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At least 253 records · Page 14Linked to original sources
PubMed2005

Assessing the influence of climate variability on atmospheric concentrations of polychlorinated biphenyls using a global-scale mass balance model (BETR-global).

We introduce a new global-scale multimedia contaminant fate model (the Berkeley-Trent Global Model; BETR-Global) that integrates global climate data from the National Centers for Environmental Prediction (NCEP). BETR-Global represents the global environment as a connected set of 288 multimedia regions on a 15 degrees grid. We evaluate the model by simulating the global fate and transport of seven PCB congeners over a 70 year period and find satisfactory agreement between model output and observations of atmospheric PCB concentrations at 11 long-term monitoring stations in the Northern Hemisphere. We demonstrate the use of the model as a tool for understanding global pollutant dynamics by examining the hypothesis that variability in global-scale climate conditions, as reflected bythe North Atlantic Oscillation (NAO), influences atmospheric PCB concentrations in the Northern Hemisphere. We estimate that the maximum variability in atmospheric PCB concentrations attributable to NAO variability is approximately a factor of 2. The influence of variability in the NAO on PCB concentrations in air is most likely to be observed in the winter and spring at monitoring sites in Northern Europe and the Arctic. Analysis of long-term monitoring data from 11 sites shows some statistically significant relationships between NAO indices and atmospheric PCB concentrations during the winter and spring. Giving consideration to competing factors that influence atmospheric PCB concentrations, longer time series of monitoring data are required to fully evaluate the modeling results and to improve our understanding of the role of climate variability on the long-term fate of persistent semivolatile pollutants.

Arctic Regions↗
PubMed2006

Flux rates of atmospheric lead pollution within soils of a small catchment in northern Sweden and their implications for future stream water quality.

It is not well-known how the accumulated pool of atmospheric lead pollution in the boreal forest soil will affect the groundwater and surface water chemistry in the future as this lead migrates through the soil profile. This study uses stable lead isotopes (206Pb/207Pb and 208Pb/ 207Pb ratios) to trace the transport of atmospheric lead pollution within the soil of a small catchment and predict future lead level changes in a stream draining the catchment. Low 206Pb/207Pb and 208Pb/207Pb ratios for the lead in the soil water (1.16 +/- 0.02; 2.43 +/- 0.03) and streamwater (1.18 +/- 0.03; 2.42 +/- 0.03) in comparison to that of the mineral soil (>1.4; >2.5) suggest that atmospheric pollution contributes by about 90% (65-100%) to the lead pool found in these matrixes. Calculated transport rates of atmospheric lead along a soil transect indicate that the mean residence time of lead in organic and mineral soil layers is at a centennial to millennial time scale. A maximum release of the present pool of lead pollution in the soil to the stream is predicted to occur within 200-800 years. Even though the uncertainty of the prediction is large, it emphasizes the magnitude of the time lag between the accumulation of atmospheric lead pollution in soils and the subsequent response in streamwater quality.

Atmosphere↗
PubMed2006

Empirical and modeling evidence of the long-range atmospheric transport of decabromodiphenyl ether.

Understanding of the long-range atmospheric transport (LRT) behavior of decabromodiphenyl ether (BDE-209) is still limited. Most existing model-based approaches to assessing an organic chemical's potential for LRT have assumed invariant environmental conditions, even though many factors impacting on the atmospheric residence time are known to vary considerably over a variety of time scales. Model estimates of LRT also suffer from limited evaluation against observational evidence. Such evidence was sought from dated sediment cores taken from lakes along a latitudinal transect in North America. BDE-209 was generally detected only in recent sediment horizons, and sedimentation fluxes were found to decline exponentially with latitude. The empirical half-distance (EHD) for BDE-209 derived from surface flux data is approximately half that of the sigmaPCBs. A dynamic multimedia fate and transport model provides further insight into the temporal variability of processes that control LRT for BDE-209 and PCBs. The variability of precipitation, and in particular, the occurrence of time periods without precipitation coinciding with strong winds, influences the LRT potential of chemicals that combine a sufficiently long atmospheric half-life with very low volatility. Likewise, the forest filter effect may be important for a wider range of chemicals than believed previously, because models assuming constant precipitation fail to account for the impact of differences in dry deposition on days without rain. Chemicals that are both sorbed to particles and potentially persistent in the atmosphere, such as BDE-209, may have a larger potential for LRT than anticipated on the basis of earlier model evaluations. Still, the EHDs illustrate that the model seems to underestimate atmospheric loss processes of potential significance to BDE-209, illustrating the need to critically compare predictions of LRT against observations. Processes that need to be understood better in order to improve predictions of LRT for BDE-209 include particle dry deposition, precipitation scavenging, and photolysis in the sorbed state.

