate (ARCPAC) study and the NASA DC-8 aircraft during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) study. Fast (1 s) and sensitive (detection limits at the low pptv level) measurements of BrCl and BrO were obtained from three different chemical ionization mass spectrometer (CIMS) instruments, and soluble bromide was measured with a mist chamber. The CIMS instruments also detected Br2. Subsequent laboratory studies showed that HOBr rapidly converts to Br2 on the Teflon instrument inlets. This detected Br2 is identified as active bromine and represents a lower limit of the sum HOBr + Br2. The measured active bromine is shown to likely be HOBr during daytime flights in the arctic. In the MBL over the Arctic Ocean, soluble bromide and active bromine were consistently elevated and ozone was depleted. Ozone depletion and active bromine enhancement were confined to the MBL that was capped by a temperature inversion at 200–500 m altitude. In ozone-depleted air, BrO rarely exceeded 10 pptv and was always substantially lower than soluble bromide that was as high as 40 pptv. BrCl was rarely enhanced above the 2 pptv detection limit, either in the MBL, over Alaska, or in the arctic free troposphere.

The Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) mission: design, execution, and first results

Abstract. The NASA Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) mission was conducted in two 3-week deployments based in Alaska (April 2008) and western Canada (June–July 2008). Its goal was to better understand the factors driving current changes in Arctic atmospheric composition and climate, including (1) influx of mid-latitude pollution, (2) boreal forest fires, (3) aerosol radiative forcing, and (4) chemical processes. The June–July deployment was preceded by one week of flights over California (ARCTAS-CARB) focused on (1) improving state emission inventories for greenhouse gases and aerosols, (2) providing observations to test and improve models of ozone and aerosol pollution. ARCTAS involved three aircraft: a DC-8 with a detailed chemical payload, a P-3 with an extensive aerosol and radiometric payload, and a B-200 with aerosol remote sensing instrumentation. The aircraft data augmented satellite observations of Arctic atmospheric composition, in particular from the NASA A-Train. The spring phase (ARCTAS-A) revealed pervasive Asian pollution throughout the Arctic as well as significant European pollution below 2 km. Unusually large Siberian fires in April 2008 caused high concentrations of carbonaceous aerosols and also affected ozone. Satellite observations of BrO column hotspots were found not to be related to Arctic boundary layer events but instead to tropopause depressions, suggesting the presence of elevated inorganic bromine (5–10 pptv) in the lower stratosphere. Fresh fire plumes from Canada and California sampled during the summer phase (ARCTAS-B) indicated low NOx emission factors from the fires, rapid conversion of NOx to PAN, no significant secondary aerosol production, and no significant ozone enhancements except when mixed with urban pollution.

Analysis of snow bidirectional reflectance from ARCTAS Spring-2008 Campaign

Abstract. The spring 2008 Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) experiment was one of major intensive field campaigns of the International Polar Year aimed at detailed characterization of atmospheric physical and chemical processes in the Arctic region. A part of this campaign was a unique snow bidirectional reflectance experiment on the NASA P-3B aircraft conducted on 7 and 15 April by the Cloud Absorption Radiometer (CAR) jointly with airborne Ames Airborne Tracking Sunphotometer (AATS) and ground-based Aerosol Robotic Network (AERONET) sunphotometers. The CAR data were atmospherically corrected to derive snow bidirectional reflectance at high 1° angular resolution in view zenith and azimuthal angles along with surface albedo. The derived albedo was generally in good agreement with ground albedo measurements collected on 15 April. The CAR snow bidirectional reflectance factor (BRF) was used to study the accuracy of analytical Ross-Thick Li-Sparse (RTLS), Modified Rahman-Pinty-Verstraete (MRPV) and Asymptotic Analytical Radiative Transfer (AART) BRF models. Except for the glint region (azimuthal angles φ<40°), the best fit MRPV and RTLS models fit snow BRF to within ±0.05. The plane-parallel radiative transfer (PPRT) solution was also analyzed with the models of spheres, spheroids, randomly oriented fractal crystals, and with a synthetic phase function. The latter merged the model of spheroids for the forward scattering angles with the fractal model in the backscattering direction. The PPRT solution with synthetic phase function provided the best fit to measured BRF in the full range of angles. Regardless of the snow grain shape, the PPRT model significantly over-/underestimated snow BRF in the glint/backscattering regions, respectively, which agrees with other studies. To improve agreement with experiment, we introduced a model of macroscopic snow surface roughness by averaging the PPRT solution over the slope distribution function and by adding a simple model of shadows. With macroscopic roughness described by two parameters, the AART model achieved an accuracy of about ±0.05 with a possible bias of ±0.03 in the spectral range 0.4–2.2 μm. This high accuracy holds at view zenith angles below 55–60° covering the practically important range for remote sensing applications, and includes both glint and backscattering directions.

