992 resultados para Atmospheric Chemistry, Ozone, Nitrogen oxides, Marine boundary layer, Photochemistry


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In situ high resolution aircraft measurements of cloud microphysical properties were made in coordination with ground based remote sensing observations of a line of small cumulus clouds, using Radar and Lidar, as part of the Aerosol Properties, PRocesses And InfluenceS on the Earth's climate (APPRAISE) project. A narrow but extensive line (~100 km long) of shallow convective clouds over the southern UK was studied. Cloud top temperatures were observed to be higher than −8 °C, but the clouds were seen to consist of supercooled droplets and varying concentrations of ice particles. No ice particles were observed to be falling into the cloud tops from above. Current parameterisations of ice nuclei (IN) numbers predict too few particles will be active as ice nuclei to account for ice particle concentrations at the observed, near cloud top, temperatures (−7.5 °C). The role of mineral dust particles, consistent with concentrations observed near the surface, acting as high temperature IN is considered important in this case. It was found that very high concentrations of ice particles (up to 100 L−1) could be produced by secondary ice particle production providing the observed small amount of primary ice (about 0.01 L−1) was present to initiate it. This emphasises the need to understand primary ice formation in slightly supercooled clouds. It is shown using simple calculations that the Hallett-Mossop process (HM) is the likely source of the secondary ice. Model simulations of the case study were performed with the Aerosol Cloud and Precipitation Interactions Model (ACPIM). These parcel model investigations confirmed the HM process to be a very important mechanism for producing the observed high ice concentrations. A key step in generating the high concentrations was the process of collision and coalescence of rain drops, which once formed fell rapidly through the cloud, collecting ice particles which caused them to freeze and form instant large riming particles. The broadening of the droplet size-distribution by collision-coalescence was, therefore, a vital step in this process as this was required to generate the large number of ice crystals observed in the time available. Simulations were also performed with the WRF (Weather, Research and Forecasting) model. The results showed that while HM does act to increase the mass and number concentration of ice particles in these model simulations it was not found to be critical for the formation of precipitation. However, the WRF simulations produced a cloud top that was too cold and this, combined with the assumption of continual replenishing of ice nuclei removed by ice crystal formation, resulted in too many ice crystals forming by primary nucleation compared to the observations and parcel modelling.

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A mechanism for amplification of mountain waves, and their associated drag, by parametric resonance is investigated using linear theory and numerical simulations. This mechanism, which is active when the Scorer parameter oscillates with height, was recently classified by previous authors as intrinsically nonlinear. Here it is shown that, if friction is included in the simplest possible form as a Rayleigh damping, and the solution to the Taylor-Goldstein equation is expanded in a power series of the amplitude of the Scorer parameter oscillation, linear theory can replicate the resonant amplification produced by numerical simulations with some accuracy. The drag is significantly altered by resonance in the vicinity of n/l_0 = 2, where l_0 is the unperturbed value of the Scorer parameter and n is the wave number of its oscillation. Depending on the phase of this oscillation, the drag may be substantially amplified or attenuated relative to its non-resonant value, displaying either single maxima or minima, or double extrema near n/l_0 = 2. Both non-hydrostatic effects and friction tend to reduce the magnitude of the drag extrema. However, in exactly inviscid conditions, the single drag maximum and minimum are suppressed. As in the atmosphere friction is often small but non-zero outside the boundary layer, modelling of the drag amplification mechanism addressed here should be quite sensitive to the type of turbulence closure employed in numerical models, or to computational dissipation in nominally inviscid simulations.

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The characteristics of the boundary layer separating a turbulence region from an irrotational (or non-turbulent) flow region are investigated using rapid distortion theory (RDT). The turbulence region is approximated as homogeneous and isotropic far away from the bounding turbulent/non-turbulent (T/NT) interface, which is assumed to remain approximately flat. Inviscid effects resulting from the continuity of the normal velocity and pressure at the interface, in addition to viscous effects resulting from the continuity of the tangential velocity and shear stress, are taken into account by considering a sudden insertion of the T/NT interface, in the absence of mean shear. Profiles of the velocity variances, turbulent kinetic energy (TKE), viscous dissipation rate (epsilon), turbulence length scales, and pressure statistics are derived, showing an excellent agreement with results from direct numerical simulations (DNS). Interestingly, the normalized inviscid flow statistics at the T/NT interface do not depend on the form of the assumed TKE spectrum. Outside the turbulent region, where the flow is irrotational (except inside a thin viscous boundary layer), epsilon decays as z^{-6}, where z is the distance from the T/NT interface. The mean pressure distribution is calculated using RDT, and exhibits a decrease towards the turbulence region due to the associated velocity fluctuations, consistent with the generation of a mean entrainment velocity. The vorticity variance and epsilon display large maxima at the T/NT interface due to the inviscid discontinuities of the tangential velocity variances existing there, and these maxima are quantitatively related to the thickness delta of the viscous boundary layer (VBL). For an equilibrium VBL, the RDT analysis suggests that delta ~ eta (where eta is the Kolmogorov microscale), which is consistent with the scaling law identified in a very recent DNS study for shear-free T/NT interfaces.