Air Movements↗
PubMed2006

High sensitivity in situ monitoring of NO3 in an atmospheric simulation chamber using incoherent broadband cavity-enhanced absorption spectroscopy.

We describe the application of incoherent broadband cavity-enhanced absorption spectroscopy (IBBCEAS) for the in situ detection of atmospheric trace gases and radicals (NO3, NO2, O3, H2O) in an atmospheric simulation chamber under realistic atmospheric conditions. The length of the optical cavity across the reaction chamber is 4.5 m, which is significantly longer than in previous studies that use high finesse optical cavities to achieve high absorption sensitivity. Using a straightforward spectrometer configuration, we show that detection limits corresponding to typical atmospheric concentrations can be achieved with a measurement time of seconds to a few minutes. In particular, with only moderate reflectivity mirrors, we report a measured sensitivity of 4 pptv to NO3 in a 1 min acquisition time. The high spatial and temporal resolution of the IBBCEAS method and its pptv sensitivity to NO3 makes it useful in laboratory studies of atmospheric processes as well as having obvious potential for field measurements.

Absorption↗
PubMed1999

Water on Mars: isotopic constraints on exchange between the atmosphere and surface.

Using a new measurement of the D/H fractionation efficiency and new estimates of the water loss, we calculate that Mars has the equivalent of a approximately 9 m global water layer in a reservoir that exchanges with the atmosphere. The measured D/H enrichment is about 5 times the terrestrial value, but without exchange, the atmosphere converges on an enrichment of 50 in about 0.5 Ma. Due to the large buffering reservoir and the rapid loss rate (10(-3) pr-micrometers yr-1), the small atmospheric reservoir, averaging 10 pr-micrometers, is unlikely to be in continuous isotopic equilibrium with the full 9 m exchangeable reservoir. Instead, it presumably equilibrates during periods of high obliquity; the atmospheric D/H ratio is expected to be enriched in between such periods. If isotopic exchange with a small (4 mm global layer) reservoir occurs under current conditions, it possible for the atmospheric D/H ratio to be within 10% of its long term equilibrium.

Atmosphere↗
PubMed1985

Oxidant abundances in rainwater and the evolution of atmospheric oxygen.

A one-dimensional photochemical model has been used to estimate the flux of dissolved hydrogen peroxide (H2O2) and of other soluble species in rainwater as a function of atmospheric oxygen level. H2O2 should have replaced O2 as the dominant oxidant in rainwater at oxygen levels below 10(-3)-10(-2) times the present atmospheric level (PAL). The exact value of pO2 at which H2O2 becomes more important than O2 depends on the abundance of trace gases such as CO, CH4, and NO. H2O2 was probably an important oxidant even in an O2-free atmosphere, provided that CO2 levels were significant higher than today's. In model atmospheres containing free O2 the concentration of photochemically produced oxidants generally exceeds that of photochemically produced reductants. The oxidizing power of rainwater is therefore greater than that due to dissolved molecular O2 alone. The difference is small at present but becomes important at O2 levels less than 10(-3) PAL. At O2 levels between 10(-4) and 10(-5) PAL the oxidizing power of rainwater is almost independent of pO2. Precambrian soils in which a part or all of the Fe2+ in their source rocks has been oxidized to Fe3+ could therefore have developed in the presence of an atmosphere with very low values of pO2. On the other hand, the upper limit for pO2 during early and mid-Precambrian time suggested by the incomplete oxidation of FeO in soils developed on basaltic rocks is affected only slightly by the presence of photochemical products in rainwater.

