ALBERT

Description: © The Author(s), 2021. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Stevens, B., Bony, S., Farrell, D., Ament, F., Blyth, A., Fairall, C., Karstensen, J., Quinn, P. K., Speich, S., Acquistapace, C., Aemisegger, F., Albright, A. L., Bellenger, H., Bodenschatz, E., Caesar, K.-A., Chewitt-Lucas, R., de Boer, G., Delanoë, J., Denby, L., Ewald, F., Fildier, B., Forde, M., George, G., Gross, S., Hagen, M., Hausold, A., Heywood, K. J., Hirsch, L., Jacob, M., Jansen, F., Kinne, S., Klocke, D., Kölling, T., Konow, H., Lothon, M., Mohr, W., Naumann, A. K., Nuijens, L., Olivier, L., Pincus, R., Pöhlker, M., Reverdin, G., Roberts, G., Schnitt, S., Schulz, H., Siebesma, A. P., Stephan, C. C., Sullivan, P., Touzé-Peiffer, L., Vial, J., Vogel, R., Zuidema, P., Alexander, N., Alves, L., Arixi, S., Asmath, H., Bagheri, G., Baier, K., Bailey, A., Baranowski, D., Baron, A., Barrau, S., Barrett, P. A., Batier, F., Behrendt, A., Bendinger, A., Beucher, F., Bigorre, S., Blades, E., Blossey, P., Bock, O., Böing, S., Bosser, P., Bourras, D., Bouruet-Aubertot, P., Bower, K., Branellec, P., Branger, H., Brennek, M., Brewer, A., Brilouet , P.-E., Brügmann, B., Buehler, S. A., Burke, E., Burton, R., Calmer, R., Canonici, J.-C., Carton, X., Cato Jr., G., Charles, J. A., Chazette, P., Chen, Y., Chilinski, M. T., Choularton, T., Chuang, P., Clarke, S., Coe, H., Cornet, C., Coutris, P., Couvreux, F., Crewell, S., Cronin, T., Cui, Z., Cuypers, Y., Daley, A., Damerell, G. M., Dauhut, T., Deneke, H., Desbios, J.-P., Dörner, S., Donner, S., Douet, V., Drushka, K., Dütsch, M., Ehrlich, A., Emanuel, K., Emmanouilidis, A., Etienne, J.-C., Etienne-Leblanc, S., Faure, G., Feingold, G., Ferrero, L., Fix, A., Flamant, C., Flatau, P. J., Foltz, G. R., Forster, L., Furtuna, I., Gadian, A., Galewsky, J., Gallagher, M., Gallimore, P., Gaston, C., Gentemann, C., Geyskens, N., Giez, A., Gollop, J., Gouirand, I., Gourbeyre, C., de Graaf, D., de Groot, G. E., Grosz, R., Güttler, J., Gutleben, M., Hall, K., Harris, G., Helfer, K. C., Henze, D., Herbert, C., Holanda, B., Ibanez-Landeta, A., Intrieri, J., Iyer, S., Julien, F., Kalesse, H., Kazil, J., Kellman, A., Kidane, A. T., Kirchner, U., Klingebiel, M., Körner, M., Kremper, L. A., Kretzschmar, J., Krüger, O., Kumala, W., Kurz, A., L'Hégaret, P., Labaste, M., Lachlan-Cope, T., Laing, A., Landschützer, P., Lang, T., Lange, D., Lange, I., Laplace, C., Lavik, G., Laxenaire, R., Le Bihan, C., Leandro, M., Lefevre, N., Lena, M., Lenschow, D., Li, Q., Lloyd, G., Los, S., Losi, N., Lovell, O., Luneau, C., Makuch, P., Malinowski, S., Manta, G., Marinou, E., Marsden, N., Masson, S., Maury, N., Mayer, B., Mayers-Als, M., Mazel, C., McGeary, W., McWilliams, J. C., Mech, M., Mehlmann, M., Meroni, A. N., Mieslinger, T., Minikin, A., Minnett, P., Möller, G., Morfa Avalos, Y., Muller, C., Musat, I., Napoli, A., Neuberger, A., Noisel, C., Noone, D., Nordsiek, F., Nowak, J. L., Oswald, L., Parker, D. J., Peck, C., Person, R., Philippi, M., Plueddemann, A., Pöhlker, C., Pörtge, V., Pöschl, U., Pologne, L., Posyniak, M., Prange, M., Quiñones Meléndez, E., Radtke, J., Ramage, K., Reimann, J., Renault, L., Reus, K., Reyes, A., Ribbe, J., Ringel, M., Ritschel, M., Rocha, C. B., Rochetin, N., Röttenbacher, J., Rollo, C., Royer, H., Sadoulet, P., Saffin, L., Sandiford, S., Sandu, I., Schäfer, M., Schemann, V., Schirmacher, I., Schlenczek, O., Schmidt, J., Schröder, M., Schwarzenboeck, A., Sealy, A., Senff, C. J., Serikov, I., Shohan, S., Siddle, E., Smirnov, A., Späth, F., Spooner, B., Stolla, M. K., Szkółka, W., de Szoeke, S. P., Tarot, S., Tetoni, E., Thompson, E., Thomson, J., Tomassini, L., Totems, J., Ubele, A. A., Villiger, L., von Arx, J., Wagner, T., Walther, A., Webber, B., Wendisch, M., Whitehall, S., Wiltshire, A., Wing, A. A., Wirth, M., Wiskandt, J., Wolf, K., Worbes, L., Wright, E., Wulfmeyer, V., Young, S., Zhang, C., Zhang, D., Ziemen, F., Zinner, T., and Zöger, M.: EUREC4A. Earth System Science Data, 13(8), (2021): 4067–4119, https://doi.org/10.5194/essd-13-4067-2021.

