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1.
Proc Natl Acad Sci U S A ; 113(51): 14639-14644, 2016 12 20.
Artigo em Inglês | MEDLINE | ID: mdl-27930294

RESUMO

Acidification of airborne dust particles can dramatically increase the amount of bioavailable phosphorus (P) deposited on the surface ocean. Experiments were conducted to simulate atmospheric processes and determine the dissolution behavior of P compounds in dust and dust precursor soils. Acid dissolution occurs rapidly (seconds to minutes) and is controlled by the amount of H+ ions present. For H+ < 10-4 mol/g of dust, 1-10% of the total P is dissolved, largely as a result of dissolution of surface-bound forms. At H+ > 10-4 mol/g of dust, the amount of P (and calcium) released has a direct proportionality to the amount of H+ consumed until all inorganic P minerals are exhausted and the final pH remains acidic. Once dissolved, P will stay in solution due to slow precipitation kinetics. Dissolution of apatite-P (Ap-P), the major mineral phase in dust (79-96%), occurs whether calcium carbonate (calcite) is present or not, although the increase in dissolved P is greater if calcite is absent or if the particles are externally mixed. The system was modeled adequately as a simple mixture of Ap-P and calcite. P dissolves readily by acid processes in the atmosphere in contrast to iron, which dissolves more slowly and is subject to reprecipitation at cloud water pH. We show that acidification can increase bioavailable P deposition over large areas of the globe, and may explain much of the previously observed patterns of variability in leachable P in oceanic areas where primary productivity is limited by this nutrient (e.g., Mediterranean).


Assuntos
Atmosfera/química , Poeira/análise , Oceanos e Mares , Fósforo/análise , Água do Mar/química , Cálcio/análise , Carbonato de Cálcio/análise , Ciclo do Carbono , Geografia , Concentração de Íons de Hidrogênio , Ferro/química , Minerais , Nitrogênio , Óxidos/química , Fosfatos/análise , Solubilidade , Propriedades de Superfície
2.
Proc Natl Acad Sci U S A ; 113(21): 5781-90, 2016 May 24.
Artigo em Inglês | MEDLINE | ID: mdl-27222566

RESUMO

The effect of an increase in atmospheric aerosol concentrations on the distribution and radiative properties of Earth's clouds is the most uncertain component of the overall global radiative forcing from preindustrial time. General circulation models (GCMs) are the tool for predicting future climate, but the treatment of aerosols, clouds, and aerosol-cloud radiative effects carries large uncertainties that directly affect GCM predictions, such as climate sensitivity. Predictions are hampered by the large range of scales of interaction between various components that need to be captured. Observation systems (remote sensing, in situ) are increasingly being used to constrain predictions, but significant challenges exist, to some extent because of the large range of scales and the fact that the various measuring systems tend to address different scales. Fine-scale models represent clouds, aerosols, and aerosol-cloud interactions with high fidelity but do not include interactions with the larger scale and are therefore limited from a climatic point of view. We suggest strategies for improving estimates of aerosol-cloud relationships in climate models, for new remote sensing and in situ measurements, and for quantifying and reducing model uncertainty.

3.
Proc Natl Acad Sci U S A ; 113(21): 5820-7, 2016 May 24.
Artigo em Inglês | MEDLINE | ID: mdl-26848136

RESUMO

The largest uncertainty in the historical radiative forcing of climate is caused by the interaction of aerosols with clouds. Historical forcing is not a directly measurable quantity, so reliable assessments depend on the development of global models of aerosols and clouds that are well constrained by observations. However, there has been no systematic assessment of how reduction in the uncertainty of global aerosol models will feed through to the uncertainty in the predicted forcing. We use a global model perturbed parameter ensemble to show that tight observational constraint of aerosol concentrations in the model has a relatively small effect on the aerosol-related uncertainty in the calculated forcing between preindustrial and present-day periods. One factor is the low sensitivity of present-day aerosol to natural emissions that determine the preindustrial aerosol state. However, the major cause of the weak constraint is that the full uncertainty space of the model generates a large number of model variants that are equally acceptable compared to present-day aerosol observations. The narrow range of aerosol concentrations in the observationally constrained model gives the impression of low aerosol model uncertainty. However, these multiple "equifinal" models predict a wide range of forcings. To make progress, we need to develop a much deeper understanding of model uncertainty and ways to use observations to constrain it. Equifinality in the aerosol model means that tuning of a small number of model processes to achieve model-observation agreement could give a misleading impression of model robustness.