Atmosphere↗
PubMed1989

Hydrogen and deuterium loss from the terrestrial atmosphere: a quantitative assessment of nonthermal escape fluxes.

A comprehensive one-dimensional photochemical model extending from the middle atmosphere (50 km) to the exobase (432 km) has been used to study the escape of hydrogen and deuterium from the Earth's atmosphere. The model incorporates recent advances in chemical kinetics as well as atmospheric observations by satellites, especially the Atmosphere Explorer C satellite. The results suggest: (1) the escape fluxes of both H and D are limited by the upward transport of total hydrogen and total deuterium at the homopause (this result is known as Hunten's limiting flux theorem); (2) about one fourth of total hydrogen escape is thermal, the rest being nonthermal; (3) escape of D is nonthermal; and (4) charge exchange and polar wind are important mechanisms for the nonthermal escape of H and D, but other nonthermal mechanisms may be required. The efficiency to escape from the terrestrial atmosphere for D is 0.74 of the efficiency for H. If the difference between the D/H ratio measured in deep-sea tholeiite glass and that of standard sea water, delta D = -77%, were caused by the escape of H and D, we estimate that as much water as the equivalent of 36% of the present ocean might have been lost in the past.

Atmosphere↗
PubMed2000

Detection and classification of atmospheric methane oxidizing bacteria in soil.

Well-drained non-agricultural soils mediate the oxidation of methane directly from the atmosphere, contributing 5 to 10% towards the global methane sink. Studies of methane oxidation kinetics in soil infer the activity of two methanotrophic populations: one that is only active at high methane concentrations (low affinity) and another that tolerates atmospheric levels of methane (high affinity). The activity of the latter has not been demonstrated by cultured laboratory strains of methanotrophs, leaving the microbiology of methane oxidation at atmospheric concentrations unclear. Here we describe a new pulse-chase experiment using long-term enrichment with 12CH4 followed by short-term exposure to 13CH4 to isotopically label methanotrophs in a soil from a temperate forest. Analysis of labelled phospholipid fatty acids (PLFAs) provided unambiguous evidence of methane assimilation at true atmospheric concentrations (1.8-3.6 p.p.m.v.). High proportions of 13C-labelled C18 fatty acids and the co-occurrence of a labelled, branched C17 fatty acid indicated that a new methanotroph, similar at the PLFA level to known type II methanotrophs, was the predominant soil micro-organism responsible for atmospheric methane oxidation.

Atmosphere↗
PubMed2000

Reduced calcification of marine plankton in response to increased atmospheric CO2.

The formation of calcareous skeletons by marine planktonic organisms and their subsequent sinking to depth generates a continuous rain of calcium carbonate to the deep ocean and underlying sediments. This is important in regulating marine carbon cycling and ocean-atmosphere CO2 exchange. The present rise in atmospheric CO2 levels causes significant changes in surface ocean pH and carbonate chemistry. Such changes have been shown to slow down calcification in corals and coralline macroalgae, but the majority of marine calcification occurs in planktonic organisms. Here we report reduced calcite production at increased CO2 concentrations in monospecific cultures of two dominant marine calcifying phytoplankton species, the coccolithophorids Emiliania huxleyi and Gephyrocapsa oceanica. This was accompanied by an increased proportion of malformed coccoliths and incomplete coccospheres. Diminished calcification led to a reduction in the ratio of calcite precipitation to organic matter production. Similar results were obtained in incubations of natural plankton assemblages from the north Pacific ocean when exposed to experimentally elevated CO2 levels. We suggest that the progressive increase in atmospheric CO2 concentrations may therefore slow down the production of calcium carbonate in the surface ocean. As the process of calcification releases CO2 to the atmosphere, the response observed here could potentially act as a negative feedback on atmospheric CO2 levels.

