993 resultados para CH4 fluxes


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In late February 2010 the extraordinary windstorm Xynthia crossed over Southwestern and Central Europe and caused severe damage, affecting particularly the Spanish and French Atlantic coasts. The storm was embedded in uncommon large-scale atmospheric and boundary conditions prior to and during its development, namely enhanced sea surface temperatures (SST) within the low-level entrainment zone of air masses, an unusual southerly position of the polar jet stream, and a remarkable split jet structure in the upper troposphere. To analyse the processes that led to the rapid intensification of this exceptional storm originating close to the subtropics (30°N), the sensitivity of the cyclone intensification to latent heat release is determined using the regional climate model COSMO-CLM forced with ERA-Interim data. A control simulation with observed SST shows that moist and warm air masses originating from the subtropical North Atlantic were involved in the cyclogenesis process and led to the formation of a vertical tower with high values of potential vorticity (PV). Sensitivity studies with reduced SST or increased laminar boundary roughness for heat led to reduced surface latent heat fluxes. This induced both a weaker and partly retarded development of the cyclone and a weakening of the PV-tower together with reduced diabatic heating rates, particularly at lower and mid levels. We infer that diabatic processes played a crucial role during the phase of rapid deepening of Xynthia and thus to its intensity over the Southeastern North Atlantic. We suggest that windstorms like Xynthia may occur more frequently under future climate conditions due to the warming SSTs and potentially enhanced latent heat release, thus increasing the windstorm risk for Southwestern Europe.

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This manuscript describes the energy and water components of a new community land surface model called the Joint UK Land Environment Simulator (JULES). This is developed from the Met Office Surface Exchange Scheme (MOSES). It can be used as a stand alone land surface model driven by observed forcing data, or coupled to an atmospheric global circulation model. The JULES model has been coupled to the Met Office Unified Model (UM) and as such provides a unique opportunity for the research community to contribute their research to improve both world-leading operational weather forecasting and climate change prediction systems. In addition JULES, and its forerunner MOSES, have been the basis for a number of very high-profile papers concerning the land-surface and climate over the last decade. JULES has a modular structure aligned to physical processes, providing the basis for a flexible modelling platform.

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The role of eddy fluxes in the general circulation is often approached by treating eddies as (macro)turbulence. In this approach, the eddies act to diffuse certain quasiconservative quantities, such as potential vorticity (PV), along isentropic surfaces in the free atmosphere. The eddy fluxes are determined primarily by the eddy diffusivities and are necessarily down-gradient of the basic state PV field. Support for the (macro)turbulence approach stems from the fact that the eddy fluxes of PV in the free atmosphere are generally down-gradient in the long-term mean. Here we call attention to a pronounced and significant region of upgradient eddy PV fluxes on the poleward flank of the jet core in both hemispheres. The region of up-gradient (i.e., notionally “antidiffusive”) eddy PV fluxes is most pronounced during the winter and spring seasons and partially contradicts the turbulence approach described above. Analyses of the PV variance (potential enstrophy) budget suggest that the up-gradient PV fluxes represent local wave decay and are maintained by poleward fluxes of PV variance. Finite-amplitude effects thus represent leading order contributions to the PV variance budget, whereas dissipation is only of secondary importance locally. The appearance of up-gradient PV fluxes in the long-term mean is associated with the poleward shift of the jet—and thus the region of wave decay relative to wave growth—following wave-breaking events.

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Sensible heat fluxes (QH) are determined using scintillometry and eddy covariance over a suburban area. Two large aperture scintillometers provide spatially integrated fluxes across path lengths of 2.8 km and 5.5 km over Swindon, UK. The shorter scintillometer path spans newly built residential areas and has an approximate source area of 2-4 km2, whilst the long path extends from the rural outskirts to the town centre and has a source area of around 5-10 km2. These large-scale heat fluxes are compared with local-scale eddy covariance measurements. Clear seasonal trends are revealed by the long duration of this dataset and variability in monthly QH is related to the meteorological conditions. At shorter time scales the response of QH to solar radiation often gives rise to close agreement between the measurements, but during times of rapidly changing cloud cover spatial differences in the net radiation (Q*) coincide with greater differences between heat fluxes. For clear days QH lags Q*, thus the ratio of QH to Q* increases throughout the day. In summer the observed energy partitioning is related to the vegetation fraction through use of a footprint model. The results demonstrate the value of scintillometry for integrating surface heterogeneity and offer improved understanding of the influence of anthropogenic materials on surface-atmosphere interactions.

