Wildfires inject large amounts of black carbon (BC) particles into the atmosphere, which can reach the lowermost stratosphere (LMS) and cause strong radiative forcing. During a 14-month period of ...observations on board a passenger aircraft flying between Europe and North America, we found frequent and widespread biomass burning (BB) plumes, influencing 16 of 160 flight hours in the LMS. The average BC mass concentrations in these plumes (∼140 ng·m−3, standard temperature and pressure) were over 20 times higher than the background concentration (∼6 ng·m−3) with more than 100-fold enhanced peak values (up to ∼720 ng·m−3). In the LMS, nearly all BC particles were covered with a thick coating. The average mass equivalent diameter of the BC particle cores was ∼120 nm with a mean coating thickness of ∼150 nm in the BB plume and ∼90 nm with a coating of ∼125 nm in the background. In a BB plume that was encountered twice, we also found a high diameter growth rate of ∼1 nm·h−1 due to the BC particle coatings. The observed high concentrations and thick coatings of BC particles demonstrate that wildfires can induce strong local heating in the LMS and may have a significant influence on the regional radiative forcing of climate.
The nucleation of atmospheric vapours is an important source of new aerosol particles that can subsequently grow to form cloud condensation nuclei in the atmosphere. Most field studies of atmospheric ...aerosols over continents are influenced by atmospheric vapours of anthropogenic origin (for example, ref. 2) and, in consequence, aerosol processes in pristine, terrestrial environments remain poorly understood. The Amazon rainforest is one of the few continental regions where aerosol particles and their precursors can be studied under near-natural conditions, but the origin of small aerosol particles that grow into cloud condensation nuclei in the Amazon boundary layer remains unclear. Here we present aircraft- and ground-based measurements under clean conditions during the wet season in the central Amazon basin. We find that high concentrations of small aerosol particles (with diameters of less than 50 nanometres) in the lower free troposphere are transported from the free troposphere into the boundary layer during precipitation events by strong convective downdrafts and weaker downward motions in the trailing stratiform region. This rapid vertical transport can help to maintain the population of particles in the pristine Amazon boundary layer, and may therefore influence cloud properties and climate under natural conditions.
Size-resolved long-term measurements of atmospheric aerosol and cloud condensation nuclei (CCN) concentrations and hygroscopicity were conducted at the remote Amazon Tall Tower Observatory (ATTO) in ...the central Amazon Basin over a 1-year period and full seasonal cycle (March 2014–February 2015). The measurements provide a climatology of CCN properties characteristic of a remote central Amazonian rain forest site.The CCN measurements were continuously cycled through 10 levels of supersaturation (S = 0.11 to 1.10 %) and span the aerosol particle size range from 20 to 245 nm. The mean critical diameters of CCN activation range from 43 nm at S = 1.10 % to 172 nm at S = 0.11 %. The particle hygroscopicity exhibits a pronounced size dependence with lower values for the Aitken mode (κAit = 0.14 ± 0.03), higher values for the accumulation mode (κAcc = 0.22 ± 0.05), and an overall mean value of κmean = 0.17 ± 0.06, consistent with high fractions of organic aerosol.The hygroscopicity parameter, κ, exhibits remarkably little temporal variability: no pronounced diurnal cycles, only weak seasonal trends, and few short-term variations during long-range transport events. In contrast, the CCN number concentrations exhibit a pronounced seasonal cycle, tracking the pollution-related seasonality in total aerosol concentration. We find that the variability in the CCN concentrations in the central Amazon is mostly driven by aerosol particle number concentration and size distribution, while variations in aerosol hygroscopicity and chemical composition matter only during a few episodes.For modeling purposes, we compare different approaches of predicting CCN number concentration and present a novel parametrization, which allows accurate CCN predictions based on a small set of input data.