Atmosphere↗
PubMed2000

Effect of iron supply on Southern Ocean CO2 uptake and implications for glacial atmospheric CO2.

Photosynthesis by marine phytoplankton in the Southern Ocean, and the associated uptake of carbon, is thought to be currently limited by the availability of iron. One implication of this limitation is that a larger iron supply to the region in glacial times could have stimulated algal photosynthesis, leading to lower concentrations of atmospheric CO2. Similarly, it has been proposed that artificial iron fertilization of the oceans might increase future carbon sequestration. Here we report data from a whole-ecosystem test of the iron-limitation hypothesis in the Southern Ocean, which show that surface uptake of atmospheric CO2 and uptake ratios of silica to carbon by phytoplankton were strongly influenced by nanomolar increases of iron concentration. We use these results to inform a model of global carbon and ocean nutrients, forced with atmospheric iron fluxes to the region derived from the Vostok ice-core dust record. During glacial periods, predicted magnitudes and timings of atmospheric CO2 changes match ice-core records well. At glacial terminations, the model suggests that forcing of Southern Ocean biota by iron caused the initial approximately 40 p.p.m. of glacial-interglacial CO2 change, but other mechanisms must have accounted for the remaining 40 p.p.m. increase. The experiment also confirms that modest sequestration of atmospheric CO2 by artificial additions of iron to the Southern Ocean is in principle possible, although the period and geographical extent over which sequestration would be effective remain poorly known.

Atmosphere↗
PubMed1992

Possible cometary origin of heavy noble gases in the atmospheres of Venus, Earth and Mars

Models that trace the origin of noble gases in the atmospheres of the terrestrial planets (Venus, Earth and Mars) to the 'planetary component' in chondritic meteorites confront several problems. The 'missing' xenon in the atmospheres of Mars and Earth is one of the most obvious; this gas is not hidden or trapped in surface materials. On Venus, the absolute abundances of neon and argon per gram of rock are higher even than those in carbonaceous chondrites, whereas the relative abundances of argon and krypton are closer to solar than to chondritic values (there is only an upper limit on xenon). Pepin has developed a model that emphasizes hydrodynamic escape of early, massive hydrogen atmospheres to explain the abundances and isotope ratios of noble gases on all three planets. We have previously suggested that the unusual abundances of heavy noble gases on Venus might be explained by the impact of a low-temperature comet. Further consideration of the probable history of the martian atmosphere, the noble-gas data from the (Mars-derived) SNC meteorites and laboratory experiments on the trapping of noble gases in ice lead us to propose here that the noble gases in the atmospheres of all of the terrestrial planets are dominated by a mixture of an internal component and contribution from impacting icy planetesimals (comets). If true, this hypothesis illustrates the importance of impacts in determining the volatile inventories of these planets.

Argon↗
PubMed1995

Detection of an oxygen atmosphere on Jupiter's moon Europa.

Europa, the second large satellite out from Jupiter, is roughly the size of Earth's Moon, but unlike the Moon, it has water ice on its surface. There have been suggestions that an oxygen atmosphere should accumulate around such a body, through reactions which break up the water molecules and form molecular hydrogen and oxygen. The lighter H2 molecules would escape from Europa relatively easily, leaving behind an atmosphere rich in oxygen. Here we report the detection of atomic oxygen emission from Europa, which we interpret as being produced by the simultaneous dissociation and excitation of atmospheric O2 by electrons from Jupiter's magnetosphere. Europa's molecular oxygen atmosphere is very tenuous, with a surface pressure about 10(-11) that of the Earth's atmosphere at sea level.

Atmosphere↗
PubMed2003

High CO2 levels in the Proterozoic atmosphere estimated from analyses of individual microfossils.