4.
Proc Natl Acad Sci U S A ; 113(21): 5812-9, 2016 May 24.
Artigo em Inglês | MEDLINE | ID: mdl-26831092

RESUMO

The topic of cloud radiative forcing associated with the atmospheric aerosol has been the focus of intense scrutiny for decades. The enormity of the problem is reflected in the need to understand aspects such as aerosol composition, optical properties, cloud condensation, and ice nucleation potential, along with the global distribution of these properties, controlled by emissions, transport, transformation, and sinks. Equally daunting is that clouds themselves are complex, turbulent, microphysical entities and, by their very nature, ephemeral and hard to predict. Atmospheric general circulation models represent aerosol-cloud interactions at ever-increasing levels of detail, but these models lack the resolution to represent clouds and aerosol-cloud interactions adequately. There is a dearth of observational constraints on aerosol-cloud interactions. We develop a conceptual approach to systematically constrain the aerosol-cloud radiative effect in shallow clouds through a combination of routine process modeling and satellite and surface-based shortwave radiation measurements. We heed the call to merge Darwinian and Newtonian strategies by balancing microphysical detail with scaling and emergent properties of the aerosol-cloud radiation system.

5.
Nature ; 525(7568): 234-8, 2015 Sep 10.
Artigo em Inglês | MEDLINE | ID: mdl-26354482

RESUMO

The amount of ice present in clouds can affect cloud lifetime, precipitation and radiative properties. The formation of ice in clouds is facilitated by the presence of airborne ice-nucleating particles. Sea spray is one of the major global sources of atmospheric particles, but it is unclear to what extent these particles are capable of nucleating ice. Sea-spray aerosol contains large amounts of organic material that is ejected into the atmosphere during bubble bursting at the organically enriched sea-air interface or sea surface microlayer. Here we show that organic material in the sea surface microlayer nucleates ice under conditions relevant for mixed-phase cloud and high-altitude ice cloud formation. The ice-nucleating material is probably biogenic and less than approximately 0.2 micrometres in size. We find that exudates separated from cells of the marine diatom Thalassiosira pseudonana nucleate ice, and propose that organic material associated with phytoplankton cell exudates is a likely candidate for the observed ice-nucleating ability of the microlayer samples. Global model simulations of marine organic aerosol, in combination with our measurements, suggest that marine organic material may be an important source of ice-nucleating particles in remote marine environments such as the Southern Ocean, North Pacific Ocean and North Atlantic Ocean.


Assuntos
Atmosfera/química , Gelo , Aerossóis/síntese química , Aerossóis/química , Ar , Organismos Aquáticos/química , Regiões Árticas , Diatomáceas/química , Congelamento , Compostos Orgânicos/análise , Compostos Orgânicos/química , Fitoplâncton/química , Água do Mar/química
6.
Proc Natl Acad Sci U S A ; 111(52): 18466-71, 2014 Dec 30.
Artigo em Inglês | MEDLINE | ID: mdl-25512511

RESUMO

Natural aerosols define a preindustrial baseline state from which the magnitude of anthropogenic aerosol effects on climate are calculated and are a major component of the large uncertainty in anthropogenic aerosol-cloud radiative forcing. This uncertainty would be reduced if aerosol environments unperturbed by air pollution could be studied in the present--day atmosphere, but the pervasiveness of air pollution makes identification of unperturbed regions difficult. Here, we use global model simulations to define unperturbed aerosol regions in terms of two measures that compare 1750 and 2000 conditions-the number of days with similar aerosol concentrations and the similarity of the aerosol response to perturbations in model processes and emissions. The analysis shows that the aerosol system in many present-day environments looks and behaves like it did in the preindustrial era. On a global annual mean, unperturbed aerosol regions cover 12% of the Earth (16% of the ocean surface and 2% of the land surface). There is a strong seasonal variation in unperturbed regions of between 4% in August and 27% in January, with the most persistent conditions occurring over the equatorial Pacific. About 90% of unperturbed regions occur in the Southern Hemisphere, but in the Northern Hemisphere, unperturbed conditions are transient and spatially patchy. In cloudy regions with a radiative forcing relative to 1750, model results suggest that unperturbed aerosol conditions could still occur on a small number of days per month. However, these environments are mostly in the Southern Hemisphere, potentially limiting the usefulness in reducing Northern Hemisphere forcing uncertainty.

