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Abstract. The wet-season atmosphere in the central Amazon resembles natural conditions with minimal anthropogenic influence, making it one of the rare preindustrial-like continental areas worldwide. Previous long-term studies have analyzed the properties and sources of the natural Amazonian background aerosol. However, the vertical profile of the planetary boundary layer (PBL) has not been assessed systematically. Since 2017, such a profile assessment has been possible with the 325 m high tower at the Amazon Tall Tower Observatory (ATTO), located in a largely untouched primary forest in the central Amazon. This study investigates the variability of submicrometer aerosol concentration, size distribution, and optical properties at 60 and 325 m in the Amazonian PBL. The results show significant differences in aerosol volumes and scattering coefficients in the vertical gradient. The aerosol population was well-mixed throughout the boundary layer during the daytime but became separated upon stratification during the nighttime. We also found a significant difference in the spectral dependence of the scattering coefficients between the two heights. The analysis of downdrafts and the related rainfall revealed changes in the aerosol populations before and after rain events, with absorption and scattering coefficients decreasing as optically active particles are removed by wet deposition. The recovery of absorption and scattering coefficients is faster at 325 m than at 60 m. Convective events were concomitant with rapid increases in the concentrations of sub-50 nm particles, which were likely associated with downdrafts. We found that the aerosol population near the canopy had a significantly higher mass scattering efficiency than at 325 m. There was also a clear spectral dependence, with values for λ=450, 525, and 635 nm of 7.74±0.12, 5.49±0.11, and 4.15±0.11 m2 g−1, respectively, at 60 m, while at 325 m the values were 5.26±0.06, 3.76±0.05, and 2.46±0.04 m2 g−1, respectively. The equivalent aerosol refractive index results, which were obtained for the first time for the wet season in the central Amazon, show slightly higher scattering (real) components at 60 m compared to 325 m of 1.33 and 1.27, respectively. In contrast, the refractive index's absorptive (imaginary) component was identical for both heights, at 0.006. This study shows that the aerosol physical properties at 60 and 325 m are different, likely due to aging processes, and strongly depend on the photochemistry, PBL dynamics, and aerosol sources. These findings provide valuable insights into the impact of aerosols on climate and radiative balance and can be used to improve the representation of aerosols in global climate models.

Abstract. The Amazon Basin is frequently influenced by transatlantic transport of African dust plumes during its wet season (January–April), which not only interrupts the near-pristine atmospheric condition in that season, but alsoprovides nutrient inputs to the Amazon rainforest upon deposition. In thisstudy, we use the chemical transport model GEOS-Chem to investigate theimpact of the export of African mineral dust to the Amazon Basin during theperiod of 2013–2017, constrained by multiple datasets obtained from theAErosol RObotic NETwork (AERONET), MODIS, as well as the Cayenne site and the Amazon Tall Tower Observatory (ATTO) site in the Amazon Basin. With an optimized particle mass size distribution (PMSD) of dust aerosols, the model captures observed aerosol optical depth (AOD) well in terms of both the mean value and the decline rate of the logarithm of AOD over the Atlantic Ocean along the transport path (AOaTP), implying consistency with the observed export efficiency of African dust along the transatlantic transport. With an annual emission of 0.73±0.12 Pg yr−1, African dust entering the Amazon Basin during the wet season accounts for 40±4.5 % (up to 70 %) of surface aerosol mass concentrations over the basin. Observed dust peaks over the Amazon Basin are generally associated with relatively higher African dust emissions (including the Sahara and the Sahel) and longer lifetimes of dust along the transatlantic transport, i.e., higher export efficiency of African dust across the Atlantic Ocean. The frequency of dust events during the wet season is around 18 % when averaged over the Amazon Basin, with maxima of over 60 % at the northeastern coast. During the dust events, AOD over most of the Amazon Basin is dominated by dust. Based on dust deposition, we further estimate annual inputs of 52±8.7, 0.97±0.16, and 21±3.6 mg m−2 yr−1 for iron, phosphorus, and magnesium, respectively, into the Amazon rainforest, which may to some extent compensate for the hydrologic losses of nutrients in the forest ecosystem.

The climate effects of atmospheric aerosol particles serving as cloud condensation nuclei (CCN) depend on chemical composition and hygroscopicity, which are highly variable on spatial and temporal scales. Here we present global CCN measurements, covering diverse environments from pristine to highly polluted conditions. We show that the effective aerosol hygroscopicity, κ, can be derived accurately from the fine aerosol mass fractions of organic particulate matter (ϵorg) and inorganic ions (ϵinorg) through a linear combination, κ = ϵorg ⋅ κorg + ϵinorg ⋅ κinorg. In spite of the chemical complexity of organic matter, its hygroscopicity is well captured and represented by a global average value of κorg = 0.12 ± 0.02 with κinorg = 0.63 ± 0.01 as the corresponding value for inorganic ions. By showing that the sensitivity of global climate forcing to changes in κorg and κinorg is small, we constrain a critically important aspect of global climate modelling.

This study investigates the rain-initiated mixing and variability in the mixing ratio of selected trace gases in the atmosphere over the central Amazon rain forest. It builds on comprehensive data from the Amazon Tall Tower Observatory (ATTO), spanning from 2013 to 2020 and comprising the greenhouse gases (GHGs) carbon dioxide (CO2) and methane (CH4); the reactive trace gases carbon monoxide (CO), ozone (O3), nitric oxide (NO), and nitrogen dioxide (NO2); and selected volatile organic compounds (VOCs). Based on more than 1000 analyzed rainfall events, the study resolves the trace gas mixing ratio patterns before, during, and after the rain events, along with vertical mixing ratio gradients across the forest canopy. The assessment of the rainfall events was conducted independently for daytime and nighttime periods, which allows us to elucidate the influence of solar radiation. The mixing ratios of CO2, CO, and CH4 clearly declined during rainfall, which can be attributed to the downdraft-related entrainment of pristine air from higher altitudes into the boundary layer, a reduction of the photosynthetic activity under increased cloud cover, and changes in the surface fluxes. Notably, CO showed a faster reduction than CO2, and the vertical gradient of CO2 and CO is steeper than for CH4. Conversely, the O3 mixing ratio increased across all measurement heights in the course of the rain-related downdrafts. Following the O3 enhancement by up to a factor of 2, NO, NO2, and isoprene mixing ratios decreased. The temporal and vertical variability of the trace gases is intricately linked to the diverse sink and source processes, surface fluxes, and free-troposphere transport. Within the canopy, several interactions unfold among soil, atmosphere, and plants, shaping the overall dynamics. Also, the mixing ratio of biogenic VOCs (BVOCs) clearly varied with rainfall, driven by factors such as light, temperature, physical transport, and soil processes. Our results disentangle the patterns in the trace gas mixing ratio in the course of sudden and vigorous atmospheric mixing during rainfall events. By selectively uncovering processes that are not clearly detectable under undisturbed conditions, our results contribute to a better understanding of the trace gas life cycle and its interplay with meteorology, cloud dynamics, and rainfall in the Amazon.

