The Amazon is one of the few continental regions where atmospheric aerosol particles and their effects on climate are not dominated by anthropogenic sources. During the wet season, the ambient conditions approach those of the pristine pre-industrial era. We show that the fine submicrometer particles accounting for most cloud condensation nuclei are predominantly composed of secondary organic material formed by oxidation of gaseous biogenic precursors. Supermicrometer particles, which are relevant as ice nuclei, consist mostly of primary biological material directly released from rainforest biota. The Amazon Basin appears to be a biogeochemical reactor, in which the biosphere and atmospheric photochemistry produce nuclei for clouds and precipitation sustaining the hydrological cycle. The prevailing regime of aerosol-cloud interactions in this natural environment is distinctly different from polluted regions.

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[1] Dust samples were collected onboard the UK community BAe-146 research aircraft of the Facility for Airborne Atmospheric Measurements (FAAM) operated over Niger during the winter Special Observation Period of the African Monsoon Multidisciplinary Analysis project (AMMA SOP0/DABEX). Particle size, morphology, and composition were assessed using single-particle analysis by analytical scanning and transmission electron microscopy. The aerosol was found to be composed of externally mixed mineral dust and biomass burning particles. Mineral dust consists mainly of aluminosilicates in the form of illite and kaolinite and quartz, accounting for up to 80% of the aerosol number. Fe-rich particles (iron oxides) represented 4% of the particle number in the submicron fraction. Diatoms were found on all the samples, suggesting that emissions from the Bodélé depression were also contributing to the aerosol load. Satellite images confirm that the Bodélé source was active during the period of investigation. Biomass burning aerosols accounted for about 15% of the particle number of 0.1-0.6 mm diameter and were composed almost exclusively of particles containing potassium and sulfur. Soot particles were very rare. The aspect ratio AR is a measure of particle elongation. The upper limit of the AR value distribution is 5 and the median is 1.7, which suggests that mineral dust particles could be described as ellipsoids whose major axis never exceeds 1.9 Â D p (the spherical geometric diameter). This is consistent with other published values for mineral dust, including the recent Aerosol Robotic Network retrieval results of Dubovik et al. (2006).

[1] Real-time measurements of ammonia, nitric acid, hydrochloric acid, sulfur dioxide and the water-soluble inorganic aerosol species, ammonium, nitrate, chloride, and sulfate were performed at a pasture site in the Amazon Basin (Rondônia, Brazil). The measurements were made during the late dry season (biomass burning), the transition period, and the onset of the wet season (clean conditions) using a wet-annular denuder (WAD) in combination with a Steam-Jet Aerosol Collector (SJAC). Measurements were conducted from 12 September to 14 November 2002 within the framework of LBA-SMOCC (Large-Scale Biosphere Atmosphere Experiment in Amazonia -Smoke Aerosols, Clouds, Rainfall, and Climate: Aerosols From Biomass Burning Perturb Global and Regional Climate). Real-time data were combined with measurements of sodium, potassium, calcium, magnesium, and low-molecular weight (LMW) polar organic acids determined on 12-, 24-, and 48-hours integrated filter samples. The contribution of inorganic species to the fine particulate mass (D p 2.5 mm) was frequently below 20% by mass, indicating the preponderance of organic matter. The measured concentration products of NH 3 Â HNO 3 and NH 3 Â HCl persistently remained below the theoretical equilibrium dissociation constants of the NH 3 /HNO 3 /NH 4 NO 3 and NH 3 /HCl/NH 4 Cl systems during daytime (RH < 90%). The application of four thermodynamic equilibrium models (EQMs) indicates that the fine mode aerosol anions NO 3 À , Cl À , and SO 4 2À were balanced predominantly by mineral cations (particularly pyrogenic K + ) during daytime. At nighttime (RH > 90%) fine-mode NH 4 NO 3 and NH 4 Cl are predicted to be formed in the aqueous aerosol phase. Probably, Cl À was driven out of the aerosol phase largely by reaction of pyrogenic KCl with HNO 3 and H 2 SO 4 . As shown by an updated version of the equilibrium simplified aerosol model (EQSAM2), which incorporates mineral aerosol species and lumped LMW polar organic acids, daytime aerosol NH 4 + was mainly balanced by organic compounds. -H 2 O aerosol system and its gas phase precursors at a pasture site in the Amazon Basin: How relevant are mineral cations and soluble organic acids?,

