Abstract. Aerosol measurements at Barrow, Alaska during the past 30 years have identified the long range transport of pollution associated with Arctic Haze as well as ocean-derived aerosols of more local origin. Here, we focus on measurements of aerosol chemical composition to assess (1) trends in Arctic Haze aerosol and implications for source regions, (2) the interaction between pollution-derived and ocean-derived aerosols and the resulting impacts on the chemistry of the Arctic boundary layer, and (3) the response of aerosols to a changing climate. Aerosol chemical composition measured at Barrow, AK during the Arctic haze season is compared for the years 1976-1977 and 1997-2008. Based on these two data sets, concentrations of non-sea salt (nss) sulfate (SO = 4 ) and non-crustal (nc) vanadium (V) have decreased by about 60% over this 30 year period. Consistency in the ratios of nss SO = 4 /ncV and nc manganese (Mn)/ncV between the two data sets indicates that, although emissions have decreased in the source regions, the source regions have remained the same over this time period. The measurements from 1997-2008 indicate that, during the haze season, the nss SO = 4 aerosol at Barrow is becoming less neutralized by ammonium (NH + 4 ) yielding an increasing sea salt aerosol chloride (Cl − ) deficit. The expected consequence is an increase in the release of Cl atoms to the atmosphere and a change in the lifetime of volatile organic compounds (VOCs) including methane. In addition, summertime concentrations of biogenically-derived methanesulfonate (MSA − ) andCorrespondence to: P. K. Quinn (patricia.k.quinn@noaa.gov) nss SO = 4 are increasing at a rate of 12 and 8% per year, respectively. Further research is required to assess the environmental factors behind the increasing concentrations of biogenic aerosol.

[1] The air quality and climate forcing impacts of atmospheric aerosols in a metropolitan region depend on the amount, composition, and size of the aerosol transported into the region; the input and removal of aerosols and aerosol precursors within the region; and the subsequent chemical processing in the atmosphere. These factors were studied in the Houston-Galveston-Gulf of Mexico region, aboard the NOAA R/V Ronald H. Brown during the Texas Air Quality Study and Gulf of Mexico Atmospheric Composition and Climate Study (TexAQS/GoMACCS 2006). The aerosol measured in the Gulf of Mexico during onshore flow (low radon concentrations indicating no contact with land for several days) was highly impacted by Saharan dust and what appear to be ship emissions (acidic sulfate and nitrate). Mean (median) mass concentrations of the total submicrometer and supermicrometer aerosol were 6.5 (4.6) mg m À3 and 17.2 (8.7) mg m À3 , respectively. These mass loadings of ''background'' aerosol are much higher than typically observed in the marine atmosphere and thus have a substantial impact on the radiative energy balance over the Gulf of Mexico and particulate matter (PM) loadings (air quality) in the Houston-Galveston area. As this background aerosol moved onshore, local urban and industrial sources added an organic rich submicrometer component (66% particulate organic matter (POM), 20% sulfate, 14% elemental carbon) but no significant supermicrometer aerosol. The resulting aerosol had mean (median) mass concentrations of the total submicrometer and supermicrometer aerosol of 10.0 (9.1) mg m À3 and 16.8 (11.2) mg m À3 , respectively. These air masses, with minimal processing of urban emissions contained the highest SO 2 /(SO 2 + SO 4 = ) ratios and the highest hydrocarbon-like organic aerosol to total organic aerosol ratios (HOA/POM). In contrast, during periods of offshore flow, the aerosol was more processed and, therefore, much richer in oxygenated organic aerosol (OOA). Mean (median) mass concentrations of the total submicrometer and supermicrometer aerosol were 20.8 (18.6) mg m À3 and 7.4 (5.0) mg m À3 , respectively. Sorting air masses based on their trajectories and time over land provides a means to examine the effects of transport and subsequent chemical processing. Understanding and parameterizing these processes is critical for the chemical transport modeling that forms the basis for air quality forecasts and radiative forcing calculations.

The chemical, physical, and optical properties of sub‐ and supermicrometer aerosols over the equatorial Indian Ocean were measured on board the R/V Revelle during the fall 2011 Dynamics of the Madden‐Julian Oscillation field campaign. During this time, both the retreating of the Asian monsoon and two Madden‐Julian Oscillation (MJO) events were observed. The R/V Revelle was on station (0.1°N and 80.5°E) to measure atmospheric and oceanic conditions between 4 October and 30 October 2011 (Leg 2) and 11 November and 4 December 2011 (Leg 3). Throughout the campaign, background marine atmospheric conditions were usually observed. As the Asian monsoon season retreated over the boreal fall and the general wind direction changed from southerly to northerly transporting, respectively, clean marine and polluted continental air masses, the average submicrometer aerosol mass nearly doubled from Leg 2 to Leg 3 and the aerosol appeared to be more influenced by continental sources. The effect of MJO‐associated convection anomalies on aerosols in the remote marine boundary layer (MBL) was measured during November when a complete MJO convection wave moved over the equatorial Indian Ocean and during October when a partial MJO event was observed. MJO‐associated convection strongly affected the local aerosol as increased vertical mixing introduced new particles into the MBL, rainout cleared the atmosphere of submicrometer aerosol particles, and high winds enhanced the concentration of sea salt aerosol particles in the local atmosphere. Four stages of MJO‐affected aerosol population changes in the remote Indian Ocean are defined.

Carbon dioxide is the most important greenhouse gas other than water vapor, and its modulation by the biosphere is of fundamental importance to our understanding of global climate change. We have developed a new technique for vertical profiling of CO2 and meteorological parameters through the atmospheric boundary layer and well into the free troposphere. Vertical profiling of CO2 mixing ratios allows estimates of landscape-scale fluxes characteristic of approximately100 km2 of an ecosystem. The method makes use of a powered parachute as a platform and a new Tedlar bag air sampling technique. Air samples are returned to the ground where measurements of CO2 mixing ratios are made with high precision (< or =0.1%) and accuracy (< or =0.1%) using a conventional nondispersive infrared analyzer. Laboratory studies are described that characterize the accuracy and precision of the bag sampling technique and that measure the diffusion coefficient of CO2 through the Tedlar bag wall. The technique has been applied in field studies in the proximity of two AmeriFlux sites, and results are compared with tower measurements of CO2.