The wet-season atmosphere in the central Amazon resembles natural conditions with minimal anthropogenic influence, making it one of the rare preindustrial-like continental areas worldwide. Previous long-term studies have analyzed the properties and sources of the natural Amazonian background aerosol. However, the vertical profile of the planetary boundary layer (PBL) has not been assessed systematically. Since 2017, such a profile assessment has been possible with the 325 m high tower at the Amazon Tall Tower Observatory (ATTO), located in a largely untouched primary forest in the central Amazon. This study investigates the variability of submicrometer aerosol concentration, size distribution, and optical properties at 60 and 325 m in the Amazonian PBL. The results show significant differences in aerosol volumes and scattering coefficients in the vertical gradient. The aerosol population was well-mixed throughout the boundary layer during the daytime but became separated upon stratification during the nighttime. We also found a significant difference in the spectral dependence of the scattering coefficients between the two heights. The analysis of downdrafts and the related rainfall revealed changes in the aerosol populations before and after rain events, with absorption and scattering coefficients decreasing as optically active particles are removed by wet deposition. The recovery of absorption and scattering coefficients is faster at 325 m than at 60 m. Convective events were concomitant with rapid increases in the concentrations of sub-50 nm particles, which were likely associated with downdrafts. We found that the aerosol population near the canopy had a significantly higher mass scattering efficiency than at 325 m. There was also a clear spectral dependence, with values for λ=450, 525, and 635 nm of 7.74±0.12, 5.49±0.11, and 4.15±0.11 m2 g−1, respectively, at 60 m, while at 325 m the values were 5.26±0.06, 3.76±0.05, and 2.46±0.04 m2 g−1, respectively. The equivalent aerosol refractive index results, which were obtained for the first time for the wet season in the central Amazon, show slightly higher scattering (real) components at 60 m compared to 325 m of 1.33 and 1.27, respectively. In contrast, the refractive index's absorptive (imaginary) component was identical for both heights, at 0.006. This study shows that the aerosol physical properties at 60 and 325 m are different, likely due to aging processes, and strongly depend on the photochemistry, PBL dynamics, and aerosol sources. These findings provide valuable insights into the impact of aerosols on climate and radiative balance and can be used to improve the representation of aerosols in global climate models.

This study introduces a first glance at Amazonian aerosols in the N–Dg–σ phase space. Aerosol data, measured from May 2021 to April 2022 at the Amazon Tall Tower Observatory (ATTO), were fitted by a multi-modal lognormal function and separated into three modes: the sub-50 nm, the Aitken (50–100 nm), and the accumulation modes. The fit results were then evaluated in the N–Dg–σ phase space, which represents a three-dimensional space based on the three lognormal fit parameters. These parameters represent, for a given mode i, the number concentration (Ni), the median geometric diameter (Dg,i), and the geometric standard deviation (σi). Each state of a particle number size distribution (PNSD) is represented by a single dot in this space, while a collection of dots shows the delimitation of all PNSD states under given conditions. The connections in ensembles of data points show trajectories caused by pseudo-forces, such as precipitation regimes and vertical movement. We showed that all three modes have a preferential arrangement in this space, reflecting their intrinsic behaviors in the atmosphere. These arrangements were interpreted as volumetric figures, elucidating the boundaries of each mode. Time trajectories in seasonal and diurnal cycles revealed that fits with the sub-20 nm mode are associated with rainfall events that happen in the morning and in the afternoon. But in the morning they grow rapidly into the Aitken mode, and in the afternoon they remain below 50 nm. Also, certain modes demonstrated well-defined curves in the space, e.g., the seasonal trajectory of the accumulation mode follows an ellipsoid, while the diurnal cycle of the sub-50 nm mode in the dry season follows a linear trajectory. As an effect of the precipitation on the PNSDs and vice versa, N and Dg were found to increase for the sub-50 nm mode and to decrease for the Aitken and accumulation modes after the precipitation peak. Afternoons with precipitation were preceded by mornings with larger particles of the accumulation mode, whose Dg was ∼ 10 nm larger than in days without precipitation. Nevertheless, this large Dg in the morning seems to influence subsequent rainfall only in the dry season, while in the wet season both N and Dg seem to have the same weight of influence. The observed patterns of the PNSDs in the N–Dg–σ phase space showed to be a promising tool for the characterization of atmospheric aerosols, to contribute to our understanding of the main processes in aerosol–cloud interactions, and to open new perspectives on aerosol parameterizations and model validation.

AbstractSmoke 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.

Abstract. Nucleation and condensation associated with biogenicvolatile organic compounds (BVOCs) are important aerosol formation pathways,yet their contribution to the upper-tropospheric aerosols remainsinconclusive, hindering the understanding of aerosol climate effects. Here,we develop new schemes describing these organic aerosol formation processesin the WRF-Chem model and investigate their impact on the abundance of cloudcondensation nuclei (CCN) in the upper troposphere (UT) over the AmazonBasin. We find that the new schemes significantly increase the simulated CCNnumber concentrations in the UT (e.g., up to ∼ 400 cm−3at 0.52 % supersaturation) and greatly improve the agreement with theaircraft observations. Organic condensation enhances the simulated CCNconcentration by 90 % through promoting particle growth, while organicnucleation, by replenishing new particles, contributes an additional 14 %.Deep convection determines the rate of these organic aerosol formationprocesses in the UT through controlling the upward transport of biogenicprecursors (i.e., BVOCs). This finding emphasizes the importance of thebiosphere–atmosphere coupling in regulating upper-tropospheric aerosolconcentrations over the tropical forest and calls for attention to itspotential role in anthropogenic climate change.

Abstract Natural aerosol feedbacks are expected to become more important in the future, as anthropogenic aerosol emissions decrease due to air quality policy. One such feedback is initiated by the increase in biogenic volatile organic compound (BVOC) emissions with higher temperatures, leading to higher secondary organic aerosol (SOA) production and a cooling of the surface via impacts on cloud radiative properties. Motivated by the considerable spread in feedback strength in Earth System Models (ESMs), we here use two long-term observational datasets from boreal and tropical forests, together with satellite data, for a process-based evaluation of the BVOC-aerosol-cloud feedback in four ESMs. The model evaluation shows that the weakest modelled feedback estimates can likely be excluded, but highlights compensating errors making it difficult to draw conclusions of the strongest estimates. Overall, the method of evaluating along process chains shows promise in pin-pointing sources of uncertainty and constraining modelled aerosol feedbacks.

Abstract The climate effects of atmospheric aerosol particles serving as cloud condensation nuclei (CCN) depend on chemical composition and hygroscopicity, which are highly variable on spatial and temporal scales. Here we present global CCN measurements, covering diverse environments from pristine to highly polluted conditions. We show that the effective aerosol hygroscopicity, κ, can be derived accurately from the fine aerosol mass fractions of organic particulate matter (ϵ org) and inorganic ions (ϵ inorg) through a linear combination, κ = ϵ org ⋅ κ org + ϵ inorg ⋅ κ inorg. In spite of the chemical complexity of organic matter, its hygroscopicity is well captured and represented by a global average value of κ org = 0.12 ± 0.02 with κ inorg = 0.63 ± 0.01 as the corresponding value for inorganic ions. By showing that the sensitivity of global climate forcing to changes in κ org and κ inorg is small, we constrain a critically important aspect of global climate modelling.

The Amazon Basin is frequently influenced by transatlantic transport of African dust plumes during its wet season (January–April), which not only interrupts the near-pristine atmospheric condition in that season, but also provides nutrient inputs to the Amazon rainforest upon deposition. In this study, we use the chemical transport model GEOS-Chem to investigate the impact of the export of African mineral dust to the Amazon Basin during the period of 2013–2017, constrained by multiple datasets obtained from the AErosol RObotic NETwork (AERONET), MODIS, as well as the Cayenne site and the Amazon Tall Tower Observatory (ATTO) site in the Amazon Basin. With an optimized particle mass size distribution (PMSD) of dust aerosols, the model captures observed aerosol optical depth (AOD) well in terms of both the mean value and the decline rate of the logarithm of AOD over the Atlantic Ocean along the transport path (AOaTP), implying consistency with the observed export efficiency of African dust along the transatlantic transport. With an annual emission of 0.73±0.12 Pg yr−1, African dust entering the Amazon Basin during the wet season accounts for 40±4.5 % (up to 70 %) of surface aerosol mass concentrations over the basin. Observed dust peaks over the Amazon Basin are generally associated with relatively higher African dust emissions (including the Sahara and the Sahel) and longer lifetimes of dust along the transatlantic transport, i.e., higher export efficiency of African dust across the Atlantic Ocean. The frequency of dust events during the wet season is around 18 % when averaged over the Amazon Basin, with maxima of over 60 % at the northeastern coast. During the dust events, AOD over most of the Amazon Basin is dominated by dust. Based on dust deposition, we further estimate annual inputs of 52±8.7, 0.97±0.16, and 21±3.6 mg m−2 yr−1 for iron, phosphorus, and magnesium, respectively, into the Amazon rainforest, which may to some extent compensate for the hydrologic losses of nutrients in the forest ecosystem.

