ALBERT

Description: We used a 3-D model of chemistry and transport to investigate trends and variability in tropospheric carbon monoxide (CO) for 1988–1997 caused by changes in the overhead ozone column, fossil fuel emissions, biomass burning emissions, methane, and transport. We found that the decreasing CO burden in the northern extra-tropics (−0.85%/y) was more heavily influenced by the decrease in European emissions during our study period than by the similar increase in Asian emissions, as transport pathways from Europe favored accumulation at higher latitudes in winter and spring. However, the opposite trends in the CO burdens from these two source regions counterbalanced at lower latitudes. Elsewhere, the factors influencing CO often compete, diminishing their cumulative impact, and trends in model CO were small or insignificant for our study period, except in the tropics in boreal fall (1.1%/y), a result of emissions from major fires in Indonesia late in 1997. There was a decrease in the ozone column during the study period as a result of the phase of the solar cycle and the eruption of Pinatubo in 1991. This decrease contributed negatively to the trend in model CO by increasing the hydroxyl radical (OH). The impact of this negative contribution was diminished by a positive contribution of similar magnitude from increasing methane. However, the trends in these two factors did not cancel for tropospheric OH, which responded primarily to changes in the ozone column.

Description: We examine the response of Arctic gas and aerosol concentrations to perturbations in pollutant emissions from Europe, East and South Asia, and North America using results from a coordinated model intercomparison. These sensitivities to regional emissions (mixing ratio change per unit emission) vary widely across models and species. Intermodel differences are systematic, however, so that the relative importance of different regions is robust. North America contributes the most to Arctic ozone pollution. For aerosols and CO, European emissions dominate at the Arctic surface but Asian emissions become progressively more important with altitude, and are dominant in the upper troposphere. Sensitivities show strong seasonality: surface sensitivities typically maximize during boreal winter for European and during spring for East Asian and North American emissions. Mid-tropospheric sensitivities, however, nearly always maximize during spring or summer for all regions. Deposition of black carbon (BC) onto Greenland is most sensitive to North American emissions. North America and Europe each contribute ~40% of total BC deposition to Greenland, with ~20% from East Asia. Elsewhere in the Arctic, both sensitivity and total BC deposition are dominated by European emissions. Model diversity for aerosols is especially large, resulting primarily from differences in aerosol physics and removal. Comparison of aerosols with observations indicates problems in either the models or interpretation of the measurements. For gas phase pollutants such as CO and O3, which are relatively well-simulated, the processes contributing most to uncertainties depend on the source region. Uncertainties in the Arctic surface CO response to emissions perturbations are dominated by emissions for East Asian sources, while uncertainties in transport, emissions, and oxidation are comparable for European and North American sources. At higher levels, model-to-model variations in transport and oxidation are most important. Differences in photochemistry appear to play the largest role in the intermodel variations in Arctic ozone sensitivity.

Description: We present a modeling study of the long-range transport of pollution from Europe, showing that European emissions regularly elevate surface ozone by as much as 20 ppbv in summer in northern Africa and the Near East. European emissions cause 50–150 additional violations per year (i.e., above those that would occur without European pollution) of the European health standard for ozone (8-h average 〉120 μg/m3 or ~60 ppbv) in northern Africa and the Near East. We estimate that 19 000 additional mortalities occur annually in these regions from exposure to European ozone pollution and 50 000 additional deaths globally; the majority of the additional deaths occurs outside of Europe. Much of the pollution from Europe is exported southward at low altitudes in summer to the Mediterranean Sea, northern Africa and the Near East, regions with favorable photochemical environments for ozone production. Our results suggest that assessments of the human health benefits of reducing ozone precursor emissions in Europe should include effects outside of Europe, and that comprehensive planning to improve air quality in northern Africa and the Near East likely needs to address European emissions. We also show that the tropospheric ozone column data product derived from the OMI and MLS instruments is currently of limited value for air quality applications as the portion of the column above the boundary layer and below the tropopause is large and variable, effectively obscuring the boundary layer signal.

Description: Stratospheric intrusions have been the interest of decades of research for their ability to bring stratospheric ozone (O3) into the troposphere with the potential to enhance surface O3 concentrations. However, these intrusions have been misrepresented in models and reanalyses until recently, as the features of a stratospheric intrusion are best identified in horizontal resolutions of 50 km or smaller. NASA's Modern-Era Retrospective Analysis for Research and Applications Version-2 (MERRA-2) reanalysis is a publicly available high-resolution data set (∼50 km) with assimilated O3 that characterizes O3 on the same spatiotemporal resolution as the meteorology. We demonstrate the science capabilities of the MERRA-2 reanalysis when applied to the evaluation of stratospheric intrusions that impact surface air quality. This is demonstrated through a case study analysis of stratospheric intrusion-influenced O3 exceedances in spring 2012 in Colorado, using a combination of observations, the MERRA-2 reanalysis and Goddard Earth Observing System Model, Version 5 simulations. ©2017. American Geophysical Union. All Rights Reserved. This article has been contributed to by US Government employees and their work is in the public domain in the USA.