7.
Proc Natl Acad Sci U S A ; 111(42): 15019-24, 2014 Oct 21.
Artigo em Inglês | MEDLINE | ID: mdl-25288761

RESUMO

For atmospheric sulfuric acid (SA) concentrations the presence of dimethylamine (DMA) at mixing ratios of several parts per trillion by volume can explain observed boundary layer new particle formation rates. However, the concentration and molecular composition of the neutral (uncharged) clusters have not been reported so far due to the lack of suitable instrumentation. Here we report on experiments from the Cosmics Leaving Outdoor Droplets chamber at the European Organization for Nuclear Research revealing the formation of neutral particles containing up to 14 SA and 16 DMA molecules, corresponding to a mobility diameter of about 2 nm, under atmospherically relevant conditions. These measurements bridge the gap between the molecular and particle perspectives of nucleation, revealing the fundamental processes involved in particle formation and growth. The neutral clusters are found to form at or close to the kinetic limit where particle formation is limited only by the collision rate of SA molecules. Even though the neutral particles are stable against evaporation from the SA dimer onward, the formation rates of particles at 1.7-nm size, which contain about 10 SA molecules, are up to 4 orders of magnitude smaller compared with those of the dimer due to coagulation and wall loss of particles before they reach 1.7 nm in diameter. This demonstrates that neither the atmospheric particle formation rate nor its dependence on SA can simply be interpreted in terms of cluster evaporation or the molecular composition of a critical nucleus.

8.
Science ; 344(6185): 717-21, 2014 May 16.
Artigo em Inglês | MEDLINE | ID: mdl-24833386

RESUMO

Atmospheric new-particle formation affects climate and is one of the least understood atmospheric aerosol processes. The complexity and variability of the atmosphere has hindered elucidation of the fundamental mechanism of new-particle formation from gaseous precursors. We show, in experiments performed with the CLOUD (Cosmics Leaving Outdoor Droplets) chamber at CERN, that sulfuric acid and oxidized organic vapors at atmospheric concentrations reproduce particle nucleation rates observed in the lower atmosphere. The experiments reveal a nucleation mechanism involving the formation of clusters containing sulfuric acid and oxidized organic molecules from the very first step. Inclusion of this mechanism in a global aerosol model yields a photochemically and biologically driven seasonal cycle of particle concentrations in the continental boundary layer, in good agreement with observations.


Assuntos
Aerossóis/química , Atmosfera/química , Mudança Climática , Compostos Orgânicos/química , Ácidos Sulfúricos/química , Simulação por Computador , Modelos Químicos , Oxirredução , Processos Fotoquímicos , Estações do Ano , Volatilização
9.
Proc Natl Acad Sci U S A ; 110(43): 17223-8, 2013 Oct 22.
Artigo em Inglês | MEDLINE | ID: mdl-24101502

RESUMO

Atmospheric aerosols formed by nucleation of vapors affect radiative forcing and therefore climate. However, the underlying mechanisms of nucleation remain unclear, particularly the involvement of organic compounds. Here, we present high-resolution mass spectra of ion clusters observed during new particle formation experiments performed at the Cosmics Leaving Outdoor Droplets chamber at the European Organization for Nuclear Research. The experiments involved sulfuric acid vapor and different stabilizing species, including ammonia and dimethylamine, as well as oxidation products of pinanediol, a surrogate for organic vapors formed from monoterpenes. A striking resemblance is revealed between the mass spectra from the chamber experiments with oxidized organics and ambient data obtained during new particle formation events at the Hyytiälä boreal forest research station. We observe that large oxidized organic compounds, arising from the oxidation of monoterpenes, cluster directly with single sulfuric acid molecules and then form growing clusters of one to three sulfuric acid molecules plus one to four oxidized organics. Most of these organic compounds retain 10 carbon atoms, and some of them are remarkably highly oxidized (oxygen-to-carbon ratios up to 1.2). The average degree of oxygenation of the organic compounds decreases while the clusters are growing. Our measurements therefore connect oxidized organics directly, and in detail, with the very first steps of new particle formation and their growth between 1 and 2 nm in a controlled environment. Thus, they confirm that oxidized organics are involved in both the formation and growth of particles under ambient conditions.


