Aerosol and precipitation chemistry in a remote site in Central Amazonia: the role of biogenic contribution

International audienceA long-term (2?3 years) measurement of aerosol and precipitation chemistry was carried out in a remote site in Central Amazonia, Balbina, (1°55' S, 59°29' W, 174 m above sea level), about 200 km north of Manaus city. Aerosols were sampled using stacked filter units (SFU), which separate fine (d<2.5 ?m) and coarse mode (2.5 ?

Non-deforestation drivers of fires are increasingly important sources of aerosol and carbon dioxide emissions across Amazonia

Deforestation rates have declined substantially across the Brazilian Legal Amazon (BLA) over the period from 2000–2017. However, reductions in fire, aerosol and carbon dioxide have been far less significant than deforestation, even when accounting for inter-annual variability in precipitation. Our observations and analysis support a decoupling between fire and deforestation that has exacerbated forest degradation in the BLA. Basing aerosol and carbon dioxide emissions on deforestation rates, without accounting for forest degradation will bias these important climate and ecosystem-health parameters low, both now and in the future. Recent increases in deforestation rate since 2014 will enhance such degradation, particularly during drought-conditions, increasing emissions of aerosol and greenhouse gases. Given Brazil’s committed Nationally Determined Contribution under the Paris Agreement, failure to account for forest degradation fires will paint a false picture of prior progress and potentially have profound implications for both regional and global climate

Chemical transformations in organic aerosol from biomass burning

International audienceFine aerosol particles were collected separately during daytime and nighttime at a tropical pasture site in Rondônia, Brazil, during the burning and dry-to-wet transition period in 2002. Total carbon (TC) and water-soluble organic carbon (WSOC) were measured by evolved gas analysis (EGA). Based on the thermochemical properties of the fine aerosol, the relative amounts of the low and higher molecular weight compounds were estimated. It was found that the thermally refractory (possibly higher molecular weight) compounds dominated the TC composition. Their contribution to TC was higher in the daytime samples than in the nighttime ones. The relative share of WSOC also showed a statistically significant diel variation and so did its refractory fraction. Anhydrosugars and phenolic acids were determined by GC-MS and their diel variation was studied. Based on the decrease of their relative concentrations between the biomass burning and transition periods and their distinctly different diel variations, we suggest that the phenolic acids may undergo chemical transformations in the aerosol phase, possibly towards more refractory compounds (humic-like substances, HULIS), as has been suggested previously. These conclusions are supported by the results of the thermally assisted hydrolysis and methylation gas chromatography-mass spectrometry of the same filter samples

Robust relations between CCN and the vertical evolution of cloud drop size distribution in deep convective clouds

International audienceIn-situ measurements in convective clouds (up to the freezing level) over the Amazon basin show that smoke from deforestation fires prevents clouds from precipitating until they acquire a vertical development of at least 4 km, compared to only 1?2 km in clean clouds. The average cloud depth required for the onset of warm rain increased by ~350 m for each additional 100 cloud condensation nuclei per cm3 at a super-saturation of 0.5% (CCN0.5%). In polluted clouds, the diameter of modal liquid water content grows much slower with cloud depth (at least by a factor of ~2), due to the large number of droplets that compete for available water and to the suppressed coalescence processes. Contrary to what other studies have suggested, we did not observe this effect to reach saturation at 3000 or more accumulation mode particles per cm3. The CCN0.5% concentration was found to be a very good predictor for the cloud depth required for the onset of warm precipitation and other microphysical factors, leaving only a secondary role for the updraft velocities in determining the cloud drop size distributions. The effective radius of the cloud droplets (re) was found to be a quite robust parameter for a given environment and cloud depth, showing only a small effect of partial droplet evaporation from the cloud's mixing with its drier environment. This supports one of the basic assumptions of satellite analysis of cloud microphysical processes: the ability to look at different cloud top heights in the same region and regard their re as if they had been measured inside one well developed cloud. The dependence of re on the adiabatic fraction decreased higher in the clouds, especially for cleaner conditions, and disappeared at re?~10 µm. We propose that droplet coalescence, which is at its peak when warm rain is formed in the cloud at re~10 µm, continues to be significant during the cloud's mixing with the entrained air, canceling out the decrease in re due to evaporation