Arctic mercury depletion and its quantitative link with halogens

Gas phase elemental mercury (Hg°) was measured aboard the NASA DC-8 research aircraft during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign conducted in spring 2008 primarily over the North American Arctic. We examined the vertical distributions of Hg° and ozone (O3) together with tetrachloroethylene (C2Cl4), ethyne (C2H2), and alkanes when Hg°- and O3-depleted air masses were sampled near the surface (<1 km). This study suggests that Hg° and O3 depletions commonly occur over linear distances of ~20–200 km. Horizontally there was a sharp decreasing gradient of ~100 ppqv in Hg° over <10 km in going from the bay near Ellesmere Island to the frozen open ocean. There was a distinct land-ocean difference in the vertical thickness of the Hg°-depleted layer – being variable but around a few 100 meters over the ocean whereas occurring only very near the surface over land. Data support that atmospheric mercury depletion events are driven by Hg° reactions with halogen atoms. Derived from data collected aboard the DC-8, we present mathematical expressions giving the rates of Hg° and O3 depletions as a function of the radical concentrations. These relationships can be a useful metric to evaluate models that attempt to reproduce springtime Arctic Hg° and/or O3 depletion events, and they can also be employed to obtain order-of-magnitude estimates of radical concentrations and the ratio [Br]/[Cl].

Simultaneous retrieval of aerosol and surface optical properties from combined airborne- and ground-based direct and diffuse radiometric measurements

Abstract. This paper presents a new method for simultaneously retrieving aerosol and surface reflectance properties from combined airborne and ground-based direct and diffuse radiometric measurements. The method is based on the standard Aerosol Robotic Network (AERONET) method for retrieving aerosol size distribution, complex index of refraction, and single scattering albedo, but modified to retrieve aerosol properties in two layers, below and above the aircraft, and parameters on surface optical properties from combined datasets (Cloud Absorption Radiometer (CAR) and AERONET data). A key advantage of this method is the inversion of all available spectral and angular data at the same time, while accounting for the influence of noise in the inversion procedure using statistical optimization. The wide spectral (0.34–2.30 μm) and angular range (180°) of the CAR instrument, combined with observations from an AERONET sunphotometer, provide sufficient measurement constraints for characterizing aerosol and surface properties with minimal assumptions. The robustness of the method was tested on observations made during four different field campaigns: (a) the Southern African Regional Science Initiative 2000 over Mongu, Zambia, (b) the Intercontinental Transport Experiment-Phase B over Mexico City, Mexico (c) Cloud and Land Surface Interaction Campaign over the Atmospheric Radiation Measurement (ARM) Central Facility, Oklahoma, USA, and (d) the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) over Elson Lagoon in Barrow, Alaska, USA. The four areas are dominated by different surface characteristics and aerosol types, and therefore provide good test cases for the new inversion method.

A meteorological overview of the ARCTAS 2008 mission

Abstract. The Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) mission was a multi-aircraft project whose major objective was to investigate the factors driving changes in the Arctic's atmospheric composition and climate. It was conducted during April and June–July 2008. The summer ARCTAS deployment was preceded by a week of flights over and around California to address state issues of air quality and climate forcing. This paper focuses on meteorological conditions during the ARCTAS Spring and Summer campaigns. We examine mission averaged large-scale flow patterns at the surface, 500 hPa, and 300 hPa and determine their departures from climatology. Results from runs of the Weather Research and Forecasting (WRF) model are used to describe meteorological conditions on individual days. Our WRF configuration included a nested grid approach that provided horizontal spacing as small as 5 km. Trajectories calculated from the WRF output are used to determine transport pathways to the Arctic, including their origins and the altitudes at which they reach 70° N. We also present backward trajectories from selected legs of individual ARCTAS flights. Finally, the FLEXPART Lagrangian particle dispersion model, with the high resolution WRF data as input, is used to determine the paths of anthropogenic and biomass burning-derived CO. Results show that there was frequent and widespread transport to the Arctic during both phases of ARCTAS and that the three ARCTAS aircraft sampled air having a multitude of origins, following a myriad of paths, and experiencing many types of meteorological conditions.