Description: The science guiding the EUREC4A campaign and its measurements is presented. EUREC4A comprised roughly 5 weeks of measurements in the downstream winter trades of the North Atlantic – eastward and southeastward of Barbados. Through its ability to characterize processes operating across a wide range of scales, EUREC4A marked a turning point in our ability to observationally study factors influencing clouds in the trades, how they will respond to warming, and their link to other components of the earth system, such as upper-ocean processes or the life cycle of particulate matter. This characterization was made possible by thousands (2500) of sondes distributed to measure circulations on meso- (200 km) and larger (500 km) scales, roughly 400 h of flight time by four heavily instrumented research aircraft; four global-class research vessels; an advanced ground-based cloud observatory; scores of autonomous observing platforms operating in the upper ocean (nearly 10 000 profiles), lower atmosphere (continuous profiling), and along the air–sea interface; a network of water stable isotopologue measurements; targeted tasking of satellite remote sensing; and modeling with a new generation of weather and climate models. In addition to providing an outline of the novel measurements and their composition into a unified and coordinated campaign, the six distinct scientific facets that EUREC4A explored – from North Brazil Current rings to turbulence-induced clustering of cloud droplets and its influence on warm-rain formation – are presented along with an overview of EUREC4A's outreach activities, environmental impact, and guidelines for scientific practice. Track data for all platforms are standardized and accessible at https://doi.org/10.25326/165 (Stevens, 2021), and a film documenting the campaign is provided as a video supplement.

Description: This research has been supported by the people and government of Barbados; the Max Planck Society and its supporting members; the German Research Foundation (DFG) and the German Federal Ministry of Education and Research (grant nos. GPF18-1_69 and GPF18-2_50); the European Research Council (ERC) advanced grant EUREC4A (grant agreement no. 694768) under the European Union’s Horizon 2020 research and innovation program (H2020), with additional support from CNES (the French National Centre for Space Studies) through the EECLAT proposal, Météo-France, the CONSTRAIN H2020 project (grant agreement no. 820829), and the French AERIS Research Infrastructure; the Natural Environment Research Council (NE/S015868/1, NE/S015752/1, and NE/S015779/1); ERC under the European Union’s H2020 program (COMPASS, advanced grant agreement no. 74110); the French national program LEFE INSU, by IFREMER, the French research fleet, CNES, the French research infrastructures AERIS and ODATIS, IPSL, the Chaire Chanel program of the Geosciences Department at ENS, and the European Union's Horizon 2020 research and innovation program under grant agreement no. 817578 TRIATLAS; NOAA’s Climate Variability and Prediction Program within the Climate Program Office (grant nos. GC19-305 and GC19-301); NOAA cooperative agreement NA15OAR4320063; NOAA's Climate Program Office and base funds to NOAA/AOML's Physical Oceanography Division; Swiss National Science Foundation grant no. 188731; the UAS Program Office, Climate Program Office, and Physical Sciences Laboratory and by the US National Science Foundation (NSF) through grant AGS-1938108; Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany's Excellence Strategy – EXC 2037 “CLICCS – Climate, Climatic Change, and Society” – project no. 390683824; and Poland’s National Science Centre grant no. UMO-2018/30/M/ST10/00674 and Foundation for Polish Science grant no. POIR.04.04.00-00-3FD6/17-02.

