95 resultados para Gases, Asphyxiating and poisonous.


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In this study, we investigated the impact of global warming on the variabilities of large-scale interannual and interdecadal climate modes and teleconnection patterns with two long-term integrations of the coupled general circulation model of ECHAM4/OPYC3 at the Max-Planck-Institute for Meteorology, Hamburg. One is the control (CTRL) run with fixed present-day concentrations of greenhouse gases. The other experiment is a simulation of transient greenhouse warming, named GHG run. In the GHG run the averaged geopotential height at 500 hPa is increased significantly, and a negative phase of the Pacific/North American (PNA) teleconnection-like distribution pattern is intensified. The standard deviation over the tropics (high latitudes) is enhanced (reduced) on the interdecadal time scales and reduced (enhanced) on the interannual time scales in the GHG run. Except for an interdecadal mode related to the Southern Oscillation (SO) in the GHG run, the spatial variation patterns are similar for different (interannual + interdecadal, interannual, and interdecadal) time scales in the GHG and CTRL runs. Spatial distributions of the teleconnection patterns on the interannual and interdecadal time scales in the GHG run are also similar to those in the CTRL run. But some teleconnection patterns show linear trends and changes of variances and frequencies in the GHG run. Apart from the positive linear trend of the SO, the interdecadal modulation to the El Niño/SO cycle is enhanced during the GHG 2040 ∼ 2099. This is the result of an enhancement of the Walker circulation during that period. La Niña events intensify and El Niño events relatively weaken during the GHG 2070 ∼ 2090. It is interesting to note that with increasing greenhouse gas concentrations the relation between the SO and the PNA pattern is reversed significantly from a negative to a positive correlation on the interdecadal time scales and weakened on the interannual time scales. This suggests that the increase of the greenhouse gas concentrations will trigger the nonstationary correlation between the SO and the PNA pattern both on the interdecadal and interannual time scales.

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An analysis of the attribution of past and future changes in stratospheric ozone and temperature to anthropogenic forcings is presented. The analysis is an extension of the study of Shepherd and Jonsson (2008) who analyzed chemistry-climate simulations from the Canadian Middle Atmosphere Model (CMAM) and attributed both past and future changes to changes in the external forcings, i.e. the abundances of ozone-depleting substances (ODS) and well-mixed greenhouse gases. The current study is based on a new CMAM dataset and includes two important changes. First, we account for the nonlinear radiative response to changes in CO2. It is shown that over centennial time scales the radiative response in the upper stratosphere to CO2 changes is significantly nonlinear and that failure to account for this effect leads to a significant error in the attribution. To our knowledge this nonlinearity has not been considered before in attribution analysis, including multiple linear regression studies. For the regression analysis presented here the nonlinearity was taken into account by using CO2 heating rate, rather than CO2 abundance, as the explanatory variable. This approach yields considerable corrections to the results of the previous study and can be recommended to other researchers. Second, an error in the way the CO2 forcing changes are implemented in the CMAM was corrected, which significantly affects the results for the recent past. As the radiation scheme, based on Fomichev et al. (1998), is used in several other models we provide some description of the problem and how it was fixed.

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Dynamics affects the distribution and abundance of stratospheric ozone directly through transport of ozone itself and indirectly through its effect on ozone chemistry via temperature and transport of other chemical species. Dynamical processes must be considered in order to understand past ozone changes, especially in the northern hemisphere where there appears to be significant low-frequency variability which can look “trend-like” on decadal time scales. A major challenge is to quantify the predictable, or deterministic, component of past ozone changes. Over the coming century, changes in climate will affect the expected recovery of ozone. For policy reasons it is important to be able to distinguish and separately attribute the effects of ozone-depleting substances and greenhouse gases on both ozone and climate. While the radiative-chemical effects can be relatively easily identified, this is not so evident for dynamics — yet dynamical changes (e.g., changes in the Brewer-Dobson circulation) could have a first-order effect on ozone over particular regions. Understanding the predictability and robustness of such dynamical changes represents another major challenge. Chemistry-climate models have recently emerged as useful tools for addressing these questions, as they provide a self-consistent representation of dynamical aspects of climate and their coupling to ozone chemistry. We can expect such models to play an increasingly central role in the study of ozone and climate in the future, analogous to the central role of global climate models in the study of tropospheric climate change.

