ALBERT

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: 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: 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.

Description: The Amazon rain forest is considered a very sensitive ecosystem that could be significantly affected by a changing climate. It is still one of the few places on Earth where the atmosphere in the continent approaches near-pristine conditions for some periods of the year. The Amazon Tall Tower Observatory (ATTO) has been built in central Amazonia to monitor the atmospheric and forest ecosystem conditions. The atmospheric conditions at the ATTO site oscillate between biogenic and biomass burning (BB) dominated states. By using a comprehensive ground-based aerosol measurement setup, we studied the physical and chemical properties of aerosol particles at the ATTO site. This paper presents results from 2012 to 2017, with special focus on light absorbing aerosol particles. The aerosol absorption wavelength dependence (expressed as the absorption Ångström exponent, åabs) was usually below 1.0 and increased during the presence of smoke transported from fires in the southern and eastern regions of the Amazon or advected from savanna fires in Africa. In this study, the brown carbon (BrC) contribution to light absorption at 370 nm was obtained by calculating the theoretical wavelength dependence of åabs (WDA). Our calculations resulted in BrC contributions of 17–29 % (25th and 75th percentiles) to total light absorption at 370 nm (σap 370) during the measurement period (2012–2017). The BrC contribution increased up to 27–47 % during fire events occurring under the influence of El Niño, between September and November 2015. An extended time series of ATTO and ZF2 (another Amazon rain forest sampling site) data showed enhanced light scattering and absorption coefficients during El Niño periods in 2009 and 2015. Long-range transport (LRT) aerosol particles that reached the central Amazon Basin from Africa or from southern Amazon exhibited a wide range of black carbon (BC) to carbon monoxide (CO) enhancement ratios (ERBC) (between 4 and 15 ng m−3 ppb−1) reflecting the variability of fuels, combustion phase, and removal processes in the atmosphere. Higher ERBC were measured during the dry season when we observed values up to 15 ng m−3 ppb−1, which were related to the lowest single scattering albedo (ω0) measured during the studied period, (0.86–0.93). A parameterization of åabs as a function of the BC to OA mass ratio was investigated and was found applicable to tropical forest emissions but further investigation is required, especially by segregating fuel types. Additionally, important enhancements of the BC mass absorption cross‑section (αabs) were found over the measurement period. This enhancement could be linked to heavy coating of the BC aerosol particles. In the future, the BC mixing state should be systematically investigated by using different instrumental approaches.

Description: 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.

Description: The Amazon rain forest experiences the combined pressures from man-made deforestation and progressing climate change, causing severe and potentially disruptive perturbations of the ecosystem's integrity and stability. To intensify research on critical aspects of Amazonian biosphere-atmosphere exchange, the Amazon Tall Tower Observatory (ATTO) has been established in the central Amazon Basin. Here we present a multi-year analysis of backward trajectories to derive an effective footprint region of the observatory, which spans large parts of the particularly vulnerable eastern basin. Further, we characterize geospatial properties of the footprint regions, such as climatic conditions, distribution of ecoregions, land cover categories, deforestation dynamics, agricultural expansion, fire regimes, infrastructural development, protected areas, as well as future deforestation scenarios. This study is meant to be a resource and reference work, helping to embed the ATTO observations into the larger context of man-made transformations of Amazonia. We conclude that the chances to observe an unperturbed rain forest-atmosphere exchange will likely decrease in the future, whereas the atmospheric signals from man-made and climate change-related forest perturbations will likewise increase in frequency and intensity.

Description: Black carbon (BC) aerosols are influencing the Earth’s atmosphere and climate, but their microphysical properties, spatiotemporal distribution and long-range transport are not well constrained. This study analyzes the transatlantic transport of BC-rich African biomass burning (BB) pollution into the Amazon Basin, based on airborne observations of aerosol particles and trace gases in and off the Brazilian coast during the ACRIDICON-CHUVA campaign in September 2014, combining in-situ measurements on the research aircraft HALO with satellite remote-sensing and numerical model results. During flight AC19 over land and ocean at the Brazilian coastline in the northeast of the Amazon Basin, we observed a BC-rich atmospheric layer at ~ 3.5 km altitude with a vertical extension of ~ 0.3 km. Backward trajectory analyses 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 days of atmospheric transport and aging. The BC mass concentrations in the layer ranged from 0.5 to 2 μg m−3, and the BC particle number fraction of ~ 40 % was about 8 times higher than observed in a fresh Amazonian BB plume, representing the highest value ever observed in the region. Upon entering the Amazon Basin, the layer 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 within the broader context of 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 north-central Amazonian aerosol population during the BB-influenced season (July to November). Specifically, the early BB season in this part of the Amazon appears to be dominated by African smoke, whereas the later BB season appears to be dominated by South American fires. This dichotomy is reflected in pronounced changes of 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 7.4 to 4.4 ng m−3 ppb−1). Our results suggest that, despite the high amount of BC particles, the African BB aerosol act as efficient cloud condensation nuclei (CCN) with potentially important implications for aerosol-cloud interactions and the hydrological cycle in the Amazon Basin.