Abstract. The methyl halides, methyl chloride (CH3C1), methyl bromide (CH3Br), and methyl iodide (CH3I), were measured in regional air samples and smoke from savanna fires in southern Africa during the Southern Africa Fire-Atmosphere Research Initiative-92 (SAFARI-92) experiment (August-October 1992). All three species were significantly enhanced in the smoke plumes relative to the regional background. Good correlations were found between the methyl halides and carbon monoxide, suggesting that emission was predominantly associated with the smoldering phase of the fires. About 90% of the halogen content of the fuel burned was released to the atmosphere, mostly as halide species, but a significant fraction (3-38%) was emitted in methylated form. On the basis of comparison with

[1] During the Lindenberger Aerosol Characterization Experiment (LACE 98), impactor sampling of aerosol particles in the size range of 0.1 to 25 m was performed. The atmospheric concentrations of the elements sodium to lead (11 Յ Z Յ 83) were determined by total reflection X-ray fluorescence analysis. Approximately 15,500 individual particles were examined by high-resolution scanning electron microscopy and energydispersive X-ray microanalysis, and about 3800 particles were examined by transmission electron microscopy combined with energy-dispersive X-ray microanalysis. On the basis of morphology and chemical composition the particles were classified into 10 different groups: ammonium sulfates, calcium sulfates, sea salt, metal oxides/hydroxides, carbonates, silicates, soot, biological particles, carbon/sulfate mixed particles, and rest of carbon-rich particles C rest . The phases present in the different particle groups were determined by selected area electron diffraction in the transmission electron microscope. In addition, the heterogeneous phase composition of agglomerates was studied in detail. On the basis of the size distribution and the relative abundance of the particle groups, the average and size-resolved complex refractive index of the total aerosol were calculated. The real part of the average refractive index mainly depends on the abundance of metal oxide/hydroxide particles and varied between 1.52 and 1.57 on the different sampling days. The average imaginary part varied between 0.031 and 0.057 depending on the amounts of soot and carbon/sulfate mixed particles. The average complex refractive index deduced from the analysis of individual aerosol particles is in good agreement with the results of photometer measurements of dried filter samples.

Abstract. The relative importance of biomass-burning (pyrogenic) emissions from savannas, deforestation, agricultural waste burning, and biofuel consumption to tropospheric ozone abundance over Africa has been estimated for the year 1993, on the basis of global model calculations. We also calculated the importance of this emission source to tropospheric ozone in other regions of the world and compared it to different sources on the African regional and global scales. The estimated annual average total tropospheric ozone abundance over Africa for the reference year is 26 Tg. Pyrogenic, industrial, biogenic, and lightning emissions account for 16, 19, 12, and 27%, respectively, while stratospheric ozone input accounts for 26%. In the planetary boundary layer over Africa, the contribution by biomass burning is -24%. A large fraction of the African biomass-burning-related ozone is transported away from the continent. On a global scale, biomass burning contributes -9% to tropospheric ozone. Our model calculations suggest that Africa is the single most important region for biomass-burning-related tropospheric ozone, accounting for -35% of the global annual pyrogenic ozone enhancement of 29 Tg in 1993. IntroductionLarge-scale air pollution has traditionally been associated with anthropogenic activities in the industrialized rcgions of the world, primarily in the Northern Hemisphere. }-towever, satellite measurements of tropospheric ozone (03) have shown that in addition to distinct plumes emanating from North America, Asia, and Europe, a large amount of O3 pollution originates from tropical Africa [Fishman and Larsen, 1987;Fishman et al., 1986Fishman et al., , 1990 •Presently at University of the Witwatersrand, Johannesburg, South In this paper we report on the use of a gridded biofuelrelated trace gas emission inventory created from our studies in Africa, as partial input to a three dimensional (3-D) numerical model of atmospheric transport and chemistry (Tracer Model version 3 (TM3)). The aim is to quantitatively examine the relative influence of pyrogenic emissions on tropospheric photochemistry in Africa in particular, and globally in general, during the year 1993. Model DescriptionThe model used in this study is the Tracer Model version 3 (TM3), a 3-D atmospheric transport and chemistry model which is an updated version of TM2 described by Heimann In order to facilitate the interpretation of our model results and as a check on their numerical accuracy, we stored the tendencies by all chemical reactions, wet and dry removal processes, emissions, and transport. To reduce the output, these tendencies were stored for three vertical zones roughly representing the boundary layer, the free troposphere, and the stratosphere. Furthermore, in this study, budgets were redefined so that they are given per global region (see section 3.2.2 for the global regions used) with oceans being considered separately as a single region. For simplicity, in the budgets the troposphere is defined as the region up to 100 hPa, which in the e...

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