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Time-resolved kinetic studies of silylene, SiH2, generated by laser flash photolysis of 1-silacyclopent-3-ene and phenylsilane, have been carried out to obtain rate constants for its bimolecular reactions with methanol, ethanol, 1-propanol, 1-butanol and 2-methyl-1-butanol. The reactions were studied in the gas phase over the pressure range 1-100 Torr in SF6 bath gas, at room temperature. In the study with methanol several buffer gases were used. All five reactions showed pressure dependences characteristic of third body assisted association reactions. The rate constant pressure dependences were modelled using RRKM theory, based on Eo values of the association complexes obtained by ab initio calculation (G3 level). Transition state models were adjusted to fit experimental fall-off curves and extrapolated to obtain k∞ values in the range 1.9 to 4.5 × 10-10 cm3 molecule-1 s-1. These numbers, corresponding to the true bimolecular rate constants, indicate efficiencies of between 16 and 67% of the collision rates for these reactions. In the reaction of SiH2 + MeOH there is a small kinetic component to the rate which is second order in MeOH (at low total pressures). This suggests an additional catalysed reaction pathway, which is supported by the ab initio calculations. These calculations have been used to define specific MeOH-for-H2O substitution effects on this catalytic pathway. Where possible our experimental and theoretical results are compared with those of previous studies.

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During long-range transport, many distinct processes – including photochemistry, deposition, emissions and mixing – contribute to the transformation of air mass composition. Partitioning the effects of different processes can be useful when considering the sensitivity of chemical transformation to, for example, a changing environment or anthropogenic influence. However, transformation is not observed directly, since mixing ratios are measured, and models must be used to relate changes to processes. Here, four cases from the ITCT-Lagrangian 2004 experiment are studied. In each case, aircraft intercepted a distinct air mass several times during transport over the North Atlantic, providing a unique dataset and quantifying the net changes in composition from all processes. A new framework is presented to deconstruct the change in O3 mixing ratio (Δ O3) into its component processes, which were not measured directly, taking into account the uncertainty in measurements, initial air mass variability and its time evolution. The results show that the net chemical processing (Δ O3chem) over the whole simulation is greater than net physical processing (Δ O3phys) in all cases. This is in part explained by cancellation effects associated with mixing. In contrast, each case is in a regime of either net photochemical destruction (lower tropospheric transport) or production (an upper tropospheric biomass burning case). However, physical processes influence O3 indirectly through addition or removal of precursor gases, so that changes to physical parameters in a model can have a larger effect on Δ O3chem than Δ O3phys. Despite its smaller magnitude, the physical processing distinguishes the lower tropospheric export cases, since the net photochemical O3 change is −5 ppbv per day in all three cases. Processing is quantified using a Lagrangian photochemical model with a novel method for simulating mixing through an ensemble of trajectories and a background profile that evolves with them. The model is able to simulate the magnitude and variability of the observations (of O3, CO, NOy and some hydrocarbons) and is consistent with the time-average OH following air-masses inferred from hydrocarbon measurements alone (by Arnold et al., 2007). Therefore, it is a useful new method to simulate air mass evolution and variability, and its sensitivity to process parameters.