Assuntos
Atmosfera/química , Monoterpenos/química , Compostos Orgânicos/química , Ácidos Sulfúricos/química , Aerossóis/análise , Aerossóis/química , Amônia/análise , Amônia/química , Atmosfera/análise , Dimetilaminas/análise , Dimetilaminas/química , Monitoramento Ambiental/instrumentação , Monitoramento Ambiental/métodos , Espectrometria de Massas , Compostos Orgânicos/análise , Oxirredução , Tamanho da Partícula , Reprodutibilidade dos Testes , Volatilização
10.
Nature ; 498(7454): 355-8, 2013 Jun 20.
Artigo em Inglês | MEDLINE | ID: mdl-23760484

RESUMO

The amount of ice present in mixed-phase clouds, which contain both supercooled liquid water droplets and ice particles, affects cloud extent, lifetime, particle size and radiative properties. The freezing of cloud droplets can be catalysed by the presence of aerosol particles known as ice nuclei. One of the most important ice nuclei is thought to be mineral dust aerosol from arid regions. It is generally assumed that clay minerals, which contribute approximately two-thirds of the dust mass, dominate ice nucleation by mineral dust, and many experimental studies have therefore focused on these materials. Here we use an established droplet-freezing technique to show that feldspar minerals dominate ice nucleation by mineral dusts under mixed-phase cloud conditions, despite feldspar being a minor component of dust emitted from arid regions. We also find that clay minerals are relatively unimportant ice nuclei. Our results from a global aerosol model study suggest that feldspar ice nuclei are globally distributed and that feldspar particles may account for a large proportion of the ice nuclei in Earth's atmosphere that contribute to freezing at temperatures below about -15 °C.

11.
Faraday Discuss ; 165: 495-512, 2013.
Artigo em Inglês | MEDLINE | ID: mdl-24601019

RESUMO

Aerosol radiative forcing over the industrial period has remained the largest forcing uncertainty through all IPCC assessments since 1996. Despite the importance of this uncertainty for our understanding of past and future climate change, very little attention is given to the problem of uncertainty reduction in its own right, mainly because most uncertainty analysis approaches are not appropriate to computationally expensive global models. Here we show how a comprehensive understanding of global aerosol model parametric uncertainty can be obtained by using emulators. The approach enables a Monte Carlo sampling of the model uncertainty space based on a manageable number of simulations. This allows full probability density functions of model outputs to be generated from which the uncertainty and its causes can be diagnosed using variance decomposition. We apply this approach to global concentrations of particles larger than 3 and 50 nm diameter (N3 and N50) to produce a ranked list of twenty-eight processes and emissions that control the uncertainty. The results show that the uncertainty in N50 is much more strongly affected by emissions and processes that control the availability of gas phase H2SO4 than by uncertainties in the nucleation rate itself, which cause generally less than 10% uncertainty in N50 in July. Secondary organic aerosol production is assumed to be very uncertain (5-360 Tg a(-1) for biogenic emissions) but the effect on global N3 uncertainty is < 3% except in a few hotspots, and generally < 2% for N50. A complete understanding of the model uncertainty combined with global observations can be used to determine plausible and implausible parts of parameter space as well as to identify model structural weaknesses. In this direction, a preliminary comparison of the model ensemble with observations at Hyytiala, Finland, suggests that an organic-mediated boundary layer nucleation mechanism would help to optimise the behaviour of the model.

