[1] The study uses satellite observations, global assimilated aerosol data sets, Atmospheric Brown Clouds (ABC) observatories, a Monte Carlo aerosol-cloud-radiation model and a regional chemical transport model (STEM-2K) to characterize the spatial extent of brown clouds, regional and megacity ABC hot spots, chemical composition and the direct radiative forcing. It presents the first annual cycle of aerosol observations and forcing from the ABC observatories in the Indo-Asia-Pacific regions. East Asia, IndoGangetic Plains, Indonesian region, southern Africa and the Amazon basin are the regional hot spots defined by the criteria that anthropogenic aerosol optical depths (AODs) should exceed 0.3 and absorbing AOD > 0.03. Over these hot spots, as well as in other polluted oceanic regions, the EC mass exceeds 0.5 mg m À3 , the OC mass exceeds 2 mg m À3 and sulfate mass exceeds 10 mg m À3 from the surface to 3 km. The brown clouds also have strong seasonal dependence. In the tropics the seasonal dependence is driven by pollution accumulating during the dry seasons, December to February in Northern Hemisphere tropics and June to August in Southern Hemisphere tropics. In the extratropics the pollution peaks during the summer. The brown cloud problem is not restricted to the tropical regions. Over the eastern half of US and western Europe the AODs exceeds 0.2 and absorption AODs exceed 0.02. Brown clouds also extend well into the western Pacific Ocean, the Indian Ocean reaching as far south as 60°S and the eastern Atlantic Ocean. The largest total SO 2 emission occurs over China and US, while SO 2 emission per unit surface area is maximum over Germany and England. The largest total EC and OC emissions occur over China, but the largest OC emission per unit surface area occur over India. As a result, the maximum negative annual mean TOA direct forcing is over India and Germany. The surface annual-diurnal mean dimming over the regional hot spots is of the order of À10 W m À2 and À20 W m À2 over megacity hotpots. Citation: Ramanathan, V., et al. (2007), Atmospheric brown clouds: Hemispherical and regional variations in long-range transport, absorption, and radiative forcing,

[1] The sulfur transport and deposition model (STEM) is used to study the aerosol seasonality, distribution, and composition over south Asia from September 2004 to August 2005. Model predictions of sulfate, black carbon, primary organic carbon, other anthropogenic particulate matter, windblown mineral dusts, and sea salt are compared at two sites in south Asia where yearlong experimental observations are available from the Atmospheric Brown Cloud (ABC) project. The model predictions are able to capture both the magnitude and seasonality of aerosols over Hanimaadhoo Observatory, Maldives. However, the model is not able to explain the seasonality at the Kathmandu Observatory; but the model does capture Kathmandu's observed annual mean concentration. The absence of seasonal brick kiln emissions within Kathmandu valley in the current inventory is a probable reason for this problem. This model study reveals high-anthropogenic aerosol loading over the Ganges valley even in the monsoonal months, which needs to be corroborated by experimental observations. Modeling results also show a high dust loading over south Asia with a distinct seasonality. Model results of aerosol monthly composition are also presented at five cities in south Asia. Total and fine-mode monthly aerosol optical depth along with contribution from each aerosol species is presented; the results show that the anthropogenic fraction dominates in the postmonsoon and the early dry season with major contributions from sulfate and absorbing aerosols. Model sensitivity studies of dry deposition velocity and wet scavenging efficiency show that model improvements are needed in the treatment of carbonaceous aerosol dry and wet removal processes. Modeled SO 2 conversion rate constrained with sulfate observations at Hanimaadhoo suggests the need to increase model sulfate production rate during the dry season to account for probable sulfate production via heterogeneous pathways.

Abstract. The Kathmandu Valley in south Asia is considered as one of the global "hot spots" in terms of urban air pollution. It is facing severe air quality problems as a result of rapid urbanization and land use change, socioeconomic transformation, and high population growth. In this paper, we present the first full year (February 2013–January 2014) analysis of simultaneous measurements of two short-lived climate forcers/pollutants (SLCF/P), i.e., ozone (O3) and equivalent black carbon (hereinafter noted as BC) and aerosol number concentration at Paknajol, in the city center of Kathmandu. The diurnal behavior of equivalent BC and aerosol number concentration indicated that local pollution sources represent the major contributions to air pollution in this city. In addition to photochemistry, the planetary boundary layer (PBL) and wind play important roles in determining O3 variability, as suggested by the analysis of seasonal changes of the diurnal cycles and the correlation with meteorological parameters and aerosol properties. Especially during pre-monsoon, high values of O3 were found during the afternoon/evening. This could be related to mixing and entrainment processes between upper residual layers and the PBL. The high O3 concentrations, in particular during pre-monsoon, appeared well related to the impact of major open vegetation fires occurring at the regional scale. On a synoptic-scale perspective, westerly and regional atmospheric circulations appeared to be especially conducive for the occurrence of the high BC and O3 values. The very high values of SLCF/P, detected during the whole measurement period, indicated persisting adverse air quality conditions, dangerous for the health of over 3 million residents of the Kathmandu Valley, and the environment. Consequently, all of this information may be useful for implementing control measures to mitigate the occurrence of acute pollution levels in the Kathmandu Valley and surrounding area.

