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Long-range transport (LRT) plays an important role in the Amazon rain forest by bringing in different primary and secondary aerosol particles from distant sources. The atmospheric oxidation of dimethyl sulfide (DMS), emitted from marine plankton, is considered an important sulfate source over the Amazon rain forest, with a lesser contribution from terrestrial soil and vegetation sulfur emissions. Volcanic sulfur emissions from Africa could be a source of particulate sulfate to the Amazonian atmosphere upon transatlantic transport but no observations have been published. By using satellite observations, together with ground‑based and airborne aerosol particle observations, this paper provides evidence of the influence that volcanic emissions have on the aerosol properties that have been observed in central Amazonia. Under the volcanic influence, sulfate mass concentrations reached up to 3.6 µg m−3 (hourly mean) at ground level, the highest value ever reported in the Amazon region. The hygroscopicity parameter was higher than the characteristic dry-season average, reaching a maximum of 0.36 for accumulation mode aerosol particles. Airborne measurements and satellite data indicated the transport of two different volcanic plumes reaching the Amazon Basin in September 2014 with a sulfate-enhanced layer at an altitude between 4 and 5 km. These observations show that remote volcanic sources can episodically affect the aerosol cycling over the Amazon rain forest and perturb the background conditions. Further studies should address the long-term effect of volcanogenic aerosol particles over the Amazon Basin by running long-term and intensive field measurements in the Amazon region and by monitoring African emissions and their transatlantic transport.

International audience; During the Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) campaign, size-resolved cloud condensation nuclei (CCN) spectra were characterized at a research site (T3) 60 km downwind of the city of Manaus, Brazil, in central Amazonia for 1 year (12 March 2014 to 3 March 2015). Particle hygroscopicity (κ CCN) and mixing state were derived from the size-resolved CCN spectra, and the hygroscopicity of the organic component of the aerosol (κ org) was then calculated from κ CCN and concurrent chemical composition measurements. The annual average κ CCN increased from 0.13 at 75 nm to 0.17 at 171 nm, and the increase was largely due to an increase in sulfate volume fraction. During both wet and dry seasons, κ CCN , κ org , and particle composition under background conditions exhibited essentially no diel variations. The constant κ org of ∼ 0.15 is consistent with the largely uniform and high O : C value (∼ 0.8), indicating that the aerosols under background conditions are dominated by the aged regional aerosol particles consisting of highly oxygenated organic compounds. For air masses strongly influenced by urban pollution and/or local biomass burning, lower values of κ org and organic O : C atomic ratio were observed during night, due to accumulation of freshly emitted particles, dominated by primary organic aerosol (POA) with low hygroscopicity, within a shallow nocturnal boundary layer. The O : C, κ org , and κ CCN increased from the early morning hours and peaked around noon, driven by the formation and aging of secondary organic aerosol (SOA) and dilution of POA emissions into a deeper Published by Copernicus Publications on behalf of the European Geosciences Union. 11780 R. Thalman et al.: CCN activity and organic hygroscopicity of aerosols downwind of an urban region boundary layer, while the development of the boundary layer, which leads to mixing with aged particles from the residual layer aloft, likely also contributed to the increases. The hy-groscopicities associated with individual organic factors, derived from PMF (positive matrix factorization) analysis of AMS (aerosol mass spectrometry) spectra, were estimated through multivariable linear regression. For the SOA factors, the variation of the κ value with O : C agrees well with the linear relationship reported from earlier laboratory studies of SOA hygroscopicity. On the other hand, the variation in O : C of ambient aerosol organics is largely driven by the variation in the volume fractions of POA and SOA factors, which have very different O : C values. As POA factors have hygroscop-icity values well below the linear relationship between SOA hygroscopicity and O : C, mixtures with different POA and SOA fractions exhibit a steeper slope for the increase in κ org with O : C, as observed during this and earlier field studies. This finding helps better understand and reconcile the differences in the relationships between κ org and O : C observed in laboratory and field studies, therefore providing a basis for improved parameterization in global models, especially in a tropical context.