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Both historical and idealized climate model experiments are performed with a variety of Earth system models of intermediate complexity (EMICs) as part of a community contribution to the Intergovernmental Panel on Climate Change Fifth Assessment Report. Historical simulations start at 850 CE and continue through to 2005. The standard simulations include changes in forcing from solar luminosity, Earth's orbital configuration, CO2, additional greenhouse gases, land use, and sulphate and volcanic aerosols. In spite of very different modelled pre-industrial global surface air temperatures, overall 20th century trends in surface air temperature and carbon uptake are reasonably well simulated when compared to observed trends. Land carbon fluxes show much more variation between models than ocean carbon fluxes, and recent land fluxes appear to be slightly underestimated. It is possible that recent modelled climate trends or climate–carbon feedbacks are overestimated resulting in too much land carbon loss or that carbon uptake due to CO2 and/or nitrogen fertilization is underestimated. Several one thousand year long, idealized, 2 × and 4 × CO2 experiments are used to quantify standard model characteristics, including transient and equilibrium climate sensitivities, and climate–carbon feedbacks. The values from EMICs generally fall within the range given by general circulation models. Seven additional historical simulations, each including a single specified forcing, are used to assess the contributions of different climate forcings to the overall climate and carbon cycle response. The response of surface air temperature is the linear sum of the individual forcings, while the carbon cycle response shows a non-linear interaction between land-use change and CO2 forcings for some models. Finally, the preindustrial portions of the last millennium simulations are used to assess historical model carbon-climate feedbacks. Given the specified forcing, there is a tendency for the EMICs to underestimate the drop in surface air temperature and CO2 between the Medieval Climate Anomaly and the Little Ice Age estimated from palaeoclimate reconstructions. This in turn could be a result of unforced variability within the climate system, uncertainty in the reconstructions of temperature and CO2, errors in the reconstructions of forcing used to drive the models, or the incomplete representation of certain processes within the models. Given the forcing datasets used in this study, the models calculate significant land-use emissions over the pre-industrial period. This implies that land-use emissions might need to be taken into account, when making estimates of climate–carbon feedbacks from palaeoclimate reconstructions.

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A method of classifying the upper tropospheric/lower stratospheric (UTLS) jets has been developed that allows satellite and aircraft trace gas data and meteorological fields to be efficiently mapped in a jet coordinate view. A detailed characterization of multiple tropopauses accompanies the jet characterization. Jet climatologies show the well-known high altitude subtropical and lower altitude polar jets in the upper troposphere, as well as a pattern of concentric polar and subtropical jets in the Southern Hemisphere, and shifts of the primary jet to high latitudes associated with blocking ridges in Northern Hemisphere winter. The jet-coordinate view segregates air masses differently than the commonly-used equivalent latitude (EqL) coordinate throughout the lowermost stratosphere and in the upper troposphere. Mapping O3 data from the Aura Microwave Limb Sounder (MLS) satellite and the Winter Storms aircraft datasets in jet coordinates thus emphasizes different aspects of the circulation compared to an EqL-coordinate framework: the jet coordinate reorders the data geometrically, thus highlighting the strong PV, tropopause height and trace gas gradients across the subtropical jet, whereas EqL is a dynamical coordinate that may blur these spatial relationships but provides information on irreversible transport. The jet coordinate view identifies the concentration of stratospheric ozone well below the tropopause in the region poleward of and below the jet core, as well as other transport features associated with the upper tropospheric jets. Using the jet information in EqL coordinates allows us to study trace gas distributions in regions of weak versus strong jets, and demonstrates weaker transport barriers in regions with less jet influence. MLS and Atmospheric Chemistry Experiment-Fourier Transform Spectrometer trace gas fields for spring 2008 in jet coordinates show very strong, closely correlated, PV, tropopause height and trace gas gradients across the jet, and evidence of intrusions of stratospheric air below the tropopause below and poleward of the subtropical jet; these features are consistent between instruments and among multiple trace gases. Our characterization of the jets is facilitating studies that will improve our understanding of upper tropospheric trace gas evolution.

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An unusually strong and prolonged stratospheric sudden warming (SSW) in January 2006 was the first major SSW for which globally distributed long-lived trace gas data are available covering the upper troposphere through the lower mesosphere. We use Aura Microwave Limb Sounder (MLS), Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS) data, the SLIMCAT Chemistry Transport Model (CTM), and assimilated meteorological analyses to provide a comprehensive picture of transport during this event. The upper tropospheric ridge that triggered the SSW was associated with an elevated tropopause and layering in trace gas profiles in conjunction with stratospheric and tropospheric intrusions. Anomalous poleward transport (with corresponding quasi-isentropic troposphere-to-stratosphere exchange at the lowest levels studied) in the region over the ridge extended well into the lower stratosphere. In the middle and upper stratosphere, the breakdown of the polar vortex transport barrier was seen in a signature of rapid, widespread mixing in trace gases, including CO, H2O, CH4 and N2O. The vortex broke down slightly later and more slowly in the lower than in the middle stratosphere. In the middle and lower stratosphere, small remnants with trace gas values characteristic of the pre-SSW vortex lingered through the weak and slow recovery of the vortex. The upper stratospheric vortex quickly reformed, and, as enhanced diabatic descent set in, CO descended into this strong vortex, echoing the fall vortex development. Trace gas evolution in the SLIMCAT CTM agrees well with that in the satellite trace gas data from the upper troposphere through the middle stratosphere. In the upper stratosphere and lower mesosphere, the SLIMCAT simulation does not capture the strong descent of mesospheric CO and H2O values into the reformed vortex; this poor CTM performance in the upper stratosphere and lower mesosphere results primarily from biases in the diabatic descent in assimilated analyses.