Description: We present a modeling study of the troposphere-to-stratosphere transport (TST) of pollution from major biomass burning regions to the tropical upper troposphere and lower stratosphere (UT/LS). TST occurs predominately through 1) slow ascent in the tropical tropopause layer (TTL) to the LS and 2) quasi-horizontal exchange to the lowermost stratosphere (LMS). We show that biomass burning pollution regularly and significantly impacts the composition of the TTL, LS, and LMS. Carbon monoxide (CO) in the LS in our simulation and data from the Aura Microwave Limb Sounder (MLS) shows an annual oscillation in its composition that results from the interaction of an annual oscillation in slow ascent from the TTL to the LS and seasonal variations in sources, including a semi-annual oscillation in CO from biomass burning. The impacts of CO sources that peak when ascent is seasonally low are damped (e.g. Southern Hemisphere biomass burning) and vice-versa for sources that peak when ascent is seasonally high (e.g. extra-tropical fossil fuels). Interannual variation of CO in the UT/LS is caused primarily by year-to-year variations in biomass burning and the locations of deep convection. During our study period, 1994–1998, we find that the highest concentrations of CO in the UT/LS occurred during the strong 1997–1998 El Niño event for two reasons: i. tropical deep convection shifted to the eastern Pacific Ocean, closer to South American and African CO sources, and ii. emissions from Indonesian biomass burning were higher. This extreme event can be seen as an upper bound on the impact of biomass burning pollution on the UT/LS. We estimate that the 1997 Indonesian wildfires increased CO in the entire TTL and tropical LS (〉60 mb) by more than 40% and 10%, respectively, for several months. Zonal mean ozone increased and the hydroxyl radical decreased by as much as 20%, increasing the lifetimes and, subsequently TST, of trace gases. Our results indicate that the impact of biomass burning pollution on the UT/LS is likely greatest during an El Niño event due to favorable dynamics and historically higher burning rates.

Description: We present a modeling study of the long-range transport of pollution from Europe, showing that European emissions regularly elevate surface ozone by as much as 20 ppbv in summer in northern Africa and the Near East. European emissions cause 50–150 additional violations per year (i.e. above those that would occur without European pollution) of the European health standard for ozone (8-h average 〉120 μg/m3 or ~60 ppbv) in northern Africa and the Near East. We estimate that European ozone pollution is responsible for 50 000 premature mortalities globally each year, of which the majority occurs outside of Europe itself, including 37% (19 000) in northern Africa and the Near East. Much of the pollution from Europe is exported southward at low altitudes in summer to the Mediterranean Sea, northern Africa and the Near East, regions with favorable photochemical environments for ozone production. Our results suggest that assessments of the human health benefits of reducing ozone precursor emissions in Europe should include effects outside of Europe, and that comprehensive planning to improve air quality in northern Africa and the Near East likely needs to address European emissions.

Description: We used the seasonality of a combination of atmospheric trace gases and idealized tracers to examine stratosphere-to-troposphere transport and its influence on tropospheric composition in the Arctic. Maximum stratosphere-to-troposphere transport of CFCs and O3 occurs in April as driven by the Brewer-Dobson circulation. Stratosphere-troposphere exchange (STE) occurs predominantly between 40° N to 80° N with stratospheric influx in the mid-latitudes (30–70° N) accounting for 67–81% of the air of stratospheric origin in the Northern Hemisphere extratropical troposphere. Transport from the lower stratosphere to the lower troposphere (LT) takes three months on average, one month to cross the tropopause, the second month to travel from the upper troposphere (UT) to the middle troposphere (MT), and the third month to reach the LT. During downward transport, the seasonality of a trace gas can be greatly impacted by wet removal and chemistry. A comparison of idealized tracers with varying lifetimes suggests that when initialized with the same concentrations and seasonal cycles at the tropopause, trace gases that have shorter lifetimes display lower concentrations, smaller amplitudes, and earlier seasonal maxima during transport to the LT. STE contributes to O3 in the Arctic troposphere directly from the transport of O3 and indirectly from the transport of NOy. Direct transport of O3 from the stratosphere accounts for 78% of O3 in the Arctic UT with maximum contributions occurring from March to May. The stratospheric contribution decreases significantly in the MT/LT (20–25% of total O3) and shows a very weak March–April maximum. Our NOx budget analysis in the Arctic UT shows that during spring and summer, the stratospheric injection of NOy-rich air increases NOx concentrations above the 20 pptv threshold level, thereby shifting the Arctic UT from a regime of net photochemical ozone loss to one of net production with rates as high as +16 ppbv/month.