Rapid formation of isoprene photo-oxidation products observed in Amazonia

Isoprene represents the single most important reactive hydrocarbon for atmospheric chemistry in the tropical atmosphere. It plays a central role in global and regional atmospheric chemistry and possible climate feedbacks. Photo-oxidation of primary hydrocarbons (e.g. isoprene) leads to the formation of oxygenated VOCs (OVOCs). The evolution of these intermediates affects the oxidative capacity of the atmosphere (by reacting with OH) and can contribute to secondary aerosol formation, a poorly understood process. An accurate and quantitative understanding of VOC oxidation processes is needed for model simulations of regional air quality and global climate. Based on field measurements conducted during the Amazonian Aerosol Characterization Experiment (AMAZE-08) we show that the production of certain OVOCs (e.g. hydroxyacetone) from isoprene photo-oxidation in the lower atmosphere is significantly underpredicted by standard chemistry schemes. Recently reported fast secondary production could explain 50% of the observed discrepancy with the remaining part possibly produced via a novel primary production channel, which has been proposed theoretically. The observations of OVOCs are also used to test a recently proposed HO&lt;sub&gt;x&lt;/sub&gt; recycling mechanism via degradation of isoprene peroxy radicals. If generalized our observations suggest that prompt photochemical formation of OVOCs and other uncertainties in VOC oxidation schemes could result in uncertainties of modelled OH reactivity, potentially explaining a fraction of the missing OH sink over forests which has previously been largely attributed to a missing source of primary biogenic VOCs

The effect of atmospheric aerosol particles and clouds on net ecosystem exchange in the Amazon

Carbon cycling in the Amazon is closely linked to atmospheric processes and climate in the region as a consequence of the strong coupling between the atmosphere and biosphere. This work examines the effects of changes in net radiation due to atmospheric aerosol particles and clouds on the net ecosystem exchange (NEE) of CO₂ in the Amazon region. Some of the major environmental factors affecting the photosynthetic activity of plants, such as air temperature and relative humidity, were also examined. An algorithm for clear-sky irradiance was developed and used to determine the relative irradiance, <i>f</i>, which quantifies the percentage of solar radiation absorbed and scattered due to atmospheric aerosol particles and clouds. Aerosol optical depth (AOD) was calculated from irradiances measured with the MODIS (Moderate Resolution Imaging Spectroradiometer) sensor, onboard the Terra and Aqua satellites, and was validated with ground-based AOD measurements from AERONET (Aerosol Robotic Network) sun photometers. Carbon fluxes were measured using eddy covariance technique at the Large-Scale Biosphere-Atmosphere Experiment in Amazonia (LBA) flux towers. Two sites were studied: the Jaru Biological Reserve (RBJ), located in Rondonia, and the Cuieiras Biological Reserve at the K34 LBA tower (located in a preserved region in the central Amazon). Analysis was performed continuously from 1999 to 2009 at K34 and from 1999 to 2002 at RBJ, and includes wet, dry and transition seasons. In the Jaru Biological Reserve, a 29% increase in carbon uptake (NEE) was observed when the AOD ranged from 0.10 to 1.5 at 550 nm. In the Cuieiras Biological Reserve, the aerosol effect on NEE was smaller, accounting for an approximate 20% increase in NEE. High aerosol loading (AOD above 3 at 550 nm) or high cloud cover leads to reductions in solar flux and strong decreases in photosynthesis up to the point where NEE approaches zero. The observed increase in NEE is attributed to an enhancement (~50%) in the diffuse fraction of photosynthetic active radiation (PAR). The enhancement in diffuse PAR can be done through increases in aerosols and/or clouds. In the present study, it was not possible to separate these two components. Significant changes in air temperature and relative humidity resulting from changes in solar radiation fluxes under high aerosol loading were also observed at both sites. Considering the long-range transport of aerosols in the Amazon, the observed changes in NEE for these two sites may occur over large areas in the Amazon, significantly altering the carbon balance in the largest rainforest in the world