Description: Black carbon (BC) aerosols influence the Earth's atmosphere and climate, but their microphysical properties, spatiotemporal distribution, and long-range transport are not well constrained. This study presents airborne observations of the transatlantic transport of BC-rich African biomass burning (BB) smoke into the Amazon Basin using a Single Particle Soot Photometer (SP2) as well as several complementary techniques. We base our results on observations of aerosols and trace gases off the Brazilian coast onboard the HALO (High Altitude and LOng range) research aircraft during the ACRIDICON-CHUVA campaign in September 2014. During flight AC19 over land and ocean at the northeastern coastline of the Amazon Basin, we observed a BC-rich layer at ∼3.5 km altitude with a vertical extension of ∼0.3 km. Backward trajectories suggest that fires in African grasslands, savannas, and shrublands were the main source of this pollution layer and that the observed BB smoke had undergone more than 10 d of atmospheric transport and aging over the South Atlantic before reaching the Amazon Basin. The aged smoke is characterized by a dominant accumulation mode, centered at about 130 nm, with a particle concentration of Nacc=850±330 cm−3. The rBC particles account for ∼15 % of the submicrometer aerosol mass and ∼40 % of the total aerosol number concentration. This corresponds to a mass concentration range from 0.5 to 2 µg m−3 (1st to 99th percentiles) and a number concentration range from 90 to 530 cm−3. Along with rBC, high cCO (150±30 ppb) and cO3 (56±9 ppb) mixing ratios support the biomass burning origin and pronounced photochemical aging of this layer. Upon reaching the Amazon Basin, it started to broaden and to subside, due to convective mixing and entrainment of the BB aerosol into the boundary layer. Satellite observations show that the transatlantic transport of pollution layers is a frequently occurring process, seasonally peaking in August/September. By analyzing the aircraft observations together with the long-term data from the Amazon Tall Tower Observatory (ATTO), we found that the transatlantic transport of African BB smoke layers has a strong impact on the northern and central Amazonian aerosol population during the BB-influenced season (July to December). In fact, the early BB season (July to September) in this part of the Amazon appears to be dominated by African smoke, whereas the later BB season (October to December) appears to be dominated by South American fires. This dichotomy is reflected in pronounced changes in aerosol optical properties such as the single scattering albedo (increasing from 0.85 in August to 0.90 in November) and the BC-to-CO enhancement ratio (decreasing from 11 to 6 ng m−3 ppb−1). Our results suggest that, despite the high fraction of BC particles, the African BB aerosol acts as efficient cloud condensation nuclei (CCN), with potentially important implications for aerosol–cloud interactions and the hydrological cycle in the Amazon.

Description: Methane (CH4) atmospheric mixing ratio measurements are analyzed for the period between June 2013 and November 2018 at the Amazon Tall Tower Observatory (ATTO). We describe the seasonal and diurnal patterns of nighttime events in which CH4 mixing ratios at the uppermost (79 m a.g.l.) inlet are significantly higher than the lowermost inlet (4 m a.g.l.) by 8 ppb or more. These nighttime events were found to be associated with a wind direction originating from the southeast and wind speeds between 2 and 5 m s−1. We found that these events happen under specific nighttime atmospheric conditions when compared to other nights, exhibiting less variable sensible heat flux, low net radiation and a strong thermal stratification above the canopy. Our analysis indicates that even at wind speeds of 5.8 m s−1 the turbulence intensity, given by the standard deviation of the vertical velocity, is suppressed to values lower than 0.3 m s−1. Given these findings, we suggest that these nighttime CH4 enhancements are advected from their source location by horizontal nonturbulent motions. The most likely source location is the Uatumã River, possibly influenced by dead stands of flooded forest trees that may be enhancing CH4 emissions from those areas. Finally, biomass burning and the Amazon River were discarded as potential CH4 sources.