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Anthropogenic emissions of heat and exhaust gases play an important role in the atmospheric boundary layer, altering air quality, greenhouse gas concentrations and the transport of heat and moisture at various scales. This is particularly evident in urban areas where emission sources are integrated in the highly heterogeneous urban canopy layer and directly linked to human activities which exhibit significant temporal variability. It is common practice to use eddy covariance observations to estimate turbulent surface fluxes of latent heat, sensible heat and carbon dioxide, which can be attributed to a local scale source area. This study provides a method to assess the influence of micro-scale anthropogenic emissions on heat, moisture and carbon dioxide exchange in a highly urbanized environment for two sites in central London, UK. A new algorithm for the Identification of Micro-scale Anthropogenic Sources (IMAS) is presented, with two aims. Firstly, IMAS filters out the influence of micro-scale emissions and allows for the analysis of the turbulent fluxes representative of the local scale source area. Secondly, it is used to give a first order estimate of anthropogenic heat flux and carbon dioxide flux representative of the building scale. The algorithm is evaluated using directional and temporal analysis. The algorithm is then used at a second site which was not incorporated in its development. The spatial and temporal local scale patterns, as well as micro-scale fluxes, appear physically reasonable and can be incorporated in the analysis of long-term eddy covariance measurements at the sites in central London. In addition to the new IMAS-technique, further steps in quality control and quality assurance used for the flux processing are presented. The methods and results have implications for urban flux measurements in dense urbanised settings with significant sources of heat and greenhouse gases.

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Amounts of source gases with stratospheric sinks (CFCs, N2O, CH4) are affected by changes in Brewer–Dobson circulation. Source gases and their degradation products are important for atmospheric chemistry and climate. With a simple model, we examine how amounts and lifetimes of source gases and products depend on speed of the circulation. Transient results differ from steady-state and stratospheric results differ from those for stratosphere plus troposphere. Increases in speed increase the stratospheric burden of source gases, but reduce products and reduce total burdens and lifetimes of source gases

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Cloud computing is usually regarded as being energy efficient and thus emitting less greenhouse gases (GHG) than traditional forms of computing. When the energy consumption of Microsoft’s cloud computing Office 365 (O365) and traditional Office 2010 (O2010) software suites were tested and modeled, some cloud services were found to consume more energy than the traditional form. The developed model in this research took into consideration the energy consumption at the three main stages of data transmission; data center, network, and end user device. Comparable products from each suite were selected and activities were defined for each product to represent a different computing type. Microsoft provided highly confidential data for the data center stage, while the networking and user device stages were measured directly. A new measurement and software apportionment approach was defined and utilized allowing the power consumption of cloud services to be directly measured for the user device stage. Results indicated that cloud computing is more energy efficient for Excel and Outlook which consumed less energy and emitted less GHG than the standalone counterpart. The power consumption of the cloud based Outlook (8%) and Excel (17%) was lower than their traditional counterparts. However, the power consumption of the cloud version of Word was 17% higher than its traditional equivalent. A third mixed access method was also measured for Word which emitted 5% more GHG than the traditional version. It is evident that cloud computing may not provide a unified way forward to reduce energy consumption and GHG. Direct conversion from the standalone package into the cloud provision platform can now consider energy and GHG emissions at the software development and cloud service design stage using the methods described in this research.