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 <1.0 with episodic increases upon smoke advection. A parameterization of åabs as a function of the BC-to-OA mass ratio for Amazonian aerosol ambient measurements is presented. The brown carbon (BrC) contribution to σap at 370 nm was obtained by calculating the theoretical BC åabs, resulting in BrC contributions of 17 %–29 % (25th and 75th percentiles) to σap 370 for the entire measurement period. The BrC contribution increased to 27 %–47 % during fire events under El Niño-related drought conditions from September to November 2015. The results presented here may serve as a basis to understand Amazonian atmospheric aerosols in terms of their interactions with solar radiation and the physical and chemical-aging processes that they undergo during transport. Additionally, the analyzed aerosol properties during the last two El Niño periods in 2009/2010 and 2015/2016 offer insights that could help to assess the climate change-related potential for forest-dieback feedbacks under warmer and drier conditions.
We use a global chemical transport model (GEOS-Chem) to interpret observed light-absorbing aerosols in Amazonia during the wet season. Observed aerosol properties, including black carbon (BC) ...concentration and light absorption, at the Amazon Tall Tower Observatory (ATTO) site in the central Amazon have relatively low background levels but frequently show high peaks during the study period of January–April 2014. With daily temporal resolution for open fire emissions and modified aerosol optical properties, our model successfully captures the observed variation in fine/coarse aerosol and BC concentrations as well as aerosol light absorption and its wavelength dependence over the Amazon Basin. The source attribution in the model indicates the important influence of open fire on the observed variances of aerosol concentrations and absorption, mainly from regional sources (northern South America) and from northern Africa. The contribution of open fires from these two regions is comparable, with the latter becoming more important in the late wet season. The analysis of correlation and enhancement ratios of BC versus CO suggests transport times of < 3 days for regional fires and ∼ 11 days for African plumes arriving at ATTO during the wet season. The model performance of long-range transport of African plumes is also evaluated with observations from AERONET, MODIS, and CALIOP. Simulated absorption aerosol optical depth (AAOD) averaged over the wet season is lower than 0.0015 over the central Amazon, including the ATTO site. We find that more than 50 % of total absorption at 550 nm is from BC, except for the northeastern Amazon and the Guianas, where the influence of dust becomes significant (up to 35 %). The brown carbon contribution is generally between 20 and 30 %. The distribution of absorption Ångström exponents (AAE) suggests more influence from fossil fuel combustion in the southern part of the basin (AAE ∼ 1) but more open fire and dust influence in the northern part (AAE > 1.8). Uncertainty analysis shows that accounting for absorption due to secondary organic aerosol (SOA) and primary biogenic aerosol (PBA) particles could result in differences of < 8 and 5–40 % in total absorption, respectively.
The intercontinental transport of aerosols from the Sahara desert plays a significant role in nutrient cycles in the Amazon rainforest, since it carries many types of minerals to these otherwise ...low-fertility lands. Iron is one of the micronutrients essential for plant growth, and its long-range transport might be an important source for the iron-limited Amazon rainforest. This study assesses the bioavailability of iron Fe(II) and Fe(III) in the particulate matter over the Amazon forest, which was transported from the Sahara desert (for the sake of our discussion, this term also includes the Sahel region). The sampling campaign was carried out above and below the forest canopy at the ATTO site (Amazon Tall Tower Observatory), a near-pristine area in the central Amazon Basin, from March to April 2015. Measurements reached peak concentrations for soluble Fe(III) (48 ng m−3), Fe(II) (16 ng m−3), Na (470 ng m−3), Ca (194 ng m−3), K (65 ng m−3), and Mg (89 ng m−3) during a time period of dust transport from the Sahara, as confirmed by ground-based and satellite remote sensing data and air mass backward trajectories. Dust sampled above the Amazon canopy included primary biological aerosols and other coarse particles up to 12 µm in diameter. Atmospheric transport of weathered Saharan dust, followed by surface deposition, resulted in substantial iron bioavailability across the rainforest canopy. The seasonal deposition of dust, rich in soluble iron, and other minerals is likely to assist both bacteria and fungi within the topsoil and on canopy surfaces, and especially benefit highly bioabsorbent species. In this scenario, Saharan dust can provide essential macronutrients and micronutrients to plant roots, and also directly to plant leaves. The influence of this input on the ecology of the forest canopy and topsoil is discussed, and we argue that this influence would likely be different from that of nutrients from the weathered Amazon bedrock, which otherwise provides the main source of soluble mineral nutrients.
