Abstract. Every year, from December to April, anthropogenic haze spreads over most of the North Indian Ocean, and South and Southeast Asia. The Indian Ocean Experiment (INDOEX) documented this Indo-Asian haze at scales ranging from individual particles to its contribution to the regional climate forcing. This study integrates the multiplatform observations (satellites, aircraft, ships, surface stations, and balloons) with one-and fourdimensional models to derive the regional aerosol forcing resulting from the direct, the semidirect and the two indirect effects. The haze particles consisted of several inorganic and carbonaceous species, including absorbing black carbon clusters, fly ash, and mineral dust. The most striking result was the large loading of aerosols over most of the South Asian region and the North Indian Ocean. The January to March 1999 visible optical depths were about 0.5 over most of the continent and reached values as large as 0.2 over the equatorial Indian ocean due to long-range transport. The aerosol layer extended as high as 3 km. Black carbon contributed about 14% to the fine particle mass and 11% to the visible optical depth. The single-scattering albedo estimated by several independent methods was consistently around 0.9 both inland and over the open ocean. Anthropogenic sources contributed as much as 80% (_+10%) to the aerosol loading and the optical depth. The in situ data, which clearly support the existence of the first indirect effect (increased aerosol concentration producing more cloud drops with smaller effective radii), are used to develop a composite indirect effect scheme. The Indo-Asian aerosols impact the radiative forcing through a complex set of heating (positive forcing) and cooling (negative forcing) processes. Clouds and black carbon emerge as the major players. The dominant factor, however, is the large negative forcing (-20 +_ 4 W m -t) at the surface and the comparably large atmospheric heating. Regionally, the absorbing haze decreased the surface solar radiation by an amount comparable to 50% of the total ocean heat flux and nearly doubled the lower tropospheric solar heating. We demonstrate with a general circulation model how this additional heating significantly perturbs the tropical rainfall patterns and the hydrological cycle with implications to global climate.

[1] Results are presented from 3 years of simultaneous measurements of aerosol chemical composition and light scattering and absorption at Barrow, Alaska. All results are reported at the measurement relative humidity of 40%. Reported are the annual cycles of the concentration of aerosol mass, sea salt, non-sea-salt (nss) sulfate, methanesulfonate or MSA À , NH 4 + , and nss K + , Mg +2 , and Ca +2 for the submicron and supermicron size ranges. Submicron nss SO 4 = , NH 4 + , and nss K + , Mg +2 , and Ca +2 peak in winter and early spring corresponding to the arrival and persistence of Arctic Haze. Submicron sea salt displays a similar annual cycle presumably due to long-range transport from the northern Pacific Ocean. Supermicron sea salt peaks in summer corresponding to a decrease in sea ice extent. Submicron and supermicron MSA À peak in the summer due to a seasonal increase in the flux of dimethylsulfide from the ocean to the atmosphere. A correlation of MSA À and particle number concentrations suggests that summertime particle production is associated with this biogenic sulfur. Mass fractions of the dominant chemical species were calculated from the concentrations of aerosol mass and chemical species. For the submicron size range the ionic mass and associated water make up 80 to 90% of the aerosol mass from November to May. Of this ionic mass, sea salt and nss SO 4 = are the dominant species. The residual mass fraction, or fraction of mass that is chemically unanalyzed, is equivalent to the ionic mass fraction in June through October. For the supermicron size range the ionic mass and associated water make up 60 to 80% of the aerosol mass throughout the year with sea salt being the dominant species. Also reported for the submicron size range are the annual cycles of aerosol light scattering and absorption at 550 nm, Å ngström exponent for the 450 and 700 nm wavelength pair, and single scattering albedo at 550 nm. On the basis of linear regressions between the concentrations of sea salt and nss SO 4 = and the light scattering coefficient, sea salt has a dominant role in controlling light scattering during the winter, nss SO 4 = is dominant in the spring, and both components contribute to scattering in the summer. Submicron mass scattering efficiencies of the dominant aerosol chemical components (nss SO 4 = , sea salt, and residual mass) were calculated from a multiple linear regression of the measured light scattering versus the component concentrations. Submicron nss SO 4 = mass scattering efficiencies were relatively constant throughout the year with seasonal averages ranging from 4.1 ± 2.9 to 5.8 ± 1.0 m 2 g À1 . Seasonal averages for submicron sea salt ranged from 1.8 ± 0.37 to 5.1 ± 0.97 m 2 g À1 and for the residual mass ranged from 0.21 ± 0.31 to 1.5 ± 1.0 m 2 g À1 . Finally, concentrations of nss SO 4 = measured at Barrow were compared to those measured at Poker Flat Rocket Range, Denali National Park, and Homer for the 1997/1998 and 1998/1999 Arctic Haze seasons. Concentrations were highest at Barrow ...