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.

Abstract A study on aerosols in the Brazilian subequatorial Amazon region, Tangará da Serra (TS) and Alta Floresta (AF) was conducted and compared to findings in an additional site with background characteristics (Manaus, AM). TS and AF counties suffer from intense biomass burning periods in the dry season, and it accounts for high levels of particles in the atmosphere. Chemical characterization of fine and coarse particulate matter (PM) was performed to quantify water-soluble ions (WSI) and black carbon (BC). The importance of explanatory variables was assessed using three machine learning techniques. Average concentrations of PM in AF and TS were similar (PM2.0, 17±10 µg m-3 (AF) and 16±11 µg m-3 (TS) and PM10-2.0, 13±5 µg m-3 (AF) and 11±7 µg m-3 (TS)), but higher than the background site. BC and SO4 2- were the prevalent components as they represented 27%–68% of particulates chemical composition. The combination of the machine learning techniques provided a further understanding of the pathways for PM concentration variability, and the results highlighted the influence of biomass burning for key sample groups and periods. PM2.0, BC, and most WSI presented higher concentrations in the dry season, providing further support for the influence of biomass burning.

Abstract Interactions between atmospheric aerosols, clouds, and precipitation impact Earth's radiative balance and air quality, yet remain poorly constrained. Precipitating clouds serve as major sinks for particulate matter, but recent studies suggest that precipitation may also act as a particle source. The magnitude of the sources versus sinks, particularly for cloud condensation nuclei (CCN) numbers, remain unquantified. This study analyzes multi‐year in situ observations from tropical and boreal forests, as well as Arctic marine environment, showing links between recent precipitation and enhanced particle concentrations, including CCN‐sized particles. In some cases, the magnitude of precipitation‐related source equals or surpasses corresponding removal effect. Our findings highlight the importance of cloud‐processed material in determining near‐surface particle concentrations and the value of long‐term in situ observations for understanding aerosol particle life cycle. Robust patterns emerge from sufficiently long data series, allowing for quantitative assessment of the large‐scale significance of new phenomena observed in case studies.

Dimethyl sulfide (DMS) is the primary natural contributor to the atmospheric sulfur burden. Observations concerning the fate of DMS oxidation products after long-range transport in the remote free troposphere are, however, sparse. Here we present quantitative chemical ionization mass spectrometric measurements of DMS and its oxidation products sulfuric acid (H2SO4), methanesulfonic acid (MSA), dimethylsulfoxide (DMSO), dimethylsulfone (DMSO2), methanesulfinic acid (MSIA), methyl thioformate (MTF), methanesulfenic acid (MSEA, CH3SOH), and a compound of the likely structure CH3S(O)2OOH in the gas phase, as well as measurements of the sulfate and methanesulfonate aerosol mass fractions. The measurements were performed at the Global Atmosphere Watch (GAW) station Chacaltaya in the Bolivian Andes located at 5240 m above sea level (a.s.l.). DMS and DMS oxidation products are brought to the Andean high-altitude station by Pacific air masses during the dry season after convective lifting over the remote Pacific ocean to 6000–8000 m a.s.l. and subsequent long-range transport in the free troposphere (FT). Most of the DMS reaching the station is already converted to the rather unreactive sulfur reservoirs DMSO2 in the gas phase and methanesulfonate (MS−) in the particle phase, which carried nearly equal amounts of sulfur to the station. The particulate sulfate at Chacaltaya is however dominated by regional volcanic emissions during the time of the measurement and not significantly affected by the marine air masses. In one of the FT events, even some DMS was observed next to reactive intermediates such as methyl thioformate, dimethylsulfoxide, and methanesulfinic acid. Also for this event, back trajectory calculations show that the air masses came from above the ocean (distance >330 km) with no local surface contacts. This study demonstrates the potential impact of marine DMS emissions on the availability of sulfur-containing vapors in the remote free troposphere far away from the ocean.

Nucleation and condensation associated with biogenic volatile organic compounds (BVOCs) are important aerosol formation pathways, yet their contribution to the upper-tropospheric aerosols remains inconclusive, hindering the understanding of aerosol climate effects. Here, we develop new schemes describing these organic aerosol formation processes in the WRF-Chem model and investigate their impact on the abundance of cloud condensation nuclei (CCN) in the upper troposphere (UT) over the Amazon Basin. We find that the new schemes significantly increase the simulated CCN number concentrations in the UT (e.g., up to ∼ 400 cm−3 at 0.52 % supersaturation) and greatly improve the agreement with the aircraft observations. Organic condensation enhances the simulated CCN concentration by 90 % through promoting particle growth, while organic nucleation, by replenishing new particles, contributes an additional 14 %. Deep convection determines the rate of these organic aerosol formation processes in the UT through controlling the upward transport of biogenic precursors (i.e., BVOCs). This finding emphasizes the importance of the biosphere–atmosphere coupling in regulating upper-tropospheric aerosol concentrations over the tropical forest and calls for attention to its potential role in anthropogenic climate change.

This study analyses and quantifies the effects of vertical wind shear (VWS) on the properties of shallow cumulus cloud fields over Central Amazonia. We perform idealised simulations with high resolution (50 m horizontally and 20 m vertically) using the Dutch Atmospheric Large-Eddy Simulation (DALES) model, changing the initial conditions and large-scale forcing of VWS. The resulting cloud field is analysed by applying a cloud tracking algorithm to generate Lagrangian datasets of the life cycle of individual clouds as well as their time-varying core and margin dimensions. The reference run has no wind speed or directional shear and represents a typical day in the local dry season. Numerical experiments with moderate and high wind speed shear are simulated by adding linear increases in the wind speed of 1.2 and 2.4 m s−1 km−1, respectively. Three additional runs are made by adding 90∘ of wind rotation between the surface and the top of the domain (5 km) on top of the three wind speed shear conditions. We find that clouds developing in a sheared environment have horizontal equivalent diameter increased by up to 100 m on average, but the cloud depth is reduced. Our quantification shows that VWS tends to increase the size of the cloud cores but reduces their relative area, volume, and mass fractions compared to the overall cloud dimensions. The addition of 2.4 m s−1 km−1 of VWS decreases the relative core area by about 0.03 (about 10 % of the overall average) and its volume and mass ratios by about 0.05 (10 %–25 % in relative terms). Relevant for the cloud transport properties is that the updraught speed and the liquid water content are lower within the cores, and consequently so is the upward mass flux. All quantifications of mean cloud properties point to the inhibition of convective strength by VWS, therefore hampering the shallow-to-deep transition. However, open questions still remain given that the individually deepest clouds were simulated under high environmental shear, even though they occur in small numbers. This could indicate other indirect effects of VWS that have opposite effects on cloud development if found to be significant in the future.