Description: Airborne observations over the Amazon Basin showed high aerosol particle concentrations in the upper troposphere (UT) between 8 and 15 km altitude, with number densities (normalized to standard temperature and pressure) often exceeding those in the planetary boundary layer (PBL) by 1 or 2 orders of magnitude. The measurements were made during the German–Brazilian cooperative aircraft campaign ACRIDICON–CHUVA, where ACRIDICON stands for Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems and CHUVA is the acronym for Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (global precipitation measurement), on the German High Altitude and Long Range Research Aircraft (HALO). The campaign took place in September–October 2014, with the objective of studying tropical deep convective clouds over the Amazon rainforest and their interactions with atmospheric trace gases, aerosol particles, and atmospheric radiation. Aerosol enhancements were observed consistently on all flights during which the UT was probed, using several aerosol metrics, including condensation nuclei (CN) and cloud condensation nuclei (CCN) number concentrations and chemical species mass concentrations. The UT particles differed sharply in their chemical composition and size distribution from those in the PBL, ruling out convective transport of combustion-derived particles from the boundary layer (BL) as a source. The air in the immediate outflow of deep convective clouds was depleted of aerosol particles, whereas strongly enhanced number concentrations of small particles ( 90 nm) particles in the UT, which consisted mostly of organic matter and nitrate and were very effective CCN. Our findings suggest a conceptual model, where production of new aerosol particles takes place in the continental UT from biogenic volatile organic material brought up by deep convection and converted to condensable species in the UT. Subsequently, downward mixing and transport of upper tropospheric aerosol can be a source of particles to the PBL, where they increase in size by the condensation of biogenic volatile organic compound (BVOC) oxidation products. This may be an important source of aerosol particles for the Amazonian PBL, where aerosol nucleation and new particle formation have not been observed. We propose that this may have been the dominant process supplying secondary aerosol particles in the pristine atmosphere, making clouds the dominant control of both removal and production of atmospheric particles.

Description: Size-resolved measurements of atmospheric aerosol and cloud condensation nuclei (CCN) concentrations and hygroscopicity were conducted over a full seasonal cycle at the remote Amazon Tall Tower Observatory (ATTO, March 2014–February 2015). In a preceding companion paper, we presented annually and seasonally averaged data and parametrizations (Part 1; Pöhlker et al., 2016a). In the present study (Part 2), we analyze key features and implications of aerosol and CCN properties for the following characteristic atmospheric conditions: Empirically pristine rain forest (PR) conditions, where no influence of pollution was detectable, as observed during parts of the wet season from March to May. The PR episodes are characterized by a bimodal aerosol size distribution (strong Aitken mode with DAit ≈ 70 nm and NAit ≈ 160 cm−3, weak accumulation mode with Dacc ≈ 160 nm and Nacc≈ 90 cm−3), a chemical composition dominated by organic compounds, and relatively low particle hygroscopicity (κAit≈ 0.12, κacc ≈ 0.18). Long-range-transport (LRT) events, which frequently bring Saharan dust, African biomass smoke, and sea spray aerosols into the Amazon Basin, mostly during February to April. The LRT episodes are characterized by a dominant accumulation mode (DAit ≈ 80 nm, NAit ≈ 120 cm−3 vs. Dacc ≈ 180 nm, Nacc ≈ 310 cm−3), an increased abundance of dust and salt, and relatively high hygroscopicity (κAit≈ 0.18, κacc ≈ 0.35). The coarse mode is also significantly enhanced during these events. Biomass burning (BB) conditions characteristic for the Amazonian dry season from August to November. The BB episodes show a very strong accumulation mode (DAit ≈ 70 nm, NAit ≈ 140 cm−3 vs. Dacc ≈ 170 nm, Nacc ≈ 3400 cm−3), very high organic mass fractions (∼ 90 %), and correspondingly low hygroscopicity (κAit≈ 0.14, κacc ≈ 0.17). Mixed-pollution (MPOL) conditions with a superposition of African and Amazonian aerosol emissions during the dry season. During the MPOL episode presented here as a case study, we observed African aerosols with a broad monomodal distribution (D ≈ 130 nm, NCN,10 ≈ 1300 cm−3), with high sulfate mass fractions (∼ 20 %) from volcanic sources and correspondingly high hygroscopicity (κ100nm≈ 0.22), which were periodically mixed with fresh smoke from nearby fires (D ≈ 110 nm, NCN,10 ≈ 2800 cm−3) with an organic-dominated composition and sharply decreased hygroscopicity (κ150nm≈ 0.20). Insights into the aerosol mixing state are provided by particle hygroscopicity (κ) distribution plots, which indicate largely internal mixing for the PR aerosols (narrow κ distribution) and more external mixing for the BB, LRT, and MPOL aerosols (broad κ distributions). The CCN spectra (CCN concentration plotted against water vapor supersaturation) obtained for the different case studies indicate distinctly different regimes of cloud formation and microphysics depending on aerosol properties and meteorological conditions. The measurement results suggest that CCN activation and droplet formation in convective clouds are mostly aerosol-limited under PR and LRT conditions and updraft-limited under BB and MPOL conditions. Normalized CCN efficiency spectra (CCN divided by aerosol number concentration plotted against water vapor supersaturation) and corresponding parameterizations (Gaussian error function fits) provide a basis for further analysis and model studies of aerosol–cloud interactions in the Amazon.