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.

The arctic atmosphere is the repository for surprisingly high concentrations of pollutants throughout the winter months. The polluted air mass in question includes virtually all the atmosphere above the Arctic Circle and also two great lobes that extend down over Eurasia and North America. In extent, this generally polluted airmass system is about as large as the African continent. The rather severe pollution throughout this airmass system in winter is, to a large extent, a result of the lowered rates of particle and gas removal in this cold, dark, and rather stable system. The arctic haze possibly has important climatic and ecological and global change implications that are coming under investigation in a number of planned studies.

Abstract. The VAMOS Ocean-Cloud-Atmosphere-Land Regional Experiment (VOCALS-REx) was conducted from 15 October to 15 November 2008 in the South East Pacific (SEP) region to investigate interactions between land, sea and atmosphere in this unique tropical eastern ocean environment and to improve the skill of global and regional models in representing the region. This study synthesises selected aircraft, ship and surface site observations from VOCALSREx to statistically summarise and characterise the atmospheric composition and variability of the Marine Boundary Layer (MBL) and Free Troposphere (FT) along the 20 • S parallel between 70 • W and 85 • W. Significant zonal gradients in mean MBL sub-micron aerosol particle size and composition, carbon monoxide, sulphur dioxide and ozone were seen over the campaign, with a generally more variable and polluted coastal environment and a less variable, more pristine remote maritime regime. Gradients in aerosol and trace gas concentrations were observed to be associated with strong gradients in cloud droplet number. The FT wasCorrespondence to: G. Allen (grant.allen@manchester.ac.uk) often more polluted in terms of trace gases than the MBL in the mean; however increased variability in the FT composition suggests an episodic nature to elevated concentrations. This is consistent with a complex vertical interleaving of airmasses with diverse sources and hence pollutant concentrations as seen by generalised back trajectory analysis, which suggests contributions from both local and longrange sources. Furthermore, back trajectory analysis demonstrates that the observed zonal gradients both in the boundary layer and the free troposphere are characteristic of marked changes in airmass history with distance offshore -coastal boundary layer airmasses having been in recent contact with the local land surface and remote maritime airmasses having resided over ocean for in excess of ten days. Boundary layer composition to the east of 75 • W was observed to be dominated by coastal emissions from sources to the west of the Andes, with evidence for diurnal pumping of the Andean boundary layer above the height of the marine capping inversion. Analysis of intra-campaign variability in atmospheric composition was not found to be significantly correlated with observed low-frequency variability in the large scale flow pattern; campaign-average interquartile ranges of Published by Copernicus Publications on behalf of the European Geosciences Union. 5238 G. Allen et al.: South East Pacific composition during VOCALS-REx CO, SO 2 and O 3 concentrations at all longitudes were observed to dominate over much smaller differences in median concentrations calculated between periods of different flow regimes. The campaign climatology presented here aims to provide a valuable dataset to inform model simulation and future process studies, particularly in the context of aerosolcloud interaction and further evaluation of dynamical processes in the SEP region for conditions analogous to those during VOCALS-REx....