A large number of published and unpublished measurements of cloud condensation nuclei (CCN) concentrations and aerosol optical thickness (AOT) measurements have been analyzed. AOT measurements were ...obtained mostly from the AERONET network, and selected to be collocated as closely as possible to the CCN investigations. In remote marine regions, CCN0.4 (CCN at a supersaturation of 0.4%) are around 110 cm−3 and the mean AOT500 (AOT at 500 nm) is 0.057. Over remote continental areas, CCN are almost twice as abundant, while the mean AOT500 is ca. 0.075. (Sites dominated by desert dust plumes were excluded from this analysis.) Some, or maybe even most of this difference must be because even remote continental sites are in closer proximity to pollution sources than remote marine sites. This suggests that the difference between marine and continental levels must have been smaller before the advent of anthropogenic pollution. Over polluted marine and continental regions, the CCN concentrations are about one order of magnitude higher than over their remote counterparts, while AOT is about five times higher over polluted than over clean regions. The average CCN concentrations from all studies show a remarkable correlation to the corresponding AOT values, which can be expressed as a power law. This can be very useful for the parameterization of CCN concentrations in modeling studies, as it provides an easily measured proxy for this variable, which is difficult to measure directly. It also implies that, at least at large scales, the radiative and microphysical effects of aerosols on cloud physics are correlated and not free to vary fully independently. While the observed strong empirical correlation is remarkable, it must still be noted that there is about a factor-of-four range of CCN concentrations at a given AOT, and that there remains considerable room for improvement in remote sensing techniques for CCN abundance.
Since the publication of the compilation of biomass burning emission factors by Andreae and Merlet (2001), a large number of studies have greatly expanded the amount of available data on emissions ...from various types of biomass burning. Using essentially the same methodology as Andreae and Merlet (2001), this paper presents an updated compilation of emission factors. The data from over 370 published studies were critically evaluated and integrated into a consistent format. Several new categories of biomass burning were added, and the number of species for which emission data are presented was increased from 93 to 121. Where field data are still insufficient, estimates based on appropriate extrapolation techniques are proposed. For key species, the updated emission factors are compared with previously published values. Based on these emission factors and published global activity estimates, I have derived estimates of pyrogenic emissions for important species released by the various types of biomass burning.
Atmospheric aerosol particles serve as condensation nuclei for the formation of both, cloud droplets and atmospheric ice particles. As a result, they exert a substantial influence on the ...microphysical properties of water and ice clouds, which in turn affect the processes that lead to the formation of rain, snow, hail, and other forms of precipitation. In recent years, considerable progress has been made in understanding the chemical composition of aerosols, their microphysical properties, and the factors that enable them to act as cloud condensation nuclei (CCN) and ice nuclei (IN).
The first part of this review article will focus on the nature and sources of CCN and IN. We discuss the fundamentals of the cloud droplet and ice nucleation processes, and the role that the chemical composition and particle size play in this process. We show that, in many instances, the influence of chemical composition can be represented by a simple parameterization, which leaves particle size as the main variable controlling CCN efficiency.
Aerosol particles are produced either directly by anthropogenic and natural sources (dust, sea salt, soot, biological particles, etc.), or they are formed in the atmosphere by condensation of low-volatility compounds (e.g., sulfuric acid or oxidized organic compounds). We discuss the magnitude of these sources, and the CCN and IN characteristics of the particles they produce. In contrast to previous assessments, which focused on the aerosol mass, we are emphasizing the number of particles being produced, as this is the key variable in cloud microphysics. Large uncertainties still exist for many aerosol sources, e.g., the submicron part of the seaspray aerosol, the particles produced by the biosphere, and the secondary organic aerosol. We conclude with a discussion on what particle concentrations may have been in the pristine atmosphere, before the onset on anthropogenic pollution. Model calculations and observations in remote continental regions consistently suggest that CCN concentrations over the pristine continents were similar to those now prevailing over the remote oceans, suggesting that human activities have modified cloud microphysics more than what is reflected in conventional wisdom. The second part of this review will address the effects of changing CCN and IN abundances on precipitation processes, the water cycle, and climate.