[1] Fourteen research flights were conducted in the Pacific Dust Experiment (PACDEX) during April and May 2007 to sample pollution and dust outbreaks from east Asia as they traveled across the northern Pacific Ocean into North America and interacted with maritime storms. Significant concentrations of black carbon (BC, consisting of soot and other light-absorbing particles measured with a soot photometer 2 instrument) and dust were observed both in the west and east Pacific Ocean from Asian plumes of dust and pollution. BC particles were observed through much of the troposphere, but the major finding is that the percentage of these particles compared with the total number of accumulation mode particles increased significantly (by a factor of 2-4) with increasing altitude, with peak values occurring between 5 and 10 km. Dust plumes had only a small impact on total cloud condensation nuclei at the sampling supersaturations but did exhibit high concentrations of ice nuclei (IN). IN concentrations in dust plumes exceeded typical tropospheric values by 4-20 times and were similar to previous studies in the Saharan aerosol layer when differences in the number concentrations of dust are accounted for. Enhanced IN concentrations were found in the upper troposphere off the coast of North America, providing a first direct validation of the transport of high-IN-containing dust layers near the tropopause entering the North American continent from distant sources. A source-specific chemical transport model was used to predict dust and other aerosols during PACDEX. The model was able to predict several features of the in situ observations, including the general altitudes where BC was found and a peak in the ratio of BC to sulfate between 5 and 10 km.

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Aerosol distributions in Asia calculated over a 4-year period and constrained by satellite observations of aerosol optical depth (AOD) are presented. Vast regions in Asia that include > 80% of the population have PM2.5 concentrations that exceed on an annual basis the WHO guideline of 10 microg/m3, often by factors of 2 to 4. These high aerosol loadings also have important radiative effects, causing a significant dimming at the surface, and mask approximately 45% of the warming by greenhouse gases. Black carbon (BC) concentrations are high throughout Asia, representing 5-10% of the total AOD, and contributing significantly to atmospheric warming (its warming potential is approximately 55% of that due to CO2). PM levels and AODs in year 2030, estimated based on simulations that consider future changes in emissions, are used to explore opportunities for win-win strategies built upon addressing air quality and climate change together. It is found that in 2030 the PM2.5 levels in significant parts of Asia will increase and exacerbate health impacts; but the aerosols will have a larger masking effect on radiative forcing, due to a decrease in BC and an increase in SO2 emissions.

Abstract. Multi-scale tracer and full-chemistry simulations with the STEM atmospheric chemistry model are used to analyze the effects of transported background ozone (O 3 ) from the eastern Pacific on California air quality during the ARCTAS-CARB experiment conducted in June, 2008. Previous work has focused on the importance of long-range transport of O 3 to North America air quality in springtime. However during this summer experiment the longrange transport of O 3 is also shown to be important. Simulated and observed O 3 transport patterns from the coast to inland northern California are shown to vary based on meteorological conditions and the O 3 profiles over the oceans, which are strongly episodically affected by Asian inflows. Analysis of the correlations of O 3 at various altitudes above the coastal site at Trinidad Head and at a downwind surface site in northern California, show that under long-range transport events, high O 3 air-masses (O 3 >60 ppb) at altitudes between about 2 and 4 km can be transported inland and can Correspondence to: M. Huang (mhuang1@engineering.uiowa.edu) significantly influence surface O 3 20-30 h later. These results show the importance of characterizing the vertical structure of the lateral boundary conditions (LBC) needed in air quality simulations. The importance of the LBC on O 3 prediction during this period is further studied through a series of sensitivity studies using different forms of LBC. It is shown that the use of the LBC downscaled from RAQMS global model that assimilated MLS and OMI data improves the model performance. We also show that the predictions can be further improved through the use of LBC based on NASA DC-8 airborne observations during the ARCTAS-CARB experiment. These results indicate the need to develop observational strategies to provide information on the three-dimensional nature of pollutant distributions, in order to improve our capability to predict pollution levels and to better quantify the influence of these Asian inflows on the US west coast air quality.

Abstract. The Sulfur Transport and dEposition Model (STEM) is applied to the analysis of observations obtained during the Intercontinental Chemical Transport Experiment-Phase B (INTEX-B), conducted over the eastern Pacific Ocean during spring 2006. Predicted trace gas and aerosol distributions over the Pacific are presented and discussed in terms of transport and source region contributions. Trace species distributions show a strong west (high) to east (low) gradient, with the bulk of the pollutant transport over the central Pacific occurring between ~20° N and 50° N in the 2–6 km altitude range. These distributions are evaluated in the eastern Pacific by comparison with the NASA DC-8 and NSF/NCAR C-130 airborne measurements along with observations from the Mt. Bachelor (MBO) surface site. Thirty different meteorological, trace gas and aerosol parameters are compared. In general the meteorological fields are better predicted than gas phase species, which in turn are better predicted than aerosol quantities. PAN is found to be significantly overpredicted over the eastern Pacific, which is attributed to uncertainties in the chemical reaction mechanisms used in current atmospheric chemistry models in general and to the specifically high PAN production in the SAPRC-99 mechanism used in the regional model. A systematic underprediction of the elevated sulfate layer in the eastern Pacific observed by the C-130 is another issue that is identified and discussed. Results from source region tagged CO simulations are used to estimate how the different source regions around the Pacific contribute to the trace gas species distributions. During this period the largest contributions were from China and from fires in South/Southeast and North Asia. For the C-130 flights, which operated off the coast of the Northwest US, the regional CO contributions range as follows: China (35%), South/Southeast Asia fires (35%), North America anthropogenic (20%), and North Asia fires (10%). The transport of pollution into the western US is studied at MBO and a variety of events with elevated Asian dust, and periods with contributions from China and fires from both Asia and North America are discussed. The role of heterogeneous chemistry on the composition over the eastern Pacific is also studied. The impacts of heterogeneous reactions at specific times can be significant, increasing sulfate and nitrate aerosol production and reducing gas phase nitric acid levels appreciably (~50%).