One of the least understood aspects in atmospheric chemistry is how urban emissions influence the formation of natural organic aerosols, which affect Earth's energy budget. The Amazon rainforest, during its wet season, is one of the few remaining places on Earth where atmospheric chemistry transitions between preindustrial and urban-influenced conditions. Here, we integrate insights from several laboratory measurements and simulate the formation of secondary organic aerosols (SOA) in the Amazon using a high-resolution chemical transport model. Simulations show that emissions of nitrogen-oxides from Manaus, a city of ~2 million people, greatly enhance production of biogenic SOA by 60-200% on average with peak enhancements of 400%, through the increased oxidation of gas-phase organic carbon emitted by the forests. Simulated enhancements agree with aircraft measurements, and are much larger than those reported over other locations. The implication is that increasing anthropogenic emissions in the future might substantially enhance biogenic SOA in pristine locations like the Amazon.

In the Amazon basin, particles containing mixed sodium salts are routinely observed and are attributed to marine aerosols transported from the Atlantic Ocean. Using chemical imaging analysis, we show that, during the wet season, fungal spores emitted by the forest biosphere contribute at least 30% (by number) to sodium salt particles in the central Amazon basin. Hydration experiments indicate that sodium content in fungal spores governs their growth factors. Modeling results suggest that fungal spores account for ~69% (31-95%) of the total sodium mass during the wet season and that their fractional contribution increases during nighttime. Contrary to common assumptions that sodium-containing aerosols originate primarily from marine sources, our results suggest that locally-emitted fungal spores contribute substantially to the number and mass of coarse particles containing sodium. Hence, their role in cloud formation and contribution to salt cycles and the terrestrial ecosystem in the Amazon basin warrant further consideration.

New particle formation (NPF), referring to the nucleation of molecular clusters and their subsequent growth into the cloud condensation nuclei (CCN) size range, is a globally significant and climate-relevant source of atmospheric aerosols. Classical NPF exhibiting continuous growth from a few nanometers to the Aitken mode around 60–70 nm is widely observed in the planetary boundary layer (PBL) around the world but not in central Amazonia. Here, classical NPF events are rarely observed within the PBL, but instead, NPF begins in the upper troposphere (UT), followed by downdraft injection of sub-50 nm (CN) particles into the PBL and their subsequent growth. Central aspects of our understanding of these processes in the Amazon have remained enigmatic, however. Based on more than 6 years of aerosol and meteorological data from the Amazon Tall Tower Observatory (ATTO; February 2014 to September 2020), we analyzed the diurnal and seasonal patterns as well as meteorological conditions during 254 of such Amazonian growth events on 217 event days, which show a sudden occurrence of particles between 10 and 50 nm in the PBL, followed by their growth to CCN sizes. The occurrence of events was significantly higher during the wet season, with 88 % of all events from January to June, than during the dry season, with 12 % from July to December, probably due to differences in the condensation sink (CS), atmospheric aerosol load, and meteorological conditions. Across all events, a median growth rate (GR) of 5.2 nm h−1 and a median CS of 1.1 × 10−3 s−1 were observed. The growth events were more frequent during the daytime (74 %) and showed higher GR (5.9 nm h−1) compared to nighttime events (4.0 nm h−1), emphasizing the role of photochemistry and PBL evolution in particle growth. About 70 % of the events showed a negative anomaly of the equivalent potential temperature (Δθe′) – as a marker for downdrafts – and a low satellite brightness temperature (Tir) – as a marker for deep convective clouds – in good agreement with particle injection from the UT in the course of strong convective activity. About 30 % of the events, however, occurred in the absence of deep convection, partly under clear-sky conditions, and with a positive Δθe′ anomaly. Therefore, these events do not appear to be related to downdraft transport and suggest the existence of other currently unknown sources of sub-50 nm particles.

Biogenic volatile organic compounds (BVOCs) from the Amazon forest region represent the largest source of organic carbon emissions to the atmosphere globally. These BVOC emissions dominantly consist of volatile and intermediate-volatility terpenoid compounds that undergo chemical transformations in the atmosphere to form oxygenated condensable gases and secondary organic aerosol (SOA). We collected quartz filter samples with 12 h time resolution and performed hourly in situ measurements with a semi-volatile thermal desorption aerosol gas chromatograph (SV-TAG) at a rural site ("T3") located to the west of the urban center of Manaus, Brazil as part of the Green Ocean Amazon (GoAmazon2014/5) field campaign to measure intermediate-volatility and semi-volatile BVOCs and their oxidation products during the wet and dry seasons. We speciated and quantified 30 sesquiterpenes and 4 diterpenes with mean concentrations in the range 0.01-6.04 ngm-3 (1-670ppqv). We estimate that sesquiterpenes contribute approximately 14 and 12% to the total reactive loss of O3 via reaction with isoprene or terpenes during the wet and dry seasons, respectively. This is reduced from ~ 50-70 % for within-canopy reactive O3 loss attributed to the ozonolysis of highly reactive sesquiterpenes (e.g., β-caryophyllene) that are reacted away before reaching our measurement site. We further identify a suite of their oxidation products in the gas and particle phases and explore their role in biogenic SOA formation in the central Amazon region. Synthesized authentic standards were also used to quantify gas- and particle-phase oxidation products derived from β-caryophyllene. Using tracer-based scaling methods for these products, we roughly estimate that sesquiterpene oxidation contributes at least 0.4-5 % (median 1 %) of total submicron OA mass. However, this is likely a low-end estimate, as evidence for additional unaccounted sesquiterpenes and their oxidation products clearly exists. By comparing our field data to laboratory-based sesquiterpene oxidation experiments we confirm that more than 40 additional observed compounds produced through sesquiterpene oxidation are present in Amazonian SOA, warranting further efforts towards more complete quantification.

Nitrogen oxides (NO x ) emitted from human activities are believed to regulate the atmospheric oxidation capacity of the troposphere. However, observational evidence is limited for the low-to-median NO x concentrations prevalent outside of polluted regions. Directly measuring oxidation capacity, represented primarily by hydroxyl radicals (OH), is challenging, and the span in NO x concentrations at a single observation site is often not wide. Concentrations of isoprene and its photo-oxidation products were used to infer the equivalent noontime OH concentrations. The fetch at an observation site in central Amazonia experienced varied contributions from background regional air, urban pollution, and biomass burning. The afternoon concentrations of reactive nitrogen oxides (NO y ), indicative of NO x exposure during the preceding few hours, spanned from 0.3 to 3.5 parts per billion. Accompanying the increase of NO y concentration, the inferred equivalent noontime OH concentrations increased by at least 250% from 0.6 × 106 to 1.6 × 106 cm-3. The conclusion is that, compared to background conditions of low NO x concentrations over the Amazon forest, pollution increased NO x concentrations and amplified OH concentrations, indicating the susceptibility of the atmospheric oxidation capacity over the forest to anthropogenic influence and reinforcing the important role of NO x in sustaining OH concentrations.