Biomass burning related ozone damage on vegetation over the Amazon forest: A model sensitivity study

The HadGEM2 earth system climate model was used to assess the impact of biomass burning on surface ozone concentrations over the Amazon forest and its impact on vegetation, under present-day climate conditions. Here we consider biomass burning emissions from wildfires, deforestation fires, agricultural forest burning, and residential and commercial combustion. Simulated surface ozone concentration is evaluated against observations taken at two sites in the Brazilian Amazon forest for years 2010 to 2012. The model is able to reproduce the observed diurnal cycle of surface ozone mixing ratio at the two sites, but overestimates the magnitude of the monthly averaged hourly measurements by 5-15 ppb for each available month at one of the sites. We vary biomass burning emissions over South America by ±20, 40, 60, 80 and 100% to quantify the modelled impact of biomass burning on surface ozone concentrations and ozone damage on vegetation productivity over the Amazon forest. We used the ozone damage scheme in the "high" sensitivity mode to give an upper limit for this effect. Decreasing South American biomass burning emissions by 100% (i.e. to zero) reduces surface ozone concentrations (by about 15 ppb during the biomass burning season) and suggests a 15% increase in monthly mean net primary productivity averaged over the Amazon forest, with local increases up to 60%. The simulated impact of ozone damage from present-day biomass burning on vegetation productivity is about 230 TgC yr-1. Taking into account that uncertainty in these estimates is substantial, this ozone damage impact over the Amazon forest is of the same order of magnitude as the release of carbon dioxide due to fire in South America; in effect it potentially doubles the impact of biomass burning on the carbon cycle.This work was funded by the Natural Environment Research Council (NERC) South AMerican Biomass Burning Analysis (SAMBBA) project grant code NE/J010057/1. The UK Met Office contribution to this project was funded by the DECC under the Hadley Centre Climate Programme contract (GA01101). The Brazilian contribution was funded by Fundacao de Amparo a Pesquisa do Estado de Sao Paulo (FAPESP, projects 08/58100-2 and 12/14437-9). We thank INPA (Instituto Nacional de Pesquisas da Amazonia) for the coordination work of the LBA Experiment. We thank USP technicians for the support on data sampling: Alcides Ribeiro, Ana Lucia Loureiro, Fernando Morais and Fabio Jorge

A possible role of ground-based microorganisms on cloud formation in the atmosphere

The formation of clouds is an important process for the atmosphere, the hydrological cycle, and climate, but some aspects of it are not completely understood. In this work, we show that microorganisms might affect cloud formation without leaving the Earth's surface by releasing biological surfactants (or biosurfactants) in the environment, that make their way into atmospheric aerosols and could significantly enhance their activation into cloud droplets. <br><br> In the first part of this work, the cloud-nucleating efficiency of standard biosurfactants was characterized and found to be better than that of any aerosol material studied so far, including inorganic salts. These results identify molecular structures that give organic compounds exceptional cloud-nucleating properties. In the second part, atmospheric aerosols were sampled at different locations: a temperate coastal site, a marine site, a temperate forest, and a tropical forest. Their surface tension was measured and found to be below 30 mN/m, the lowest reported for aerosols, to our knowledge. This very low surface tension was attributed to the presence of biosurfactants, the only natural substances able to reach to such low values. <br><br> The presence of strong microbial surfactants in aerosols would be consistent with the organic fractions of exceptional cloud-nucleating efficiency recently found in aerosols, and with the correlations between algae bloom and cloud cover reported in the Southern Ocean. The results of this work also suggest that biosurfactants might be common in aerosols and thus of global relevance. If this is confirmed, a new role for microorganisms on the atmosphere and climate could be identified

Low molecular weight organic acids in aerosol particles from Rondônia, Brazil, during the biomass-burning, transition and wet periods