Description: Wildfires raged throughout western Russia and parts of Eastern Europe during a persistent heat wave in the summer of 2010. Anomalously high surface temperatures (35–41 °C) and low relative humidity (9–25 %) from mid-June to mid-August 2010 shown by analysis of radiosonde data from multiple sites in western Russia were ideal conditions for the wildfires to thrive. Measurements of outgoing longwave radiation (OLR) from the Atmospheric Infrared Sounder (AIRS) over western Russian indicate persistent subsidence during the heat wave. Daily three-day back-trajectories initiated over Moscow reveal a persistent anti-cyclonic circulation for 18 days in August, coincident with the most intense period of fire activity observed by Moderate Resolution Imaging Spectroradiometer (MODIS). This unfortunate meteorological coincidence allowed transport of polluted air from the region of intense fires to Moscow and the surrounding area. We demonstrate that the 2010 Russian wildfires are unique in the record of observations obtained by remote-sensing instruments on-board NASA satellites: Aura and Aqua (part of the A-Train Constellation) and Terra. Analysis of the distribution of MODIS fire products and aerosol optical thickness (AOT), UV aerosol index (AI) and single-scattering albedo (SSA) from Aura's Ozone Monitoring Instrument (OMI), and total column carbon monoxide (CO) from Aqua's Atmospheric Infrared Sounder (AIRS) show that the region in the center of western Russia surrounding Moscow (52°–58° N, 33°–43° E) is most severely impacted by wildfire emissions. Over this area, AIRS CO, OMI AI, and MODIS AOT are significantly enhanced relative to the historical satellite record during the first 18 days in August when the anti-cyclonic circulation persisted. By mid-August, the anti-cyclonic circulation was replaced with westerly transport over Moscow and vicinity. The heat wave ended as anomalies of surface temperature and relative humidity, and OLR disappeared. After 18 August the fire activity greatly diminished over western Russia and levels of the satellite smoke tracers returned to values typical of previous years.

Description: We use aircraft observations obtained during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) mission to examine the distributions and source attributions of O3 and NOy in the Arctic and sub-Arctic region. Using a number of marker tracers, we distinguish various air masses from the background troposphere and examine their contributions to NOx, O3, and O3 production in the Arctic troposphere. The background Arctic troposphere has a mean O3 of ~60 ppbv and NOx of ~25 pptv throughout spring and summer with CO decreasing from ~145 ppbv in spring to ~100 ppbv in summer. These observed mixing ratios are not notably different from the values measured during the 1988 ABLE-3A and the 2002 TOPSE field campaigns despite the significant changes in emissions and stratospheric ozone layer in the past two decades that influence Arctic tropospheric composition. Air masses associated with stratosphere-troposphere exchange are present throughout the mid and upper troposphere during spring and summer. These air masses, with mean O3 concentrations of 140–160 ppbv, are significant direct sources of O3 in the Arctic troposphere. In addition, air of stratospheric origin displays net O3 formation in the Arctic due to its sustainable, high NOx (75 pptv in spring and 110 pptv in summer) and NOy (~800 pptv in spring and ~1100 pptv in summer). The air masses influenced by the stratosphere sampled during ARCTAS-B also show conversion of HNO3 to PAN. This active production of PAN is the result of increased degradation of ethane in the stratosphere-troposphere mixed air mass to form CH3CHO, followed by subsequent formation of PAN under high NOx conditions. These findings imply that an adequate representation of stratospheric NOy input, in addition to stratospheric O3 influx, is essential to accurately simulate tropospheric Arctic O3, NOx and PAN in chemistry transport models. Plumes influenced by recent anthropogenic and biomass burning emissions observed during ARCTAS show highly elevated levels of hydrocarbons and NOy (mostly in the form of NOx and PAN), but do not contain O3 higher than that in the Arctic tropospheric background except some aged biomass burning plumes sampled during spring. Convection and/or lightning influences are negligible sources of O3 in the Arctic troposphere but can have significant impacts in the upper troposphere in the continental sub-Arctic during summer.