This study evaluates the effect of weather events on the aerosol particle size distribution (PSD) at the Amazon Tall Tower Observatory (ATTO). This research combines in situ measurements of PSD and remote sensing data of lightning density, brightness temperature, cloud top height, cloud liquid water, and rain rate and vertical velocity. Measurements were obtained by scanning mobility particle sizers (SMPSs), the new generation of GOES satellites (GOES-16), the SIPAM S-band radar and the LAP 3000 radar wind profiler recently installed at the ATTO-Campina site. The combined data allow exploring changes in PSD due to different meteorological processes. The average diurnal cycle shows a higher abundance of ultrafine particles (NUFP) in the early morning, which is coupled with relatively lower concentrations in Aitken (NAIT) and accumulation (NACC) mode particles. From the early morning to the middle of the afternoon, an inverse behavior is observed, where NUFP decreases and NAIT and NACC increase, reflecting a typical particle growth process. Composite figures show an increase of NUFP before, during and after lightning was detected by the satellite above ATTO. These findings strongly indicate a close relationship between vertical transport and deep convective clouds. Lightning density is connected to a large increase in NUFP, beginning approximately 100 min before the maximum lightning density and reaching peak values around 200 min later. In addition, the removal of NACC by convective transport was found. Both the increase in NUFP and the decrease in NACC appear in parallel with the increasing intensity of lightning activity. The NUFP increases exponentially with the thunderstorm intensity. In contrast, NAIT and NACC show a different behavior, decreasing from approximately 100 min before the maximum lightning activity and reaching a minimum at the time of maximum lightning activity. The effect of cloud top height, cloud liquid water and rain rate shows the same behavior, but with different patterns between seasons. The convective processes do not occur continually but are probably modulated by gravity waves in the range of 1 to 5 h, creating a complex mechanism of interaction with a succession of updrafts and downdrafts, clouds, and clear-sky situations. The radar wind profiler measured the vertical distribution of the vertical velocity. These profiles show that downdrafts are mainly located below 10 km, while aircraft observations during the ACRIDICON–CHUVA campaign had shown maximum concentrations of ultrafine particles mainly above 10 km. Our study opens new scientific questions to be evaluated in order to understand the intricate physical and chemical mechanisms involved in the production of new particles in Amazonia.

Observations of aerosol and trace gases in the remote troposphere are vital to quantify background concentrations and identify long-term trends in atmospheric composition on large spatial scales. Measurements made at high altitude are often used to study free-tropospheric air; however such high-altitude sites can be influenced by boundary layer air masses. Thus, accurate information on air mass origin and transport pathways to high-altitude sites is required. Here we present a new method, based on the source–receptor relationship (SRR) obtained from backwards WRF-FLEXPART simulations and a k-means clustering approach, to identify source regions of air masses arriving at measurement sites. Our method is tailored to areas of complex terrain and to stations influenced by both local and long-range sources. We have applied this method to the Chacaltaya (CHC) GAW station (5240 m a.s.l.; 16.35∘ S, 68.13∘ W) for the 6-month duration of the “Southern Hemisphere high-altitude experiment on particle nucleation and growth” (SALTENA) to identify where sampled air masses originate and to quantify the influence of the surface and the free troposphere. A key aspect of our method is that it is probabilistic, and for each observation time, more than one air mass (cluster) can influence the station, and the percentage influence of each air mass can be quantified. This is in contrast to binary methods, which label each observation time as influenced by either boundary layer or free-troposphere air masses. Air sampled at CHC is a mix of different provenance. We find that on average 9 % of the air, at any given observation time, has been in contact with the surface within 4 d prior to arriving at CHC. Furthermore, 24 % of the air has been located within the first 1.5 km above ground level (surface included). Consequently, 76 % of the air sampled at CHC originates from the free troposphere. However, pure free-tropospheric influences are rare, and often samples are concurrently influenced by both boundary layer and free-tropospheric air masses. A clear diurnal cycle is present, with very few air masses that have been in contact with the surface being detected at night. The 6-month analysis also shows that the most dominant air mass (cluster) originates in the Amazon and is responsible for 29 % of the sampled air. Furthermore, short-range clusters (origins within 100 km of CHC) have high temporal frequency modulated by local meteorology driven by the diurnal cycle, whereas the mid- and long-range clusters' (>200 km) variability occurs on timescales governed by synoptic-scale dynamics. To verify the reliability of our method, in situ sulfate observations from CHC are combined with the SRR clusters to correctly identify the (pre-known) source of the sulfate: the Sabancaya volcano located 400 km north-west from the station.

The Amazon rain forest plays a major role in global hydrological cycling, and biogenic aerosols are likely to influence the formation of clouds and precipitation. Information about the sources and altitude profiles of primary biological aerosol particles, however, is sparse. We used fluorescence in situ hybridization (FISH), a molecular biological staining technique largely unexplored in aerosol research, to investigate the sources and spatiotemporal distribution of Amazonian bioaerosols on the domain level. We found wet season bioaerosol number concentrations in the range of 1–5 × 105 m−3 accounting for > 70 % of the coarse mode aerosol. Eukaryotic and bacterial particles predominated, with fractions of ∼ 56 % and ∼ 26 % of the intact airborne cells. Archaea occurred at very low concentrations. Vertical profiles exhibit a steep decrease in bioaerosol numbers from the understory to 325 m height on the Amazon Tall Tower Observatory (ATTO), with a stronger decrease in Eukarya compared to Bacteria. Considering earlier investigations, our results can be regarded as representative for near-pristine Amazonian wet season conditions. The observed concentrations and profiles provide new insights into the sources and dispersion of different types of Amazonian bioaerosols as a solid basis for model studies on biosphere–atmosphere interactions such as bioprecipitation cycling.

We present the first incorporation of the Common Representative Intermediates version 2.2 tropospheric chemistry mechanism, CRI v2.2, combined with stratospheric chemistry, into the global chemistry–climate United Kingdom Chemistry and Aerosols (UKCA) model to give the CRI-Strat 2 mechanism. A rigorous comparison of CRI-Strat 2 with the earlier version, CRI-Strat, is performed in UKCA in addition to an evaluation of three mechanisms, CRI-Strat 2, CRI-Strat and the standard UKCA chemical mechanism, StratTrop v1.0, against a wide array of surface and airborne chemical data. CRI-Strat 2 comprises a state-of-the-art isoprene scheme, optimized against the Master Chemical Mechanism v3.3.1, which includes isoprene peroxy radical isomerization, HOx recycling through the addition of photolabile hydroperoxy aldehydes (HPALDs), and isoprene epoxy diol (IEPOX) formation. CRI-Strat 2 also features updates to several rate constants for the inorganic chemistry, including the reactions of inorganic nitrogen and O(1D). The update to the isoprene chemistry in CRI-Strat 2 increases OH over the lowest 500 m in tropical forested regions by 30 %–50 % relative to CRI-Strat, leading to an improvement in model–observation comparisons for surface OH and isoprene relative to CRI-Strat and StratTrop. Enhanced oxidants also cause a 25 % reduction in isoprene burden and an increase in oxidation fluxes of isoprene and other biogenic volatile organic compounds (BVOCs) at low altitudes with likely impacts on subsequent aerosol formation, atmospheric lifetime, and climate. By contrast, updates to the rate constants of O(1D) with its main reactants relative to CRI-Strat reduces OH in much of the free troposphere, producing a 2 % increase in the methane lifetime, and increases the tropospheric ozone burden by 8 %, primarily from reduced loss via O(1D)+H2O. The changes to inorganic nitrogen reaction rate constants increase the NOx burden by 4 % and shift the distribution of nitrated species closer to that simulated by StratTrop. CRI-Strat 2 is suitable for multi-decadal model integrations and the improved representation of isoprene chemistry provides an opportunity to explore the consequences of HOx recycling in the United Kingdom Earth System Model (UKESM1). This new mechanism will enable a re-evaluation of the impact of BVOCs on the chemical composition of the atmosphere and further probe the feedback between the biosphere and the climate.