Deriving absorption coefficients from Aethalometer attenuation data requires different corrections to compensate for artifacts related to filter-loading effects, scattering by filter fibers, and ...scattering by aerosol particles. In this study, two different correction schemes were applied to seven-wavelength Aethalometer data, using multi-angle absorption photometer (MAAP) data as a reference absorption measurement at 637 nm. The compensation algorithms were compared to five-wavelength offline absorption measurements obtained with a multi-wavelength absorbance analyzer (MWAA), which serves as a multiple-wavelength reference measurement. The online measurements took place in the Amazon rainforest, from the wet-to-dry transition season to the dry season (June–September 2014). The mean absorption coefficient (at 637 nm) during this period was 1.8 ± 2.1 Mm−1, with a maximum of 15.9 Mm−1. Under these conditions, the filter-loading compensation was negligible. One of the correction schemes was found to artificially increase the short-wavelength absorption coefficients. It was found that accounting for the aerosol optical properties in the scattering compensation significantly affects the absorption Ångström exponent (åABS) retrievals. Proper Aethalometer data compensation schemes are crucial to retrieve the correct åABS, which is commonly implemented in brown carbon contribution calculations. Additionally, we found that the wavelength dependence of uncompensated Aethalometer attenuation data significantly correlates with the åABS retrieved from offline MWAA measurements.
Abstract
Smoke from vegetation fires affects air quality, atmospheric cycling, and the climate in the Amazon rain forest. A major unknown has remained the quantity of long-range transported smoke ...from Africa in relation to local and regional fire emissions. Here we quantify the abundance, seasonality, and properties of African smoke in central Amazonia. We show that it accounts for ~ 60% of the black carbon concentrations during the wet season and ~ 30% during the dry season. The African smoke influences aerosol-radiation interactions across the entire Amazon, with the strongest impact on the vulnerable eastern basin, a hot spot of climate and land use change. Our findings further suggest that the direct influence of African smoke has been historically relevant for soil fertilization, the carbon and water cycles, and, thus, the development of the Amazon forest ecosystem, even in the pre-industrial era.
Air quality measurements usually consist of ground-based instrumentation at fixed locations. However, vertical profiles of pollutants are of interest for understanding processes, distribution, ...dilution and concentration. Therefore, a multicopter system has been developed to investigate the vertical distribution of the concentration of aerosol particles, black carbon, ozone, nitrogen oxides (NOx) and carbon monoxide and the meteorological parameters of temperature and humidity. This article presents the requirements by different users, the setup of the quadrocopter system, the instrumentation and the results of first applications. The vertical distribution of particulate matter next to a highway was strongly related to atmospheric stratification, with different concentrations below and above the temperature inversion present in the morning. After the qualification phase described in this article, two identically equipped multicopters will be used upwind and downwind of line or diffuse sources such as highways or urban areas to quantify the influence of their emissions on the local air quality.
Abstract
Early career (EC) Earth system scientists in the Latin America and the Caribbean region (LAC) have been facing several issues, such as limited funding opportunities, substandard scientific ...facilities, lack of security of tenure, and unrepresented groups equality issues. On top of this, the worsening regional environmental and climatic crises call for the need for this new generation of scientists to help to tackle these crises by increasing public awareness and research. Realizing the need to converge and step up in making a collective action to be a part of the solution, the Latin America Early Career Earth System Scientist Network (LAECESS) was created in 2016. LAECESS’s primary goals are to promote regional networking, foster integrated and interdisciplinary science, organize soft skills courses and workshops, and empower Latin American EC researchers. This article is an initial step towards letting the global science community grasp the current situation and hear the early career LAC science community’s perspectives. The paper also presents a series of future steps needed for better scientific and social development in the LAC region.