Abstract. Aerosol variations and trends over different land and ocean regions from 1980 to 2009 are analyzed with the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model and observations from multiple satellite sensors and available ground-based networks. Excluding time periods with large volcanic influence, aerosol optical depth (AOD) and surface concentration over polluted land regions generally vary with anthropogenic emissions, but the magnitude of this association can be dampened by the presence of natural aerosols, especially dust. Over the 30-year period in this study, the largest reduction in aerosol levels occurs over Europe, where AOD has decreased by 40–60% on average and surface sulfate concentrations have declined by a factor of up to 3–4. In contrast, East Asia and South Asia show AOD increases, but the relatively high level of dust aerosols in Asia reduces the correlation between AOD and pollutant emission trends. Over major dust source regions, model analysis indicates that the change of dust emissions over the Sahara and Sahel has been predominantly driven by the change of near-surface wind speed, but over Central Asia it has been largely influenced by the change of the surface wetness. The decreasing dust trend in the North African dust outflow region of the tropical North Atlantic and the receptor sites of Barbados and Miami is closely associated with an increase of the sea surface temperature in the North Atlantic. This temperature increase may drive the decrease of the wind velocity over North Africa, which reduces the dust emission, and the increase of precipitation over the tropical North Atlantic, which enhances dust removal during transport. Despite significant trends over some major continental source regions, the model-calculated global annual average AOD shows little change over land and ocean in the past three decades, because opposite trends in different land regions cancel each other out in the global average, and changes over large open oceans are negligible. This highlights the necessity for regional-scale assessment of aerosols and their climate impacts, as global-scale average values can obscure important regional changes.

Abstract. An assessment of global particulate nitrate and ammonium aerosol based on simulations from nine models participating in the Aerosol Comparisons between Observations and Models (AeroCom) phase III study is presented. A budget analysis was conducted to understand the typical magnitude, distribution, and diversity of the aerosols and their precursors among the models. To gain confidence regarding model performance, the model results were evaluated with various observations globally, including ground station measurements over North America, Europe, and east Asia for tracer concentrations and dry and wet depositions, as well as with aircraft measurements in the Northern Hemisphere mid-to-high latitudes for tracer vertical distributions. Given the unique chemical and physical features of the nitrate occurrence, we further investigated the similarity and differentiation among the models by examining (1) the pH-dependent NH3 wet deposition; (2) the nitrate formation via heterogeneous chemistry on the surface of dust and sea salt particles or thermodynamic equilibrium calculation including dust and sea salt ions; and (3) the nitrate coarse-mode fraction (i.e., coarse/total). It is found that HNO3, which is simulated explicitly based on full O3-HOx-NOx-aerosol chemistry by all models, differs by up to a factor of 9 among the models in its global tropospheric burden. This partially contributes to a large difference in NO3−, whose atmospheric burden differs by up to a factor of 13. The atmospheric burdens of NH3 and NH4+ differ by 17 and 4, respectively. Analyses at the process level show that the large diversity in atmospheric burdens of NO3−, NH3, and NH4+ is also related to deposition processes. Wet deposition seems to be the dominant process in determining the diversity in NH3 and NH4+ lifetimes. It is critical to correctly account for contributions of heterogeneous chemical production of nitrate on dust and sea salt, because this process overwhelmingly controls atmospheric nitrate production (typically > 80 %) and determines the coarse- and fine-mode distribution of nitrate aerosol.

Coordinated ozonesonde launches from the Intercontinental Transport Experiment (INTEX) Ozonesonde Network Study (IONS) (http://croc.gsfc.nasa.gov/intex/ions.html) in July‐August 2004 provided nearly 300 O3 profiles from eleven North American sites and the R/V Ronald H. Brown in the Gulf of Maine. With the IONS period dominated by low‐pressure conditions over northeastern North America (NENA), the free troposphere in that region was frequently enriched by stratospheric O3. Stratospheric O3 contributions to the NENA tropospheric O3 budget are computed through analyses of O3 laminae (Pierce and Grant, 1998; Teitelbaum et al., 1996), tracers (potential vorticity, water vapor), and trajectories. The lasting influence of stratospheric incursions into the troposphere is demonstrated, and the computed stratospheric contribution to tropospheric column O3 over the R/V Ronald H. Brown and six sites in Michigan, Virginia, Maryland, Rhode Island, and Nova Scotia, 23% ± 3%, is similar to summertime budgets derived from European O3 profiles (Collette and Ancellet, 2005). Analysis of potential vorticity, Wallops ozonesondes (37.9°N, 75.5°W), and Measurements of Ozone by Airbus In‐service Aircraft (MOZAIC) O3 profiles for NENA airports in June‐July‐August 1996–2004 shows that the stratospheric fraction in 2004 may be typical. Boundary layer O3 at Wallops and northeast U.S. sites during IONS also resembled O3 climatology (June‐July‐August 1996–2003). However, statistical classification of Wallops O3 profiles shows the frequency of profiles with background, nonpolluted boundary layer O3 was greater than normal during IONS.