Description: The Amazon rainforest is a sensitive ecosystem experiencing the combined pressures of progressing deforestation and climate change. Its atmospheric conditions oscillate between biogenic and biomass burning (BB) dominated states. The Amazon further represents one of the few remaining continental places where the atmosphere approaches pristine conditions during occasional wet season episodes. The Amazon Tall Tower Observatory (ATTO) has been established in central Amazonia to investigate the complex interactions between the rainforest ecosystem and the atmosphere. Physical and chemical aerosol properties have been analyzed continuously since 2012. This paper provides an in-depth analysis of the aerosol's optical properties at ATTO based on data from 2012 to 2017. The following key results have been obtained. The aerosol scattering and absorption coefficients at 637 nm, σsp,637 and σap,637, show a pronounced seasonality with lowest values in the clean wet season (mean ± SD: σsp,637=7.5±9.3 M m−1; σap,637=0.68±0.91 M m−1) and highest values in the BB-polluted dry season (σsp,637=33±25 M m−1; σap,637=4.0±2.2 M m−1). The single scattering albedo at 637 nm, ω0, is lowest during the dry season (ω0=0.87±0.03) and highest during the wet season (ω0=0.93±0.04). The retrieved BC mass absorption cross sections, αabs, are substantially higher than values widely used in the literature (i.e., 6.6 m2 g−1 at 637 nm wavelength), likely related to thick organic or inorganic coatings on the BC cores. Wet season values of αabs=11.4±1.2 m2 g−1 (637 nm) and dry season values of αabs=12.3±1.3 m2 g−1 (637 nm) were obtained. The BB aerosol during the dry season is a mixture of rather fresh smoke from local fires, somewhat aged smoke from regional fires, and strongly aged smoke from African fires. The African influence appears to be substantial, with its maximum from August to October. The interplay of African vs. South American BB emissions determines the aerosol optical properties (e.g., the fractions of black vs. brown carbon, BC vs. BrC). By analyzing the diel cycles, it was found that particles from elevated aerosol-rich layers are mixed down to the canopy level in the early morning and particle number concentrations decrease towards the end of the day. Brown carbon absorption at 370 nm, σap,BrC,370, was found to decrease earlier in the day, likely due to photo-oxidative processes. BC-to-CO enhancement ratios, ERBC, reflect the variability of burnt fuels, combustion phases, and atmospheric removal processes. A wide range of ERBC between 4 and 15 ng m−3 ppb−1 was observed with higher values during the dry season, corresponding to the lowest ω0 levels (0.86–0.93). The influence of the 2009/2010 and 2015/2016 El Niño periods and the associated increased fire activity on aerosol optical properties was analyzed by means of 9-year σsp and σap time series (combination of ATTO and ZF2 data). Significant El Niño-related enhancements were observed: in the dry season, σsp,637 increased from 24±18 to 48±33 M m−1 and σap, 637 from 3.8±2.8 to 5.3±2.5 M m−1. The absorption Ångström exponent, åabs, representing the aerosol absorption wavelength dependence, was mostly

Description: The long-range transport (LRT) of trace gases and aerosol particles plays an important role for the composition of the Amazonian rain forest atmosphere. Sulfate aerosols originate to a substantial extent from LRT sources and play an important role in the Amazonian atmosphere as strongly light-scattering particles and effective cloud condensation nuclei. The transatlantic transport of volcanic sulfur emissions from Africa has been considered as a source of particulate sulfate in the Amazon; however, direct observations have been lacking so far. This study provides observational evidence for the influence of emissions from the Nyamuragira–Nyiragongo volcanoes in Africa on Amazonian aerosol properties and atmospheric composition during September 2014. Comprehensive ground-based and airborne aerosol measurements together with satellite observations are used to investigate the volcanic event. Under the volcanic influence, hourly mean sulfate mass concentrations in the submicron size range reached up to 3.6 µg m−3 at the Amazon Tall Tower Observatory, the highest value ever reported in the Amazon region. The substantial sulfate injection increased the aerosol hygroscopicity with κ values up to 0.36, thus altering aerosol–cloud interactions over the rain forest. Airborne measurements and satellite data indicate that the transatlantic transport of volcanogenic aerosols occurred in two major volcanic plumes with a sulfate-enhanced layer between 4 and 5 km of altitude. This study demonstrates how African aerosol sources, such as volcanic sulfur emissions, can substantially affect the aerosol cycling and atmospheric processes in Amazonia.