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The microbiota of the human gastrointestinal tract plays a key role in nutrition and health. Through the process of fermentation, gut bacteria metabolize various substrates (principally dietary components) to end products such as short-chain fatty acids and gases. This anaerobic metabolism is thought to contribute positively toward host daily energy requirements. However, under certain circumstances, the fermentative process may produce undesirable metabolites. This may cause the onset of gut disorders that can be manifest through both acute and chronic conditions. Moreover, the gut flora may become contaminated by transient pathogens that serve further to upset the normal community structure. There has been a recent increase in the use of dietary components that help to maintain, or even improve, the gut microflora "balance." Probiotics are live microbial feed supplements added to appropriate food vehicles (usually fermented milks), whereas prebiotics are dietary carbohydrates that have a selective metabolism in the colon and serve to increase numbers of bacteria seen as desirable. Because of their purported health-promoting properties, lactic acid-producing bacteria, including bifidobacteria, are the usual target organisms. The market value and biological potential of both approaches are enormous. This article will summarize how efficacious types can be identified.

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Geoengineering by injection of reflective aerosols into the stratosphere has been proposed as a way to counteract the warming effect of greenhouse gases by reducing the intensity of solar radiation reaching the surface. Here, climate model simulations are used to examine the effect of geoengineering on the tropical overturning circulation. The strength of the circulation is related to the atmospheric static stability and has implications for tropical rainfall. The tropical circulation is projected to weaken under anthropogenic global warming. Geoengineering with stratospheric sulfate aerosol does not mitigate this weakening of the circulation. This response is due to a fast adjustment of the troposphere to radiative heating from the aerosol layer. This effect is not captured when geoengineering is modelled as a reduction in total solar irradiance, suggesting caution is required when interpreting model results from solar dimming experiments as analogues for stratospheric aerosol geoengineering.

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CFC-113a (CF3CCl3), CFC-112 (CFCl2CFCl2) and HCFC-133a (CF3CH2Cl) are three newly detected molecules in the atmosphere that are almost certainly emitted as a result of human activity. It is important to characterise the possible contribution of these gases to radiative forcing of climate change and also to provide information on the CO2-equivalence of their emissions. We report new laboratory measurements of absorption cross-sections of these three compounds at a resolution of 0.01 cm−1 for two temperatures 250 K and 295 K in the spectral range of 600–1730 cm−1. These spectra are then used to calculate the radiative efficiencies and global warming potentials (GWP). The radiative efficiencies are found to be between 0.15 and 0.3 W∙m−2∙ppbv−1. The GWP for a 100 year time horizon, relative to carbon dioxide, ranges from 340 for the relatively short-lived HCFC-133a to 3840 for the longer-lived CFC-112. At current (2012) concentrations, these gases make a trivial contribution to total radiative forcing; however, the concentrations of CFC-113a and HCFC-133a are continuing to increase. The 2012 CO2-equivalent emissions, using the GWP (100), are estimated to be about 4% of the current global CO2-equivalent emissions of HFC-134a

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Increasing concentrations of greenhouse gases in the atmosphere are expected to modify the global water cycle with significant consequences for terrestrial hydrology. We assess the impact of climate change on hydrological droughts in a multimodel experiment including seven global impact models (GIMs) driven by bias-corrected climate from five global climate models under four representative concentration pathways (RCPs). Drought severity is defined as the fraction of land under drought conditions. Results show a likely increase in the global severity of hydrological drought at the end of the 21st century, with systematically greater increases for RCPs describing stronger radiative forcings. Under RCP8.5, droughts exceeding 40% of analyzed land area are projected by nearly half of the simulations. This increase in drought severity has a strong signal-to-noise ratio at the global scale, and Southern Europe, the Middle East, the Southeast United States, Chile, and South West Australia are identified as possible hotspots for future water security issues. The uncertainty due to GIMs is greater than that from global climate models, particularly if including a GIM that accounts for the dynamic response of plants to CO2 and climate, as this model simulates little or no increase in drought frequency. Our study demonstrates that different representations of terrestrial water-cycle processes in GIMs are responsible for a much larger uncertainty in the response of hydrological drought to climate change than previously thought. When assessing the impact of climate change on hydrology, it is therefore critical to consider a diverse range of GIMs to better capture the uncertainty.