In this work, the relationships between size and composition of submicron particles (PM1) were analyzed at an urban site in the Metropolitan Area of São Paulo (MASP), a megacity with about 21 million inhabitants. The measurements were carried out from 20 December 2016 to 15 March 2017. The chemical composition was measured with an Aerodyne Aerosol Chemical Speciation Monitor and size distribution with a TSI Scanning Mobility Particle Sizer 3082. PM1 mass concentrations in the MASP had an average mass concentration of 11.4 µg m−3. Organic aerosol (OA) dominated the PM1 composition (56 %), followed by sulfate (15 %) and equivalent black carbon (eBC, 13 %). Four OA classes were identified using positive matrix factorization: oxygenated organic aerosol (OOA, 40 % of OA), biomass burning organic aerosol (BBOA, 13 %), and two hydrocarbon-like OA components (a typical HOA related to vehicular emissions (16 %) and a second HOA (21 %) representing a mix of anthropogenic sources). Particle number concentrations averaged 12 100±6900 cm−3, dominated by the Aitken mode. The accumulation mode increased under relatively high-PM1 conditions, suggesting an enhancement of secondary organic aerosol (SOA) production. Conversely, the contribution of nucleation-mode particles was less dependent on PM1 levels, consistent with vehicular emissions. The relationship between aerosol size modes and PM1 composition was assessed by multilinear regression (MLR) models. Secondary inorganic aerosols were partitioned between Aitken and accumulation modes, related to condensation particle growth processes. Submicron mass loading in the accumulation mode was mostly associated with highly oxidized OOA and also traffic-related emissions. To the authors' knowledge, this is the first work that uses the MLR methodology to estimate the chemical composition of the different aerosol size modes. The chemical composition with size-dependent PM provides innovative information on the properties of both primary and secondary organic aerosols, as well as inorganic aerosols in a complex urban environment. The results emphasize the relevance of vehicular emissions to the air quality at MASP and highlight the key role of secondary processes on the PM1 ambient concentrations in the region since 56 % of PM1 mass loading was attributed to SOA and secondary inorganic aerosol.

The Green Ocean Amazon experiment – GoAmazon 2014–2015 – explored the interactions between natural biogenic forest emissions from central Amazonia and urban air pollution from Manaus. Previous GoAmazon 2014–2015 studies showed that nitrogen oxide (NOx = NO + NO2) and sulfur oxide (SOx) emissions from Manaus strongly interact with biogenic volatile organic compounds (BVOCs), affecting secondary organic aerosol (SOA) formation. In previous studies, ground-based and aircraft measurements provided evidence of SOA formation and strong changes in aerosol composition and properties. Aerosol optical properties also evolve, and their impacts on the Amazonian ecosystem can be significant. As particles age, some processes, such as SOA production, black carbon (BC) deposition, particle growth and the BC lensing effect change the aerosol optical properties, affecting the solar radiation flux at the surface. This study analyzes data and models SOA formation using the Weather Research and Forecasting with Chemistry (WRF-Chem) model to assess the spatial variability in aerosol optical properties as the Manaus plumes interact with the natural atmosphere. The following aerosol optical properties are investigated: single scattering albedo (SSA), asymmetry parameter (gaer), absorption Ångström exponent (AAE) and scattering Ångström exponent (SAE). These simulations were validated using ground-based measurements at three experimental sites, namely the Amazon Tall Tower Observatory – ATTO (T0a), downtown Manaus (T1), Tiwa Hotel (T2) and Manacapuru (T3), as well as the U.S. Department of Energy (DOE) Gulfstream 1 (G-1) aircraft flights. WRF-Chem simulations were performed over 7 d during March 2014. Results show a mean biogenic SOA (BSOA) mass enrichment of 512 % at the T1 site, 450 % in regions downwind of Manaus, such as the T3 site, and 850 % in areas north of the T3 site in simulations with anthropogenic emissions. The SOA formation is rather fast, with about 80 % of the SOA mass produced in 3–4 h. Comparing the plume from simulations with and without anthropogenic emissions, SSA shows a downwind reduction of approximately 10 %, 11 % and 6 % at the T1, T2 and T3 sites, respectively. Other regions, such as those further downwind of the T3 site, are also affected. The gaer values increased from 0.62 to 0.74 at the T1 site and from 0.67 to 0.72 at the T3 site when anthropogenic emissions are active. During the Manaus plume-aging process, a plume tracking analysis shows an increase in SSA from 0.91 close to Manaus to 0.98 160 km downwind of Manaus as a result of SOA production and BC deposition.

Local and regional modelling of NH3 surface exchange is required to quantify nitrogen deposition to, and emissions from, the biosphere. However, measurements and model parameterisations for many remote ecosystems – such as tropical rainforest – remain sparse. Using 1 month of hourly measurements of NH3 fluxes and meteorological parameters over a remote Amazon rainforest site (Amazon Tall Tower Observatory, ATTO), six model parameterisations based on a bidirectional, single-layer canopy compensation point resistance model were developed to simulate observations of NH3 surface exchange. Canopy resistance was linked to either relative humidity at the canopy level (RHz0′), vapour pressure deficit, or a parameter value based on leaf wetness measurements. The ratio of apoplastic NH4+ to H+ concentration, Γs, during this campaign was inferred to be 38.5 ± 15.8. The parameterisation that reproduced the observed net exchange of NH3 most accurately was the model that used a cuticular resistance (Rw) parameterisation based on leaf wetness measurements and a value of Γs=50 (Pearson correlation r=0.71). Conversely, the model that performed the worst at replicating measured NH3 fluxes used an Rw value modelled using RHz0′ and the inferred value of Γs=38.5 (r=0.45). The results indicate that a single-layer canopy compensation point model is appropriate for simulating NH3 fluxes from tropical rainforest during the Amazonian dry season and confirmed that a direct measurement of (a non-binary) leaf wetness parameter improves the ability to estimate Rw. Current inferential methods for determining Γs were noted as having difficulties in the humid conditions present at a rainforest site.

Two complementary techniques, Scanning Transmission X-ray Microscopy/Near Edge Fine Structure spectroscopy (STXM/NEXAFS) and Scanning Electron Microscopy/Energy Dispersive X-ray spectroscopy (SEM/EDX), have been quantitatively combined to characterize individual atmospheric particles. This pair of techniques was applied to particle samples at three sampling sites (ATTO, ZF2, and T3) in the Amazon basin as part of the Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) field campaign during the dry season of 2014. The combined data was subjected to k-means clustering using mass fractions of the following elements: C, N, O, Na, Mg, P, S, Cl, K, Ca, Mn, Fe, Ni, and Zn. Cluster analysis identified 12 particle types across different sampling sites and particle sizes. Samples from the remote Amazon Tall Tower Observatory (ATTO, also T0a) exhibited less cluster variety and fewer anthropogenic clusters than samples collected at the sites nearer to the Manaus metropolitan region, ZF2 (also T0t) or T3. Samples from the ZF2 site contained aged/anthropogenic clusters not readily explained by transport from ATTO or Manaus, possibly suggesting the effects of long range atmospheric transport or other local aerosol sources present during sampling. In addition, this data set allowed for recently established diversity parameters to be calculated. All sample periods had high mixing state indices (c) that were 0.5 μm having a Di of ~2.4 and

Isoprene dominates global non-methane volatile organic compound emissions, and impacts tropospheric chemistry by influencing oxidants and aerosols. Isoprene emission rates vary over several orders of magnitude for different plants, and characterizing this immense biological chemodiversity is a challenge for estimating isoprene emission from tropical forests. Here we present the isoprene emission estimates from aircraft eddy covariance measurements over the Amazonian forest. We report isoprene emission rates that are three times higher than satellite top-down estimates and 35% higher than model predictions. The results reveal strong correlations between observed isoprene emission rates and terrain elevations, which are confirmed by similar correlations between satellite-derived isoprene emissions and terrain elevations. We propose that the elevational gradient in the Amazonian forest isoprene emission capacity is determined by plant species distributions and can substantially explain isoprene emission variability in tropical forests, and use a model to demonstrate the resulting impacts on regional air quality.

The susceptibility of air quality, weather, terrestrial ecosystems, and climate to human activities was investigated in a tropical environment.