International audienceParticles from biomass burning and regional haze were sampled in Rondônia, Brazil, during dry, transition and wet periods from September to November 2002, as part of the LBA-SMOCC (Large-Scale Biosphere-Atmosphere Experiment in Amazonia ? Smoke, Aerosols, Clouds, Rainfall, and Climate) field campaign. Water soluble organic and inorganic compounds in bulk (High Volume and Stacked Filter Unit sampler) and size-resolved (Micro Orifice Uniform Deposit Impactor ? MOUDI) smoke samples were determined by ion chromatography. It was found that low molecular weight polar organic acids account for a significant fraction of the water soluble organic carbon (WSOC) in biomass burning aerosols (C2-C6 dicarboxylic acids reached up to 3.7% and one-ring aromatic acids reached up to 2% of fine fraction WSOC during burning period). Short dicarboxylic (C2-C6) acids are dominated by oxalic acid followed by malonic and succinic acids. The largest ionic species is ammonium sulfate (60?70% of ionic mass). It was found that most of the ionic mass is concentrated in submicrometer-sized particles. Based on the size distribution and correlations with K+, a known biomass burning tracer, it is suggested that many of the organic acids are directly emitted by vegetation fires. Concentrations of dicarboxylic acids in the front and back filters of high volume sampler were determined. Based on these measurements, it was concluded that in the neutral or slightly basic smoke particles typical of this region, dicarboxylic acids are mostly confined to the particulate phase. Finally, it is shown that the distribution of water soluble species shifts to larger aerosols sizes as the aerosol population ages and mixes with other aerosol types in the atmosphere

Size distribution and hygroscopic properties of aerosol particles from dry-season biomass burning in Amazonia

International audienceAerosol particle number size distributions and hygroscopic properties were measured at a pasture site in the southwestern Amazon region (Rondonia). The measurements were performed 11 September-14 November 2002 as part of LBA-SMOCC (Large scale Biosphere atmosphere experiment in Amazonia - SMOke aerosols, Clouds, rainfall and Climate), and cover the later part of the dry season (with heavy biomass burning), a transition period, and the onset of the wet period. Particle number size distributions were measured with a DMPS (Differential Mobility Particle Sizer, 3-850nm) and an APS (Aerodynamic Particle Sizer), extending the distributions up to 3.3 µm in diameter. An H-TDMA (Hygroscopic Tandem Differential Mobility Analyzer) measured the hygroscopic diameter growth factors (Gf) at 90% relative humidity (RH), for particles with dry diameters (dp) between 20-440 nm, and at several occasions RH scans (30-90% RH) were performed for 165nm particles. These data provide the most extensive characterization of Amazonian biomass burning aerosol, with respect to particle number size distributions and hygroscopic properties, presented until now. The evolution of the convective boundary layer over the course of the day causes a distinct diel variation in the aerosol physical properties, which was used to get information about the properties of the aerosol at higher altitudes. The number size distributions averaged over the three defined time periods showed three modes; a nucleation mode with geometrical median diameters (GMD) of ~12 nm, an Aitken mode (GMD=61-92 nm) and an accumulation mode (GMD=128-190 nm). The two larger modes were shifted towards larger GMD with increasing influence from biomass burning. The hygroscopic growth at 90% RH revealed a somewhat external mixture with two groups of particles; here denoted nearly hydrophobic (Gf~1.09 for 100 nm particles) and moderately hygroscopic (Gf~1.26). While the hygroscopic growth factors were surprisingly similar over the periods, the number fraction of particles belonging to each hygroscopic group varied more, with the dry period aerosol being more dominated by nearly hydrophobic particles. As a result the total particle water uptake rose going into the cleaner period. The fraction of moderately hygroscopic particles was consistently larger for particles in the accumulation mode compared to the Aitken mode for all periods. Scanning the H-TDMA over RH (30-90% RH) showed no deliquescence behavior. A parameterization of both Gf(RH) and Gf(dp), is given