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Global hydrographic and air–sea freshwater flux datasets are used to investigate ocean salinity changes over 1950–2010 in relation to surface freshwater flux. On multi-decadal timescales, surface salinity increases (decreases) in evaporation (precipitation) dominated regions, the Atlantic–Pacific salinity contrast increases, and the upper thermocline salinity maximum increases while the salinity minimum of intermediate waters decreases. Potential trends in E–P are examined for 1950–2010 (using two reanalyses) and 1979–2010 (using four reanalyses and two blended products). Large differences in the 1950–2010 E–P trend patterns are evident in several regions, particularly the North Atlantic. For 1979–2010 some coherency in the spatial change patterns is evident but there is still a large spread in trend magnitude and sign between the six E–P products. However, a robust pattern of increased E–P in the southern hemisphere subtropical gyres is seen in all products. There is also some evidence in the tropical Pacific for a link between the spatial change patterns of salinity and E–P associated with ENSO. The water cycle amplification rate over specific regions is subsequently inferred from the observed 3-D salinity change field using a salt conservation equation in variable isopycnal volumes, implicitly accounting for the migration of isopycnal surfaces. Inferred global changes of E–P over 1950–2010 amount to an increase of 1 ± 0.6 % in net evaporation across the subtropics and an increase of 4.2 ± 2 % in net precipitation across subpolar latitudes. Amplification rates are approximately doubled over 1979–2010, consistent with accelerated broad-scale warming but also coincident with much improved salinity sampling over the latter period.

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The modulation of air–sea heat fluxes by geostrophic eddies due to the stirring of temperature at the sea surface is discussed and quantified. It is argued that the damping of eddy temperature variance by such air–sea fluxes enhances the dissipation of surface temperature fields. Depending on the time scale of damping relative to that of the eddying motions, surface eddy diffusivities can be significantly enhanced over interior values. The issues are explored and quantified in a controlled setting by driving a tracer field, a proxy for sea surface temperature, with surface altimetric observations in the Antarctic Circumpolar Current (ACC) of the Southern Ocean. A new, tracer-based diagnostic of eddy diffusivity is introduced, which is related to the Nakamura effective diffusivity. Using this, the mixed layer lateral eddy diffusivities associated with (i) eddy stirring and small-scale mixing and (ii) surface damping by air–sea interaction is quantified. In the ACC, a diffusivity associated with surface damping of a comparable magnitude to that associated with eddy stirring (;500 m2 s21) is found. In frontal regions prevalent in the ACC, an augmentation of surface lateral eddy diffusivities of this magnitude is equivalent to an air–sea flux of 100 W m22 acting over a mixed layer depth of 100 m, a very significant effect. Finally, the implications for other tracer fields such as salinity, dissolved gases, and chlorophyll are discussed. Different tracers are found to have surface eddy diffusivities that differ significantly in magnitude.

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Airborne measurements within the urban mixing layer (360 m) over Greater London are used to quantify CO2 emissions at the meso-scale. Daytime CO2 fluxes, calculated by the Integrative Mass Boundary Layer (IMBL) method, ranged from 46 to 104 μmol CO2 m−2 s−1 for four days in October 2011. The day-to-day variability of IMBL fluxes is at the same order of magnitude as for surface eddy-covariance fluxes observed in central London. Compared to fluxes derived from emissions inventory, the IMBL method gives both lower (by −37%) and higher (by 19%) estimates. The sources of uncertainty of applying the IMBL method in urban areas are discussed and guidance for future studies is given.

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We report for the first time a detailed procedure for creating a simulation model of energetically stable, folded graphene-like pores and simulation results of CO2/CH4 and CO2/N2 separation using these structures. We show that folding of graphene structures is a very promising method to improve the separation of CO2 from mixtures with CH4 and N2. The separation properties of the analyzed materials are compared with carbon nanotubes having similar diameters or S/V ratio. The presented results have potential importance in the field of CO2 capture and sequestration.

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Transport of pollution and heatout of streets into the boundary layer above is not currently understood and so fluxes cannot be quantified. Scalar concentration within the street is determined by the flux out of it and so quantifying fluxes for turbulent flow over a rough urban surface is essential. We have developed a naphthalene sublimation technique to measure transfer from a two-dimensional street canyon in a wind tunnel for the case of flow perpendicular to the street. The street was coated with naphthalene, which sublimes at room temperature, so that the vapour represented the scalar source. The transfer velocity wT relates the flux out of the canyon to the concentration within it and is shown to be linearly related to windspeed above the street. The dimensionless transfer coefficient wT/Uδ represents the ventilation efficiency of the canyon (here, wT is a transfer velocity,Uδ is the wind speed at the boundary-layer top). Observed values are between 1.5 and 2.7 ×10-3 and, for the case where H/W→0 (ratio of buildingheight to street width), values are in the same range as estimates of transfer from a flat plate, giving confidence that the technique yields accurate values for street canyon scalar transfer. wT/Uδ varies with aspect ratio (H/W), reaching a maximum in the wake interference regime (0.3 < H/W < 0.65). However, when upstream roughness is increased, the maximum in wT/Uδ reduces, suggesting that street ventilation is less sensitive to H/W when the flow is in equilibrium with the urban surface. The results suggest that using naphthalene sublimation with wind-tunnel models of urban surfaces can provide a direct measure of area-averaged scalar fluxes.

