[1] We report summertime measurements of CO and O 3 obtained during 2001-2003 at the PICO-NARE mountaintop station in the Azores. Frequent events of elevated CO mixing ratios were observed. On the basis of backward trajectories arriving in the free troposphere and global simulations of biomass burning plumes, we attribute nearly all these events to North American pollution outflow and long-range transport of biomass burning emissions. There was a high degree of interannual variability in CO levels: median [CO] ranged from 65 ppbv in 2001 to 104 ppbv in 2003. The highest concentrations were associated with transport of Siberian fire emissions during summer 2003, when Siberian fire activity was unusually high. Ozone mixing ratios also increased (by up to $30 ppbv) during the fire events. These findings demonstrate the significant hemispheric scale impact that biomass burning events have on background CO and O 3 levels. O 3 enhancements of similar magnitude were also observed in North American pollution outflow. O 3 and CO were correlated during North American outflow events, with a slope averaging 1., ppbv/ppbv) when no fire impact was present. This slope is more than 80% larger than early 1990s observations made in the eastern United States and nearshore outflow region, even after accounting for declining U.S. CO emissions and for CO loss during transport to the Azores, and is not consistent with simple dilution of U.S. outflow with marine background air. We conclude that a significantly larger amount of O 3 production occurred in the air sampled during this study, and we suggest several potential reasons for this, each of which could imply potentially significant shortcomings in current estimates of the hemispheric impact of North American emissions on tropospheric ozone and should be evaluated in future studies.

Abstract. The Maritime Aerosol Network (MAN) has been collecting data over the oceans since November 2006. Over 80 cruises were completed through early 2010 with deployments continuing. Measurement areas included various parts of the Atlantic Ocean, the Northern and Southern Pacific Ocean, the South Indian Ocean, the Southern Ocean, the Arctic Ocean and inland seas. MAN deploys Microtops handheld sunphotometers and utilizes a calibration procedure and data processing traceable to AERONET. Data collection included areas that previously had no aerosol optical depth (AOD) coverage at all, particularly vast areas of the Southern Ocean. The MAN data archive provides a valuable resource for aerosol studies in maritime environments. In the current paper we present results of AOD measurements over the oceans, and make a comparison with satellite AOD retrievals and model simulations.

Summertime observations of O3 and CO made at the PICO‐NARE station during 2001, 2003, and 2004 are used to assess the impact of boreal forest fires on the distribution of O3 mixing ratios in the midlatitude Northern Hemisphere (NH) lower free troposphere (FT). Backward trajectories were used to select measurements impacted by outflow from high‐latitude regions. Measurements during these periods were segregated into two subsets: those obtained during periods with and without apparent significant upwind fire emissions. Periods affected by fire emissions were identified based on enhanced CO levels confirmed by global simulations of fire emissions transport. During fire‐impacted periods, O3 was shifted toward higher mixing ratios, with medians significantly higher than in periods without detectable upwind fire impacts. This implies a significant impact of boreal wildfires on midlatitude lower FT background O3 during summer. Predicted future increases in boreal wildfires may therefore affect summertime O3 levels over large regions.

[1] W126 is a cumulative ozone exposure index based on sigmoidally weighted daytime ozone concentrations used to evaluate the impacts of ozone on vegetation. We quantify W126 in the U.S. in the absence of North American anthropogenic emissions (North American background or "NAB") using three regional or global chemical transport models for May-July 2010. All models overestimate W126 in the eastern U.S. due to a persistent bias in daytime ozone, while the models are relatively unbiased in California and the Intermountain West. Substantial difference in the magnitude and spatial and temporal variability of the estimates of W126 NAB between models supports the need for a multimodel approach. While the average NAB contribution to daytime ozone in the Intermountain West is 64-78%, the average W126 NAB is only 9-27% of current levels, owing to the weight given to high O 3 concentrations in W126. Based on a three-model mean, NAB explains 30% of the daily variability in the W126 daily index in the Intermountain West. Adjoint sensitivity analysis shows that nationwide W126 is influenced most by NO x emissions from anthropogenic (58% of the total sensitivity) and natural (25%) sources followed by nonmethane volatile organic compounds (10%) and CO (7%). Most of the influence of anthropogenic NO x comes from the U.S. (80%), followed by Canada (9%), Mexico (4%), and China (3%). Thus, long-range transport of pollution has a relatively small impact on W126 in the U.S., and domestic emissions control should be effective for reducing W126 levels.

Abstract. Aerosol loading in the marine environment is investigated using aerosol composition measurements from several research ship campaigns (ICEALOT, MAP, RHaMBLe, VOCALS and OOMPH), observations of total AOD column from satellite (MODIS) and ship-based instruments (Maritime Aerosol Network, MAN), and a global chemical transport model (GEOS-Chem). This work represents the most comprehensive evaluation of oceanic OM emission inventories to date, by employing aerosol composition measurements obtained from campaigns with wide spatial and temporal coverage. The model underestimates AOD over the remote ocean on average by 0.02 (21 %), compared to satellite observations, but provides an unbiased simulation of ground-based Maritime Aerosol Network (MAN) observations. Comparison with cruise data demonstrates that the GEOS-Chem simulation of marine sulfate, with the mean observed values ranging between 0.22 µg m −3 and 1.34 µg m −3 , is generally unbiased, however surface organic matter (OM) concentrations, with the mean observed concentrations between 0.07 µg m −3 and 0.77 µg m −3 , are underestimated by a factor of 2-5 for the standard model run. Addition of a sub-micron marine OM source of approximately 9 TgC yr −1 brings the model into agreement with the ship-based measurements, however this additional OM source does not exCorrespondence to: K. Lapina (klapina@atmos.colostate.edu) plain the model underestimate of marine AOD. The model underestimate of marine AOD is therefore likely the result of a combination of satellite retrieval bias and a missing marine aerosol source (which exhibits a different spatial pattern than existing aerosol in the model).