Solar luminosity on the early Earth was significantly lower than today. Therefore, solar luminosity models suggest that, in the atmosphere of the early Earth, the concentration of greenhouse gases such as carbon dioxide and methane must have been much higher. However, empirical estimates of Proterozoic levels of atmospheric carbon dioxide concentrations have not hitherto been available. Here we present ion microprobe analyses of the carbon isotopes in individual organic-walled microfossils extracted from a Proterozoic ( approximately 1.4-gigayear-old) shale in North China. Calculated magnitudes of the carbon isotope fractionation in these large, morphologically complex microfossils suggest elevated levels of carbon dioxide in the ancient atmosphere--between 10 and 200 times the present atmospheric level. Our results indicate that carbon dioxide was an important greenhouse gas during periods of lower solar luminosity, probably dominating over methane after the atmosphere and hydrosphere became pervasively oxygenated between 2 and 2.2 gigayears ago.

Atmosphere↗
PubMed2004

Dating the rise of atmospheric oxygen.

Several lines of geological and geochemical evidence indicate that the level of atmospheric oxygen was extremely low before 2.45 billion years (Gyr) ago, and that it had reached considerable levels by 2.22 Gyr ago. Here we present evidence that the rise of atmospheric oxygen had occurred by 2.32 Gyr ago. We found that syngenetic pyrite is present in organic-rich shales of the 2.32-Gyr-old Rooihoogte and Timeball Hill formations, South Africa. The range of the isotopic composition of sulphur in this pyrite is large and shows no evidence of mass-independent fractionation, indicating that atmospheric oxygen was present at significant levels (that is, greater than 10(-5) times that of the present atmospheric level) during the deposition of these units. The presence of rounded pebbles of sideritic iron formation at the base of the Rooihoogte Formation and an extensive and thick ironstone layer consisting of haematitic pisolites and oölites in the upper Timeball Hill Formation indicate that atmospheric oxygen rose significantly, perhaps for the first time, during the deposition of the Rooihoogte and Timeball Hill formations. These units were deposited between what are probably the second and third of the three Palaeoproterozoic glacial events.

Atmosphere↗
PubMed2006

Sulphur isotope evidence for an oxic Archaean atmosphere.

The presence of mass-independently fractionated sulphur isotopes (MIF-S) in many sedimentary rocks older than approximately 2.4 billion years (Gyr), and the absence of MIF-S in younger rocks, has been considered the best evidence for a dramatic change from an anoxic to oxic atmosphere around 2.4 Gyr ago. This is because the only mechanism known to produce MIF-S has been ultraviolet photolysis of volcanic sulphur dioxide gas in an oxygen-poor atmosphere. Here we report the absence of MIF-S throughout approximately 100-m sections of 2.76-Gyr-old lake sediments and 2.92-Gyr-old marine shales in the Pilbara Craton, Western Australia. We propose three possible interpretations of the MIF-S geologic record: (1) the level of atmospheric oxygen fluctuated greatly during the Archaean era; (2) the atmosphere has remained oxic since approximately 3.8 Gyr ago, and MIF-S in sedimentary rocks represents times and regions of violent volcanic eruptions that ejected large volumes of sulphur dioxide into the stratosphere; or (3) MIF-S in rocks was mostly created by non-photochemical reactions during sediment diagenesis, and thus is not linked to atmospheric chemistry.

Archaea↗
PubMed2005

Uptake and reaction of atmospheric organic vapours on organic films.