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The state-resolved reaction probability of CH4 on Pt�110-�1�2 was measured as a function of CH4 translational energy for four vibrational eigenstates comprising different amounts of C-H stretch and bend excitation. Mode-specific reactivity is observed both between states from different polyads and between isoenergetic states belonging to the same polyad of CH4. For the stretch/bend combination states, the vibrational efficacy of reaction activation is observed to be higher than for either pure C-H stretching or pure bending states, demonstrating a concerted role of stretch and bend excitation in C-H bond scission. This concerted role, reflected by the nonadditivity of the vibrational efficacies, is consistent with transition state structures found by ab initio calculations and indicates that current dynamical models of CH4 chemisorption neglect an important degree of freedom by including only C-H stretching motion.

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The chemisorption of CH4 on Pt{110}-(1 x 2) has been studied by vibrational analysis of the reaction pathway defined by the potential energy surface and, in time reversal, by first-principles molecular dynamics simulations of CH4 associative desorption, with the electronic structure treated explicitly using density functional theory. We find that the symmetric stretch vibration ν1 is strongly coupled to the reaction coordinate; our results therefore provide a firm theoretical basis for recently reported state-resolved reactivity measurements, which show that excitation of the ν1 normal mode is the most efficient way to enhance the reaction probability

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We have investigated methane (CH4) dissociative chemisorption on the Ni{100} surface by first-principles molecular dynamics (MD) simulations. Our results show that this reaction is mode-specific, with the n1 state being the most strongly coupled to efficient energy flow into the reaction coordinate when the molecule reaches the transition state. By performing MD simulations for two different transition state (TS) structures we provide evidence of TS structure-specific energy redistribution in methane chemisorption. Our results are compared with recently reported state-resolved measurement of methane adsorption probability on nickel surfaces, and we find that a strong correlation exists between the highest vibrational efficacy measured on Ni{100} for the n1 state and the calculated highest fractional vibrational energy content in this mode.

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A millimetre-wave scintillometer was paired with an infrared scintillometer, enabling estimation of large-area evapotranspiration across northern Swindon, a suburban area in the UK. Both sensible and latent heat fluxes can be obtained using this "two-wavelength" technique, as it is able to provide both temperature and humidity structure parameters, offering a major advantage over conventional single-wavelength scintillometry. The first paper of this two-part series presented the measurement theory and structure parameters. In this second paper, heat fluxes are obtained and analysed. These fluxes, estimated using two-wavelength scintillometry over an urban area, are the first of their kind. Source area modelling suggests the scintillometric fluxes are representative of 5–10 km2. For comparison, local-scale (0.05–0.5 km2) fluxes were measured by an eddy covariance station. Similar responses to seasonal changes are evident at the different scales but the energy partitioning varies between source areas. The response to moisture availability is explored using data from 2 consecutive years with contrasting rainfall patterns (2011–2012). This extensive data set offers insight into urban surface-atmosphere interactions and demonstrates the potential for two-wavelength scintillometry to deliver fluxes over mixed land cover, typically representative of an area 1–2 orders of magnitude greater than for eddy covariance measurements. Fluxes at this scale are extremely valuable for hydro-meteorological model evaluation and assessment of satellite data products

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We utilized an ecosystem process model (SIPNET, simplified photosynthesis and evapotranspiration model) to estimate carbon fluxes of gross primary productivity and total ecosystem respiration of a high-elevation coniferous forest. The data assimilation routine incorporated aggregated twice-daily measurements of the net ecosystem exchange of CO2 (NEE) and satellite-based reflectance measurements of the fraction of absorbed photosynthetically active radiation (fAPAR) on an eight-day timescale. From these data we conducted a data assimilation experiment with fifteen different combinations of available data using twice-daily NEE, aggregated annual NEE, eight-day f AP AR, and average annual fAPAR. Model parameters were conditioned on three years of NEE and fAPAR data and results were evaluated to determine the information content from the different combinations of data streams. Across the data assimilation experiments conducted, model selection metrics such as the Bayesian Information Criterion and Deviance Information Criterion obtained minimum values when assimilating average annual fAPAR and twice-daily NEE data. Application of wavelet coherence analyses showed higher correlations between measured and modeled fAPAR on longer timescales ranging from 9 to 12 months. There were strong correlations between measured and modeled NEE (R2, coefficient of determination, 0.86), but correlations between measured and modeled eight-day fAPAR were quite poor (R2 = −0.94). We conclude that this inability to determine fAPAR on eight-day timescale would improve with the considerations of the radiative transfer through the plant canopy. Modeled fluxes when assimilating average annual fAPAR and annual NEE were comparable to corresponding results when assimilating twice-daily NEE, albeit at a greater uncertainty. Our results support the conclusion that for this coniferous forest twice-daily NEE data are a critical measurement stream for the data assimilation. The results from this modeling exercise indicate that for this coniferous forest, average annuals for satellite-based fAPAR measurements paired with annual NEE estimates may provide spatial detail to components of ecosystem carbon fluxes in proximity of eddy covariance towers. Inclusion of other independent data streams in the assimilation will also reduce uncertainty on modeled values.