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The Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) Experiment was carried out in the environs of Manaus, Brazil, in the central region of the Amazon basin for 2 years from ...1 January 2014 through 31 December 2015. The experiment focused on the complex interactions among vegetation, atmospheric chemistry, and aerosol production on the one hand and their connections to aerosols, clouds, and precipitation on the other. The objective was to understand and quantify these linked processes, first under natural conditions to obtain a baseline and second when altered by the effects of human activities. To this end, the pollution plume from the Manaus metropolis, superimposed on the background conditions of the central Amazon basin, served as a natural laboratory. The present paper, as the introduction to the special issue of GoAmazon2014/5, presents the context and motivation of the GoAmazon2014/5 Experiment. The nine research sites, including the characteristics and instrumentation of each site, are presented. The sites range from time point zero (T0) upwind of the pollution, to T1 in the midst of the pollution, to T2 just downwind of the pollution, to T3 furthest downwind of the pollution (70 km). In addition to the ground sites, a low-altitude G-159 Gulfstream I (G-1) observed the atmospheric boundary layer and low clouds, and a high-altitude Gulfstream G550 (HALO) operated in the free troposphere. During the 2-year experiment, two Intensive Operating Periods (IOP1 and IOP2) also took place that included additional specialized research instrumentation at the ground sites as well as flights of the two aircraft. GoAmazon2014/5 IOP1 was carried out from 1 February to 31 March 2014 in the wet season. GoAmazon2014/5 IOP2 was conducted from 15 August to 15 October 2014 in the dry season. The G-1 aircraft flew during both IOP1 and IOP2, and the HALO aircraft flew during IOP2. In the context of the Amazon basin, the two IOPs also correspond to the clean and biomass burning seasons, respectively. The Manaus plume is present year-round, and it is transported by prevailing northeasterly and easterly winds in the wet and dry seasons, respectively. This introduction also organizes information relevant to many papers in the special issue. Information is provided on the vehicle fleet, power plants, and industrial activities of Manaus. The mesoscale and synoptic meteorologies relevant to the two IOPs are presented. Regional and long-range transport of emissions during the two IOPs is discussed based on satellite observations across South America and Africa. Fire locations throughout the airshed are detailed. In conjunction with the context and motivation of GoAmazon2014/5 as presented in this introduction, research articles including thematic overview articles are anticipated in this special issue to describe the detailed results and findings of the GoAmazon2014/5 Experiment.
As a part of the AMAZE-08 campaign during the wet season in the rainforest of central Amazonia, an ultraviolet aerodynamic particle sizer (UV-APS) was operated for continuous measurements of ...fluorescent biological aerosol particles (FBAP). In the coarse particle size range (> 1 mu m) the campaign median and quartiles of FBAP number and mass concentration were 7.3 x 10 super(4) m super(-3) (4.0-13.2 x 10 super(4) m super(-3)) and 0.72 mu g m super(-3) (0.42-1.19 mu g m super(-3)), respectively, accounting for 24% (11-41%) of total particle number and 47% (25-65%) of total particle mass. During the five-week campaign in February-March 2008 the concentration of coarse-mode Saharan dust particles was highly variable. In contrast, FBAP concentrations remained fairly constant over the course of weeks and had a consistent daily pattern, peaking several hours before sunrise, suggesting observed FBAP was dominated by nocturnal spore emission. This conclusion was supported by the consistent FBAP number size distribution peaking at 2.3 mu m, also attributed to fungal spores and mixed biological particles by scanning electron microscopy (SEM), light microscopy and biochemical staining. A second primary biological aerosol particle (PBAP) mode between 0.5 and 1.0 mu m was also observed by SEM, but exhibited little fluorescence and no true fungal staining. This mode may have consisted of single bacterial cells, brochosomes, various fragments of biological material, and small Chromalveolata (Chromista) spores. Particles liquid-coated with mixed organic-inorganic material constituted a large fraction of observations, and these coatings contained salts likely from primary biological origin. We provide key support for the suggestion that real-time laser-induce fluorescence (LIF) techniques using 355 nm excitation provide size-resolved concentrations of FBAP as a lower limit for the atmospheric abundance of biological particles in a pristine environment. We also show some limitations of using the instrument for ambient monitoring of weakly fluorescent particles < 2 mu m. Our measurements confirm that primary biological particles, fungal spores in particular, are an important fraction of supermicron aerosol in the Amazon and that may contribute significantly to hydrological cycling, especially when coated by mixed inorganic material.
Abiotic release of nitrous acid (HONO) in equilibrium with soil nitrite (NO 2 - ) was suggested as an important contributor to the missing source of atmospheric HONO and hydroxyl radicals (OH). The ...role of total soil-derived HONO in the biogeochemical and atmospheric nitrogen cycles, however, has remained unknown. In laboratory experiments, we found that for nonacidic soils from arid and arable areas, reactive nitrogen emitted as HONO is comparable with emissions of nitric oxide (NO). We show that ammonia-oxidizing bacteria can directly release HONO in quantities larger than expected from the acid-base and Henry's law equilibria of the aqueous phase in soil. This component of the nitrogen cycle constitutes an additional loss term for fixed nitrogen in soils and a source for reactive nitrogen in the atmosphere.