Films composed in whole or in part of organic compounds represent an important atmospheric interface. Urban surfaces are now known to be coated with a film ("grime") whose chemical composition somewhat resembles that of urban atmospheric aerosols. Such films may act as media in which atmospheric trace gases may be sequestered (leading to their removal from the gas phase); they may also act as reactive media, either as a "solvent" or as a source of reagents. Organic coatings on aqueous surfaces are also important, not just on ocean and lake surfaces ("biofilms") but also on the surfaces of fogwaters and atmospheric aerosol particles. We have initiated experimental uptake studies of trace gases into simple proxies for urban organic films using two techniques: a Knudsen cell effusion reactor and a laser-induced fluorescence method. We will discuss our first results on non-reactive uptake of organic compounds by organic films we use as proxies for urban grime coatings. In general, the measured uptake coefficients appear to track the octanol-air partition coefficients, at least qualitiatively. We have also measured the kinetics of reactions between gas-phase ozone and small polycyclic aromatic hydrocarbons (PAHs), when these are adsorbed at the air-aqueous interface or incorporated into an organic film. Reactions at the "clean" air-water interface and at a coated interface consisting of a monolayer of various amphiphilic organic compounds all follow a Langmuir-Hinshelwood mechanism, in which ozone first adsorbs to the air-aqueous interface, then reacts with already adsorbed PAH. By contrast, the reaction in the pure organic film occurs in the bulk phase. Under some circumstances, heterogeneous oxidation of PAHs by ozone may be as important in the atmosphere as their gas phase oxidation by OH.

Adsorption↗
PubMed2005

Small scale structure in the atmosphere: implications for chemical composition and observational methods.

Non-linearities in chemical processes are recognised as being important in a number of areas of atmospheric science. In this paper we show simulations using an idealised plume model which describes the relaxation of an urban plume into the background atmosphere. As might be anticipated, the initial conditions of NOx, O3 and VOCs within the plume and background are important in determining the chemistry downstream of the source, but crucially for this study, the rate of mixing (on timescales appropriate to the real atmosphere) is found to alter the composition of the atmosphere significantly. The model shows that NO3 chemistry can play a major role in the oxidation of biogenic VOCs present in the background atmosphere. In addition, the reaction of hydrocarbons with NO3 potentially has important implications for NOy speciation because a significant fraction of organic nitrates thus formed are sufficiently long-lived to leave the planetary boundary layer. A particularly critical result of the model is that under certain NOx conditions, O3 surface deposition can be significantly inhibited, with consequent effects on the O3 budget.

Aerosols↗
PubMed2006

The atmospheric photolysis of E-2-hexenal, Z-3-hexenal and E,E-2,4-hexadienal.

The atmospheric photolysis of E-2-hexenal, Z-3-hexenal and E,E-2,4-hexadienal has been investigated at the large outdoor European Photoreactor (EUPHORE) in Valencia, Spain. E-2-Hexenal and E,E-2,4-hexadienal were found to undergo rapid isomerization to produce Z-2-hexenal and a ketene-type compound (probably E-hexa-1,3-dien-1-one), respectively. Both isomerization processes were reversible with formation of the reactant slightly favoured. Values of j(E-2-hexenal)/j(NO(2)) = (1.80 +/- 0.18) x 10(-2) and j(E,E-2,4-hexadienal)/j(NO(2)) = (2.60 +/- 0.26) x 10(-2) were determined. The gas phase UV absorption cross-sections of E-2-hexenal and E,E-2,4-hexadienal were measured and used to derive effective quantum yields for photoisomerization of 0.36 +/- 0.04 for E-2-hexenal and 0.23 +/- 0.03 for E,E-2,4-hexadienal. Although photolysis appears to be an important atmospheric degradation pathway for E-2-hexenal and E,E-2,4-hexadienal, the reversible nature of the photolytic process means that gas phase reactions with OH and NO(3) radicals are ultimately responsible for the atmospheric removal of these compounds. Atmospheric photolysis of Z-3-hexenal produced CO, with a molar yield of 0.34 +/- 0.03, and 2-pentenal via a Norrish type I process. A value of j(Z-3-hexenal)/j(NO(2)) = (0.4 +/- 0.04) x 10(-2) was determined. The results suggest that photolysis is likely to be a minor atmospheric removal process for Z-3-hexenal.

Aldehydes↗