The occurrence of nonliquid and liquid physical states of submicron atmospheric particulate matter (PM) downwind of an urban region in central Amazonia was investigated. Measurements were conducted during two intensive operating periods (IOP1 and IOP2) that took place during the wet and dry seasons of the GoAmazon2014/5 campaign. Air masses representing variable influences of background conditions, urban pollution, and regional-and continental-scale biomass burning passed over the research site. As the air masses varied, particle rebound fraction, an indicator of physical state, was measured in real time at ground level using an impactor apparatus. Micrographs collected by transmission electron microscopy confirmed that liquid particles adhered, while nonliquid particles rebounded. Relative humidity (RH) was scanned to collect rebound curves. When the apparatus RH matched ambient RH, 95ĝ€% of the particles adhered as a campaign average. Secondary organic material, produced for the most part by the oxidation of volatile organic compounds emitted from the forest, produces liquid PM over this tropical forest. During periods of anthropogenic influence, by comparison, the rebound fraction dropped to as low as 60ĝ€% at 95ĝ€% RH. Analyses of the mass spectra of the atmospheric PM by positive-matrix factorization (PMF) and of concentrations of carbon monoxide, total particle number, and oxides of nitrogen were used to identify time periods affected by anthropogenic influences, including both urban pollution and biomass burning. The occurrence of nonliquid PM at high RH correlated with these indicators of anthropogenic influence. A linear model having as output the rebound fraction and as input the PMF factor loadings explained up to 70ĝ€% of the variance in the observed rebound fractions. Anthropogenic influences can contribute to the presence of nonliquid PM in the atmospheric particle population through the combined effects of molecular species that increase viscosity when internally mixed with background PM and increased concentrations of nonliquid anthropogenic particles in external mixtures of anthropogenic and biogenic PM.

Airborne biological particles, such as fungal spores and pollen, are ubiquitous in the Earth's atmosphere and may influence the atmospheric environment and climate, impacting air quality, cloud formation, and the Earth's radiation budget. The atmospheric transformations of airborne biological spores at elevated relative humidity remain poorly understood and their climatic role is uncertain. Using an environmental scanning electron microscope (ESEM), we observed rupturing of Amazonian fungal spores and subsequent release of submicrometer size fragments after exposure to high humidity. We find that fungal fragments contain elements of inorganic salts (e.g., Na and Cl). They are hygroscopic in nature with a growth factor up to 2.3 at 96% relative humidity, thus they may potentially influence cloud formation. Due to their hygroscopic growth, light scattering cross sections of the fragments are enhanced by up to a factor of 10. Furthermore, rupturing of fungal spores at high humidity may explain the bursting events of new particle formation in Amazonia.

In the period between 9 and 11 July 2014, a friagem event reached the Amazon region. On 11 July, the southwest flow related to the friagem converged with the easterly winds in the central Amazon. The interaction between these two distinct air masses formed a convection band, which intensified over the Manaus region and the Amazon Tall Tower Observatory (ATTO) site. The satellite images show the evolution of convective activity on 11 July, which led to 21 mm of precipitation at the ATTO site. Moreover, the arrival of the friagem caused a sudden drop in temperature and a predominance of southerly winds, which could be seen in Porto Velho between 7 and 8 July and in Manaus and the ATTO site from 9 to 11 July. The results of ERA-Interim reanalysis and Brazilian developments on the Regional Atmospheric Modeling System (BRAMS) simulations show that this friagem event coming from the southwest, carries a mass of air with higher O3 and NO2 mixing ratios and lower CO mixing ratio compared to the air masses present in the central Amazon. At Lake Balbina, the friagem intensifies the local circulations, such as the breeze phenomena. In the Manaus region and at the ATTO site, the main effects of the friagem event are a decrease in the incoming solar radiation (due to intense cloud formation), a large temperature drop and a distinct change in surface O3 and CO2 mixing ratios. As the cold air of the friagem was just in the lower 500 m the most probable cause of this change is that a cold pool above the forest prevented vertical mixing causing accumulation of CO2 from respiration and very low O3 mixing ratio due to photochemistry reduction and limited mixing within the boundary layer.

The Amazon rainforest presents a unique, natural laboratory for the study of surface–atmosphere interactions. Its alternation between a near-pristine marine-influenced atmosphere during the wet season and a vulnerable system affected by periodic intrusions of anthropogenic pollution during the dry season provides an opportunity to investigate some fundamental aspects of boundary-layer chemical processes. This study presents the first simultaneous hourly measurements of concentrations, fluxes, and deposition velocities of the inorganic trace gases NH3, HCl, HONO, HNO3, and SO2 as well as their water-soluble aerosol counterparts NH4+, Cl−, NO2-, NO3- and SO42- over the Amazon. Species concentrations were measured in the dry season (from 6 October to 5 November 2017), at the Amazon Tall Tower Observatory (ATTO) in Brazil, using a two-point gradient wet-chemistry instrument (GRadient of AErosols and Gases Online Registration, GRAEGOR) sampling at 42 and 60 m. Fluxes and deposition velocities were derived from the concentration gradients using a modified form of the aerodynamic gradient method corrected for measurement within the roughness sub-layer. Findings from this campaign include observations of elevated concentrations of NH3 and SO2 partially driven by long-range transport (LRT) episodes of pollution and the substantial influence of coarse Cl− and NO3- particulate on overall aerosol mass burdens. From the flux measurements, the dry season budget of total reactive nitrogen dry deposition at the ATTO site was estimated as −2.9 kg N ha-1a-1. HNO3 and HCl were deposited continuously at a rate close to the aerodynamic limit. SO2 was deposited with an average daytime surface resistance (Rc) of 28 s m−1, whilst aerosol components showed average surface deposition velocities of 2.8 and 2.7 mm s−1 for SO42- and NH4+, respectively. Deposition rates of NO3- and Cl− were higher at 7.1 and 7.8 mm s−1, respectively, reflecting their larger average size. The exchange of NH3 and HONO was bidirectional, with NH3 showing emission episodes in the afternoon and HONO in the early morning hours. This work provides a unique dataset to test and improve dry deposition schemes for these compounds for tropical rainforest, which have typically been developed by interpolation from conditions in temperate environments. A future campaign should focus on making similar measurements in the wet season in order to provide a complete view of the annual pattern of inorganic trace gas and coarse aerosol biosphere–atmosphere exchange over tropical rainforest.

Ice particle activation and evolution have important atmospheric implications for cloud formation, initiation of precipitation and radiative interactions. The initial formation of atmospheric ice by heterogeneous ice nucleation requires the presence of a nucleating seed, an ice-nucleating particle (INP), to facilitate its first emergence. Unfortunately, only a few long-term measurements of INPs exist, and as a result, knowledge about geographic and seasonal variations of INP concentrations is sparse. Here we present data from nearly 2 years of INP measurements from four stations in different regions of the world: the Amazon (Brazil), the Caribbean (Martinique), central Europe (Germany) and the Arctic (Svalbard). The sites feature diverse geographical climates and ecosystems that are associated with dissimilar transport patterns, aerosol characteristics and levels of anthropogenic impact (ranging from near pristine to mostly rural). Interestingly, observed INP concentrations, which represent measurements in the deposition and condensation freezing modes, do not differ greatly from site to site but usually fall well within the same order of magnitude. Moreover, short-term variability overwhelms all long-term trends and/or seasonality in the INP concentration at all locations. An analysis of the frequency distributions of INP concentrations suggests that INPs tend to be well mixed and reflective of large-scale air mass movements. No universal physical or chemical parameter could be identified to be a causal link driving INP climatology, highlighting the complex nature of the ice nucleation process. Amazonian INP concentrations were mostly unaffected by the biomass burning season, even though aerosol concentrations increase by a factor of 10 from the wet to dry season. Caribbean INPs were positively correlated to parameters related to transported mineral dust, which is known to increase during the Northern Hemisphere summer. A wind sector analysis revealed the absence of an anthropogenic impact on average INP concentrations at the site in central Europe. Likewise, no Arctic haze influence was observed on INPs at the Arctic site, where low concentrations were generally measured. We consider the collected data to be a unique resource for the community that illustrates some of the challenges and knowledge gaps of the field in general, while specifically highlighting the need for more long-term observations of INPs worldwide.