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The Amazon is one of the few continental regions where atmospheric aerosol particles and their effects on climate are not dominated by anthropogenic sources. During the wet season, the ambient ...conditions approach those of the pristine pre-industrial era. We show that the fine submicrometer particles accounting for most cloud condensation nuclei are predominantly composed of secondary organic material formed by oxidation of gaseous biogenic precursors. Supermicrometer particles, which are relevant as ice nuclei, consist mostly of primary biological material directly released from rainforest biota. The Amazon Basin appears to be a biogeochemical reactor, in which the biosphere and atmospheric photochemistry produce nuclei for clouds and precipitation sustaining the hydrological cycle. The prevailing regime of aerosol-cloud interactions in this natural environment is distinctly different from polluted regions.
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8.
Smoking Rain Clouds over the Amazon Andreae, M. O.; Rosenfeld, D.; Artaxo, P. ...
Science,
02/2004, Volume:
303, Issue:
5662
Journal Article
Peer reviewed
Open access
Heavy smoke from forest fires in the Amazon was observed to reduce cloud droplet size and so delay the onset of precipitation from 1.5 kilometers above cloud base in pristine clouds to more than 5 ...kilometers in polluted clouds and more than 7 kilometers in pyro-clouds. Suppression of low-level rainout and aerosol washout allows transport of water and smoke to upper levels, where the clouds appear "smoking" as they detrain much of the pollution. Elevating the onset of precipitation allows invigoration of the updrafts, causing intense thunderstorms, large hail, and greater likelihood for overshooting cloud tops into the stratosphere. There, detrained pollutants and water vapor would have profound radiative impacts on the climate system. The invigorated storms release the latent heat higher in the atmosphere. This should substantially affect the regional and global circulation systems. Together, these processes affect the water cycle, the pollution burden of the atmosphere, and the dynamics of atmospheric circulation.
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Although the definition and measurement techniques for atmospheric "black carbon" ("BC") or "elemental carbon'' ("EC") have long been subjects of scientific controversy, the recent discovery of ...light-absorbing carbon that is not black ("brown carbon, Cbrown") makes it imperative to reassess and redefine the components that make up light-absorbing carbonaceous matter (LAC) in the atmosphere. Evidence for the atmospheric presence of Cbrown comes from (1) spectral aerosol light absorption measurements near specific combustion sources, (2) observations of spectral properties of water extracts of continental aerosol, (3) laboratory studies indicating the formation of light-absorbing organic matter in the atmosphere, and (4) indirectly from the chemical analogy of aerosol species to colored natural humic substances. We show that brown carbon may severely bias measurements of "BC" and "EC" over vast parts of the troposphere, especially those strongly polluted by biomass burning, where the mass concentration of Cbrown is high relative to that of soot carbon. Chemical measurements to determine "EC" are biased by the refractory nature of Cbrown as well as by complex matrix interferences. Optical measurements of "BC" suffer from a number of problems: (1) many of the presently used instruments introduce a substantial bias into the determination of aerosol light absorption, (2) there is no unique conversion factor between light absorption and "EC" or "BC" concentration in ambient aerosols, and (3) the difference in spectral properties between the different types of LAC, as well as the chemical complexity of Cbrown, lead to several conceptual as well as practical complications. We also suggest that due to the sharply increasing absorption of Cbrown towards the UV, single-wavelength light absorption measurements may not be adequate for the assessment of absorption of solar radiation in the troposphere. We discuss the possible consequences of these effects for our understanding of tropospheric processes, including their influence on UV-irradiance, atmospheric photochemistry and radiative transfer in clouds.
Size-resolved cloud condensation nuclei (CCN) spectra measured for various aerosol types at a non-urban site in Germany showed that CCN concentrations are mainly determined by the aerosol number size ...distribution. Distinct variations of CCN activation with particle chemical composition were observed but played a secondary role. When the temporal variation of chemical effects on CCN activation is neglected, variation in the size distribution alone explains 84 to 96% of the variation in CCN concentrations. Understanding that particles' ability to act as CCN is largely controlled by aerosol size rather than composition greatly facilitates the treatment of aerosol effects on cloud physics in regional and global models.
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