Description: During the ACRIDICON-CHUVA field project (September–October 2014; based in Manaus, Brazil) aircraft-based in situ measurements of aerosol chemical composition were conducted in the tropical troposphere over the Amazon using the High Altitude and Long Range Research Aircraft (HALO), covering altitudes from the boundary layer (BL) height up to 14.4 km. The submicron non-refractory aerosol was characterized by flash-vaporization/electron impact-ionization aerosol particle mass spectrometry. The results show that significant secondary organic aerosol (SOA) formation by isoprene oxidation products occurs in the upper troposphere (UT), leading to increased organic aerosol mass concentrations above 10 km altitude. The median organic mass concentrations in the UT above 10 km range between 1.0 and 2.5 µg m−3 (referring to standard temperature and pressure; STP) with interquartile ranges of 0.6 to 3.2 µg m−3 (STP), representing 78 % of the total submicron non-refractory aerosol particle mass. The presence of isoprene-epoxydiol-derived secondary organic aerosol (IEPOX-SOA) was confirmed by marker peaks in the mass spectra. We estimate the contribution of IEPOX-SOA to the total organic aerosol in the UT to be about 20 %. After isoprene emission from vegetation, oxidation processes occur at low altitudes and/or during transport to higher altitudes, which may lead to the formation of IEPOX (one oxidation product of isoprene). Reactive uptake or condensation of IEPOX on preexisting particles leads to IEPOX-SOA formation and subsequently increasing organic mass in the UT. This organic mass increase was accompanied by an increase in the nitrate mass concentrations, most likely due to NOx production by lightning. Analysis of the ion ratio of NO+ to NO2+ indicated that nitrate in the UT exists mainly in the form of organic nitrate. IEPOX-SOA and organic nitrates are coincident with each other, indicating that IEPOX-SOA forms in the UT either on acidic nitrate particles forming organic nitrates derived from IEPOX or on already neutralized organic nitrate aerosol particles.

Description: In the Amazonian atmosphere, the aerosol coarse mode comprises a complex, diverse, and variable mixture of bioaerosols emitted from the rain forest ecosystem, long-range transported Saharan dust (we use Sahara as shorthand for the dust source regions in Africa north of the Equator), marine aerosols from the Atlantic Ocean, and coarse smoke particles from deforestation fires. For the rain forest, the coarse mode particles are of significance with respect to biogeochemical and hydrological cycling, as well as ecology and biogeography. However, knowledge on the physicochemical and biological properties as well as the ecological role of the Amazonian coarse mode is still sparse. This study presents results from multi-year coarse mode measurements at the remote Amazon Tall Tower Observatory (ATTO) site. It combines online aerosol observations, selected remote sensing and modeling results, as well as dedicated coarse mode sampling and analysis. The focal points of this study are a systematic characterization of aerosol coarse mode abundance and properties in the Amazonian atmosphere as well as a detailed analysis of the frequent, pulse-wise intrusion of African long-range transport (LRT) aerosols (comprising Saharan dust and African biomass burning smoke) into the Amazon Basin.We find that, on a multi-year time scale, the Amazonian coarse mode maintains remarkably constant concentration levels (with 0.4 cm−3 and 4.0 µg m−3 in the wet vs. 1.2 cm−3 and 6.5 µg m−3 in the dry season) with rather weak seasonality (in terms of abundance and size spectrum), which is in stark contrast to the pronounced biomass burning-driven seasonality of the submicron aerosol population and related parameters. For most of the time, bioaerosol particles from the forest biome account for a major fraction of the coarse mode background population. However, from December to April there are episodic intrusions of African LRT aerosols, comprising Saharan dust, sea salt particles from the transatlantic passage, and African biomass burning smoke. Remarkably, during the core period of this LRT season (i.e., February–March), the presence of LRT influence, occurring as a sequence of pulse-like plumes, appears to be the norm rather than an exception. The LRT pulses increase the coarse mode concentrations drastically (up to 100 µg m−3) and alter the coarse mode composition as well as its size spectrum. Efficient