resumo Estamos entrando em uma era em que nosso planeta e nossa sociedade estão enfrentando crises importantes. Convivemos simultaneamente com três emergências importantes: 1) a crise na saúde, intensificada com a pandemia da Covid-19; 2) a crise de perda de biodiversidade; e 3) a emergência climática. Salienta-se que essas crises têm ligações profundas entre si, e diferenças também importantes, mas todas provocam impactos sociais e econômicos fortes e afetam o planeta globalmente. Elas são resultado de um modelo econômico que privilegia o desenvolvimento a qualquer custo, o lucro muito rápido, mesmo à custa da sustentabilidade. A crise da Covid-19 colocou questões importantes do ponto de vista de falta de governança global. Por sua vez, a crise climática tem potencial para danos socioeconômicos muito fortes, e seus efeitos já são facilmente visíveis. A perda de biodiversidade coloca em risco nossa segurança alimentar, bem como o equilíbrio do sistema terrestre. A Amazônia, por exemplo, contém milhares de vírus em sua fauna e flora, e a continuar o processo desenfreado de sua ocupação, novos vírus similares ao Sars-CoV-2 possivelmente entrarão em contato com nossa sociedade. Sair dessas três crises requer mudanças drásticas em nosso sistema econômico, insustentável em seu formato atual. Crescimento econômico contínuo em um planeta com recursos naturais finitos não é possível. A desigualdade em países em desenvolvimento e mesmo estre nações é explosiva e injusta. Precisaremos de um novo sistema de governança global que seja capaz de harmonizar medidas dos diferentes países, estados e municípios. A sustentabilidade em nosso planeta é possível e necessária. Teremos muito trabalho em construí-la nos próximos anos, comunidade científica, sociedade, governos e outros agentes. Não temos alternativas senão construir uma nova sociedade, mais justa e sustentável.

Biomass burning (BB) aerosols can influence regional and global climate through interactions with radiation, clouds, and precipitation. Here, we investigate the impact of BB aerosols on the energy balance and hydrological cycle over the Amazon Basin during the dry season. We performed simulations with a fully coupled meteorology–chemistry model, the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem), for a range of different BB emission scenarios to explore and characterize nonlinear effects and individual contributions from aerosol–radiation interactions (ARIs) and aerosol–cloud interactions (ACIs). The ARIs of BB aerosols tend to suppress low-level liquid clouds by local warming and increased evaporation and to facilitate the formation of high-level ice clouds by enhancing updrafts and condensation at high altitudes. In contrast, the ACIs of BB aerosol particles tend to enhance the formation and lifetime of low-level liquid clouds by providing more cloud condensation nuclei (CCN) and to suppress the formation of high-level ice clouds by reducing updrafts and condensable water vapor at high altitudes (>8 km). For scenarios representing the lower and upper limits of BB emission estimates for recent years (2002–2016), we obtained total regional BB aerosol radiative forcings of −0.2 and 1.5 W m−2, respectively, showing that the influence of BB aerosols on the regional energy balance can range from modest cooling to strong warming. We find that ACIs dominate at low BB emission rates and low aerosol optical depth (AOD), leading to an increased cloud liquid water path (LWP) and negative radiative forcing, whereas ARIs dominate at high BB emission rates and high AOD, leading to a reduction of LWP and positive radiative forcing. In all scenarios, BB aerosols led to a decrease in the frequency of occurrence and rate of precipitation, caused primarily by ACI effects at low aerosol loading and by ARI effects at high aerosol loading. The dependence of precipitation reduction on BB aerosol loading is greater in a strong convective regime than under weakly convective conditions. Overall, our results show that ACIs tend to saturate at high aerosol loading, whereas the strength of ARIs continues to increase and plays a more important role in highly polluted episodes and regions. This should hold not only for BB aerosols over the Amazon, but also for other light-absorbing aerosols such as fossil fuel combustion aerosols in industrialized and densely populated areas. The importance of ARIs at high aerosol loading highlights the need for accurately characterizing aerosol optical properties in the investigation of aerosol effects on clouds, precipitation, and climate.

The Amazon basin is important for understanding the global climate because of its carbon cycle and as a laboratory for obtaining basic knowledge of the continental background atmosphere. Aerosol particles play an important role in the climate and weather, and knowledge of their compositions and mixing states is necessary to understand their influence on the climate. For this study, we collected aerosol particles from the Amazon basin during the Green Ocean Amazon (GoAmazon2014/5) campaign (February to March 2014) at the T3 site, which is located about 70 km from Manaus, and analyzed them using transmission electron microscopy (TEM). TEM has better spatial resolution than other instruments, which enables us to analyze the occurrences of components that attach to or are embedded within other particles. Based on the TEM results of more than 10 000 particles from several transport events, this study shows the occurrences of individual particles including compositions, size distributions, number fractions, and possible sources of materials that mix with other particles. Aerosol particles during the wet season were from both natural sources such as the Amazon forest, Saharan desert, Atlantic Ocean, and African biomass burning and anthropogenic sources such as Manaus and local emissions. These particles mix together at an individual particle scale. The number fractions of mineral dust and sea-salt particles increased almost 3-fold when long-range transport (LRT) from the African continent occurred. Nearly 20 % of mineral dust and primary biological aerosol particles had attached sea salts on their surfaces. Sulfates were also internally mixed with sea-salt and mineral dust particles. The TEM element mapping images showed that several components with sizes of hundreds of nanometers from different sources commonly occur within individual LRT aerosol particles. We conclude that many aerosol particles from natural sources change their compositions by mixing during transport. The compositions and mixing states of these particles after emission result in changes in their hygroscopic and optical properties and should be considered when assessing their effects on climate.

This review presents how the boreal and the tropical forests affect the atmosphere, its chemical composition, its function, and further how that affects the climate and, in return, the ecosystems through feedback processes. Observations from key tower sites standing out due to their long-term comprehensive observations: The Amazon Tall Tower Observatory in Central Amazonia, the Zotino Tall Tower Observatory in Siberia, and the Station to Measure Ecosystem-Atmosphere Relations at Hyytiäla in Finland. The review is complemented by short-term observations from networks and large experiments. The review discusses atmospheric chemistry observations, aerosol formation and processing, physiochemical aerosol, and cloud condensation nuclei properties and finds surprising similarities and important differences in the two ecosystems. The aerosol concentrations and chemistry are similar, particularly concerning the main chemical components, both dominated by an organic fraction, while the boreal ecosystem has generally higher concentrations of inorganics, due to higher influence of long-range transported air pollution. The emissions of biogenic volatile organic compounds are dominated by isoprene and monoterpene in the tropical and boreal regions, respectively, being the main precursors of the organic aerosol fraction. Observations and modeling studies show that climate change and deforestation affect the ecosystems such that the carbon and hydrological cycles in Amazonia are changing to carbon neutrality and affect precipitation downwind. In Africa, the tropical forests are so far maintaining their carbon sink. It is urgent to better understand the interaction between these major ecosystems, the atmosphere, and climate, which calls for more observation sites, providing long-term data on water, carbon, and other biogeochemical cycles. This is essential in finding a sustainable balance between forest preservation and reforestation versus a potential increase in food production and biofuels, which are critical in maintaining ecosystem services and global climate stability. Reducing global warming and deforestation is vital for tropical forests.