Transpacific Transport of Ozone Pollution and the Effect of Recent Asian Emission Increases on Air Quality in North America: An Integrated Analysis Using Satellite, Aircraft, Ozonesonde, and Surface Observations

We use an ensemble of aircraft, satellite, sonde, and surface observations for April–May 2006 (NASA/INTEX-B aircraft campaign) to better understand the mechanisms for transpacific ozone pollution and its implications for North American air quality. The observations are interpreted with a global 3-D chemical transport model (GEOS-Chem). OMI NO2 satellite observations constrain Asian anthropogenic NOx emissions and indicate a factor of 2 increase from 2000 to 2006 in China. Satellite observations of CO from AIRS and TES indicate two major events of Asian transpacific pollution during INTEX-B. Correlation between TES CO and ozone observations shows evidence for transpacific ozone pollution. The semi-permanent Pacific High and Aleutian Low cause splitting of transpacific pollution plumes over the Northeast Pacific. The northern branch circulates around the Aleutian Low and has little impact on North America. The southern branch circulates around the Pacific High and some of that air impacts western North America. Both aircraft measurements and model results show sustained ozone production driven by peroxyacetylnitrate (PAN) decomposition in the southern branch, roughly doubling the transpacific influence from ozone produced in the Asian boundary layer. Model simulation of ozone observations at Mt. Bachelor Observatory in Oregon (2.7 km altitude) indicates a mean Asian ozone pollution contribution of 9±3 ppbv to the mean observed concentration of 54 ppbv, reflecting mostly an enhancement in background ozone rather than episodic Asian plumes. Asian pollution enhanced surface ozone concentrations by 5–7 ppbv over western North America in spring 2006. The 2000–2006 rise in Asian anthropogenic emissions increased this influence by 1–2 ppbv.Earth and Planetary SciencesEngineering and Applied Science

Nitrate stable isotopes and major ions in snow and ice samples from four Svalbard sites

Increasing reactive nitrogen (N-r) deposition in the Arctic may adversely impact N-limited ecosystems. To investigate atmospheric transport of N-r to Svalbard, Norwegian Arctic, snow and firn samples were collected from glaciers and analysed to define spatial and temporal variations (1 10 years) in major ion concentrations and the stable isotope composition (delta N-15 and delta O-18) of nitrate (NO3-) across the archipelago. The delta N-15(NO3-) and delta O-18(NO3-) averaged -4 parts per thousand and 67 parts per thousand in seasonal snow (2010-11) and -9 parts per thousand and 74 parts per thousand in firn accumulated over the decade 2001-2011. East-west zonal gradients were observed across the archipelago for some major ions (non-sea salt sulphate and magnesium) and also for delta N-15(NO3-) and delta O-18(NO3-) in snow, which suggests a different origin for air masses arriving in different sectors of Svalbard. We propose that snowfall associated with long-distance air mass transport over the Arctic Ocean inherits relatively low delta N-15(NO3-) due to in-transport N isotope fractionation. In contrast, faster air mass transport from the north-west Atlantic or northern Europe results in snowfall with higher delta N-15(NO3-) because in-transport fractionation of N is then time-limited

The Carrington event not observed in most ice core nitrate records

The Carrington Event of 1859 is considered to be among the largest space weather events of the last 150 years. We show that only one out of 14 well-resolved ice core records from Greenland and Antarctica has a nitrate spike dated to 1859. No sharp spikes are observed in the Antarctic cores studied here. In Greenland numerous spikes are observed in the 40 years surrounding 1859, but where other chemistry was measured, all large spikes have the unequivocal signal, including co-located spikes in ammonium, formate, black carbon and vanillic acid, of biomass burning plumes. It seems certain that most spikes in an earlier core, including that claimed for 1859, are also due to biomass burning plumes, and not to solar energetic particle (SEP) events. We conclude that an event as large as the Carrington Event did not leave an observable, widespread imprint in nitrate in polar ice. Nitrate spikes cannot be used to derive the statistics of SEPs

Observations of hydroxyl and peroxy radicals and the impact of Br0 at Summit, Greenland in 2007 and 2008

The Greenland Summit Halogen-HO(x) (GSHOX) Campaign was performed in spring 2007 and summer 2008 to investigate the impact of halogens on HO(x) (= OH+HO(2)) cycling above the Greenland Ice Sheet. Chemical species including hydroxyl and peroxy radicals (OH and HO(2) + RO(2)), ozone (O(3)), nitrogen oxide (NO), nitric acid (HNO(3)), nitrous acid (HONO), reactive gaseous mercury (RGM), and bromine oxide (BrO) were measured during the campaign. The median midday values of HO(2) + RO(2) and OH concentrations observed by chemical ionization mass spectrometry (CIMS) were 2.7x10(8) molec cm(-3) and 3.0x10(6) molec cm(-3) in spring 2007, and 4.2x10(8) molec cm(-3) and 4.1x10(6) molec cm(-3) in summer 2008. A basic photochemical 0-D box model highly constrained by observations of H(2)O, O(3), CO, CH(4), NO, and J values predicted HO(2) + RO(2) (R = 0.90, slope = 0.87 in 2007; R = 0.79, slope = 0.96 in 2008) reasonably well and under predicted OH (R = 0.83, slope = 0.72 in 2007; R = 0.76, slope = 0.54 in 2008). Constraining the model to HONO observations did not significantly improve the ratio of OH to HO(2) + RO(2) and the correlation between predictions and observations. Including bromine chemistry in the model constrained by observations of BrO improved the correlation between observed and predicted HO(2) + RO(2) and OH, and brought the average hourly OH and HO(2) + RO(2) predictions closer to the observations. These model comparisons confirmed our understanding of the dominant HO(x) sources and sinks in this environment and indicated that BrO impacted the OH levels at Summit. Although, significant discrepancies between observed and predicted OH could not be explained by the measured BrO. Finally, observations of enhanced RGM were found to be coincident with under prediction of OH

Observations of hydroxyl and the sum of peroxy radicals at Summit, Greenland during summer 2003

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

Chemical constituents in the air and snow at Dye 3, Greenland—II. Analysis of episodes in April 1989

International audienc

Chemical constituents in the air and snow at Dye 3, Greenland—I. Seasonal variations

International audienc