transport of the LRT plumes into the Amazon Basin takes place in response to specific mesoscale circulation patterns in combination with the episodic absence of rain-related aerosol scavenging en route. Based on a modeling study, we estimated a dust deposition flux of 5–10 kg ha−1 a−1 in the region of the ATTO site. Furthermore, a chemical analysis quantified the substantial increase of crustal and sea salt elements under LRT conditions in comparison to the background coarse mode composition. With these results, we estimated the deposition fluxes of various elements that are considered as nutrients for the rain forest ecosystem. These estimates range from few g ha−1 a−1 up to several hundreds of g ha−1 a−1 in the ATTO region.The long-term data presented here provide a statistically solid basis for future studies of the manifold aspects of the dynamic coarse mode aerosol cycling in the Amazon. Thus, it may help to understand its biogeochemical relevance in this ecosystem as well as to evaluate to what extent anthropogenic influences have altered the coarse mode cycling already.

Description: In the Amazonian atmosphere, the aerosol coarse mode comprises a complex, diverse, and variable mixture of bioaerosols emitted from the rain forest ecosystem, long-range transported Saharan dust, marine aerosols from the Atlantic Ocean, and coarse smoke particles from deforestation fires. For the rain forest, the coarse mode particles are of significance with respect to biogeochemical and hydrological cycling as well as ecology and biogeography. However, detailed knowledge on the physicochemical and biological properties as well as the ecological role of the Amazonian coarse mode is still sparse. This study presents results from multi-year coarse mode measurements at the remote Amazon Tall Tower Observatory (ATTO) site. It combines online aerosol observations, selected remote sensing and modelling results, as well as dedicated coarse mode sampling and analysis. The focal points of this study are a systematic characterization of aerosol coarse mode abundance and properties in the Amazonian atmosphere as well as a detailed analysis of the frequent, pulse-wise intrusion of African long-range transport (LRT) aerosols (comprising Saharan dust and African biomass burning smoke) into the Amazon Basin. We find that, on a multi-year time scale, the Amazonian coarse mode maintains remarkably constant concentration levels (with 0.4 cm−3 and 4.0 µg m−3 in the wet vs. 1.2 cm−3 and 6.5 µg m−3 in the dry season) with rather weak seasonal trends (in terms of abundance and size spectrum), which is in stark contrast to the pronounced biomass burning-driven seasonality of the submicron aerosol population and related parameters. For most of the time, bioaerosol particles from the forest biome account for a major fraction of the coarse mode background population. However, from Dec to Apr there are episodic intrusions of African LRT aerosols, comprising Saharan dust, sea salt particles from the transatlantic passages, and African biomass burning smoke. Remarkably, during the core period of this LRT season (i.e., Feb–Mar), the presence of LRT influence, occurring as a sequence of pulse-like plumes, appears to be rather the norm than an exception. The LRT pulses increase the coarse mode concentrations drastically (up to 100 µg m−3) and alter coarse mode composition as well as its size spectrum. Efficient transport of the LRT plumes into the Amazon Basin takes place in response to specific mesoscale circulation patterns in combination with the episodic absence of rain-related aerosol scavenging en route. Based on a modelling study, we estimated a dust deposition flux of 5–10 kg ha−1 a−1 in the region of the ATTO site. Furthermore, a chemical analysis quantified the substantial increase of crustal and sea salt elements under LRT conditions in comparison to the background coarse mode composition. With these results, we estimated the deposition fluxes of various elements that are considered as nutrients for the rain forest ecosystem. These estimates range from few g ha−1 a−1 up to several hundreds of g ha−1 a−1 in the ATTO region. The long-term data presented here provide a statistically solid basis for future studies of the manifold aspects of the dynamic coarse mode aerosol cycling in the Amazon. Thus, it may help to understand its biogeochemical relevance in this ecosystem as well as to evaluate to what extent anthropogenic influences have altered the coarse mode cycling already.