12.
Proc Natl Acad Sci U S A ; 108(38): 15710-5, 2011 Sep 20.
Artigo em Inglês | MEDLINE | ID: mdl-21930954

RESUMO

Historical records show that the A.D. 1783-1784 Laki eruption in Iceland caused severe environmental stress and posed a health hazard far beyond the borders of Iceland. Given the reasonable likelihood of such an event recurring, it is important to assess the scale on which a future eruption could impact society. We quantify the potential health effects caused by an increase in air pollution during a future Laki-style eruption using a global aerosol model together with concentration-response functions derived from current epidemiological studies. The concentration of particulate matter with diameters smaller than 2.5 µm is predicted to double across central, western, and northern Europe during the first 3 mo of the eruption. Over land areas of Europe, the current World Health Organization 24-h air quality guideline for particulate matter with diameters smaller than 2.5 µm is exceeded an additional 36 d on average over the course of the eruption. Based on the changes in particulate air pollution, we estimate that approximately 142,000 additional cardiopulmonary fatalities (with a 95% confidence interval of 52,000-228,000) could occur in Europe. In terms of air pollution, such a volcanic eruption would therefore be a severe health hazard, increasing excess mortality in Europe on a scale that likely exceeds excess mortality due to seasonal influenza.


Assuntos
Poluição do Ar/efeitos adversos , Previsões , Mortalidade/tendências , Erupções Vulcânicas/efeitos adversos , Poluentes Atmosféricos/análise , Algoritmos , Saúde Ambiental/métodos , Saúde Ambiental/normas , Monitoramento Ambiental/métodos , Monitoramento Ambiental/normas , Monitoramento Epidemiológico , Europa (Continente)/epidemiologia , Geografia , História do Século XVIII , Humanos , Islândia/epidemiologia , Tamanho da Partícula , Material Particulado/análise , Medição de Risco/métodos , Medição de Risco/normas , Fatores de Risco , Erupções Vulcânicas/história
13.
Proc Natl Acad Sci U S A ; 107(15): 6646-51, 2010 Apr 13.
Artigo em Inglês | MEDLINE | ID: mdl-20133603

RESUMO

New particle formation in the atmosphere is an important parameter in governing the radiative forcing of atmospheric aerosols. However, detailed nucleation mechanisms remain ambiguous, as laboratory data have so far not been successful in explaining atmospheric nucleation. We investigated the formation of new particles in a smog chamber simulating the photochemical formation of H(2)SO(4) and organic condensable species. Nucleation occurs at H(2)SO(4) concentrations similar to those found in the ambient atmosphere during nucleation events. The measured particle formation rates are proportional to the product of the concentrations of H(2)SO(4) and an organic molecule. This suggests that only one H(2)SO(4) molecule and one organic molecule are involved in the rate-limiting step of the observed nucleation process. Parameterizing this process in a global aerosol model results in substantially better agreement with ambient observations compared to control runs.


Assuntos
Aerossóis , Compostos Orgânicos/química , Aerossóis/química , Poluentes Atmosféricos/química , Atmosfera/química , Química Orgânica/métodos , Clima , Monitoramento Ambiental/métodos , Modelos Químicos , Tamanho da Partícula , Processos Fotoquímicos , Estações do Ano , Smog , Ácidos Sulfúricos/química
14.
Philos Trans A Math Phys Eng Sci ; 366(1885): 4613-26, 2008 Dec 28.
Artigo em Inglês | MEDLINE | ID: mdl-18826917

RESUMO

Previous studies have concluded that boreal forests warm the climate because the cooling from storage of carbon in vegetation and soils is cancelled out by the warming due to the absorption of the Sun's heat by the dark forest canopy. However, these studies ignored the impacts of forests on atmospheric aerosol. We use a global atmospheric model to show that, through emission of organic vapours and the resulting condensational growth of newly formed particles, boreal forests double regional cloud condensation nuclei concentrations (from approx. 100 to approx. 200 cm(-3)). Using a simple radiative model, we estimate that the resulting change in cloud albedo causes a radiative forcing of between -1.8 and -6.7 W m(-2) of forest. This forcing may be sufficiently large to result in boreal forests having an overall cooling impact on climate. We propose that the combination of climate forcings related to boreal forests may result in an important global homeostasis. In cold climatic conditions, the snow-vegetation albedo effect dominates and boreal forests warm the climate, whereas in warmer climates they may emit sufficiently large amounts of organic vapour modifying cloud albedo and acting to cool climate.


Assuntos
Taiga , Árvores , Aerossóis , Carbono , Clima , Mudança Climática
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