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The rapid-distortion model of Hunt & Graham (1978) for the initial distortion of turbulence by a flat boundary is extended to account fully for viscous processes. Two types of boundary are considered: a solid wall and a free surface. The model is shown to be formally valid provided two conditions are satisfied. The first condition is that time is short compared with the decorrelation time of the energy-containing eddies, so that nonlinear processes can be neglected. The second condition is that the viscous layer near the boundary, where tangential motions adjust to the boundary condition, is thin compared with the scales of the smallest eddies. The viscous layer can then be treated using thin-boundary-layer methods. Given these conditions, the distorted turbulence near the boundary is related to the undistorted turbulence, and thence profiles of turbulence dissipation rate near the two types of boundary are calculated and shown to agree extremely well with profiles obtained by Perot & Moin (1993) by direct numerical simulation. The dissipation rates are higher near a solid wall than in the bulk of the flow because the no-slip boundary condition leads to large velocity gradients across the viscous layer. In contrast, the weaker constraint of no stress at a free surface leads to the dissipation rate close to a free surface actually being smaller than in the bulk of the flow. This explains why tangential velocity fluctuations parallel to a free surface are so large. In addition we show that it is the adjustment of the large energy-containing eddies across the viscous layer that controls the dissipation rate, which explains why rapid-distortion theory can give quantitatively accurate values for the dissipation rate. We also find that the dissipation rate obtained from the model evaluated at the time when the model is expected to fail actually yields useful estimates of the dissipation obtained from the direct numerical simulation at times when the nonlinear processes are significant. We conclude that the main role of nonlinear processes is to arrest growth by linear processes of the viscous layer after about one large-eddy turnover time.

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This paper evaluates the relationship between the cloud modification factor (CMF) in the ultraviolet erythe- mal range and the cloud optical depth (COD) retrieved from the Aerosol Robotic Network (AERONET) "cloud mode" algorithm under overcast cloudy conditions (confirmed with sky images) at Granada, Spain, mainly for non-precipitating, overcast and relatively homogenous water clouds. Empirical CMF showed a clear exponential dependence on experimental COD values, decreasing approximately from 0.7 for COD=10 to 0.25 for COD=50. In addition, these COD measurements were used as input in the LibRadtran radia tive transfer code allowing the simulation of CMF values for the selected overcast cases. The modeled CMF exhibited a dependence on COD similar to the empirical CMF, but modeled values present a strong underestimation with respect to the empirical factors (mean bias of 22 %). To explain this high bias, an exhaustive comparison between modeled and experimental UV erythemal irradiance (UVER) data was performed. The comparison revealed that the radiative transfer simulations were 8 % higher than the observations for clear-sky conditions. The rest of the bias (~14 %) may be attributed to the substantial underestimation of modeled UVER with respect to experimental UVER under overcast conditions, although the correlation between both dataset was high (R2 ~ 0.93). A sensitive test showed that the main reason responsible for that underestimation is the experimental AERONET COD used as input in the simulations, which has been retrieved from zenith radiances in the visible range. In this sense, effective COD in the erythemal interval were derived from an iteration procedure based on searching the best match between modeled and experimental UVER values for each selected overcast case. These effective COD values were smaller than AERONET COD data in about 80 % of the overcast cases with a mean relative difference of 22 %.

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The response of East Asian Summer Monsoon (EASM) precipitation to long term changes in regional anthropogenic aerosols (sulphate and black carbon) is explored in an atmospheric general circulation model, the atmospheric component of the UK High-Resolution Global Environment Model v1.2 (HiGAM). Separately, sulphur dioxide (SO2) and black carbon (BC) emissions in 1950 and 2000 over East Asia are used to drive model simulations, while emissions are kept constant at year 2000 level outside this region. The response of the EASM is examined by comparing simulations driven by aerosol emissions representative of 1950 and 2000. The aerosol radiative effects are also determined using an off-line radiative transfer model. During June, July and August, the EASM was not significantly changed as either SO2 or BC emissions increased from 1950 to 2000 levels. However, in September, precipitation is significantly decreased by 26.4% for sulphate aerosol and 14.6% for black carbon when emissions are at the 2000 level. Over 80% of the decrease is attributed to changes in convective precipitation. The cooler land surface temperature over China in September (0.8 °C for sulphate and 0.5 °C for black carbon) due to increased aerosols reduces the surface thermal contrast that supports the EASM circulation. However, mechanisms causing the surface temperature decrease in September are different between sulphate and BC experiments. In the sulphate experiment, the sulphate direct and the 1st indirect radiative effects contribute to the surface cooling. In the BC experiment, the BC direct effect is the main driver of the surface cooling, however, a decrease in low cloud cover due to the increased heating by BC absorption partially counteracts the direct effect. This results in a weaker land surface temperature response to BC changes than to sulphate changes. The resulting precipitation response is also weaker, and the responses of the monsoon circulation are different for sulphate and black carbon experiments. This study demonstrates a mechanism that links regional aerosol emission changes to the precipitation changes of the EASM, and it could be applied to help understand the future changes in EASM precipitation in CMIP5 simulations.

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The formulation and performance of the Met Office visibility analysis and prediction system are described. The visibility diagnostic within the limited-area Unified Model is a function of humidity and a prognostic aerosol content. The aerosol model includes advection, industrial and general urban sources, plus boundary-layer mixing and removal by rain. The assimilation is a 3-dimensional variational scheme in which the visibility observation operator is a very nonlinear function of humidity, aerosol and temperature. A quality control scheme for visibility data is included. Visibility observations can give rise to humidity increments of significant magnitude compared with the direct impact of humidity observations. We present the results of sensitivity studies which show the contribution of different components of the system to improved skill in visibility forecasts. Visibility assimilation is most important within the first 6-12 hours of the forecast and for visibilities below 1 km, while modelling of aerosol sources and advection is important for slightly higher visibilities (1-5 km) and is still significant at longer forecast times

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Results from aircraft and surface observations provided evidence for the existence of mesoscale circulations over the Boreal Ecosystem-Atmosphere Study (BOREAS) domain. Using an integrated approach that included the use of analytical modeling, numerical modeling, and data analysis, we have found that there are substantial contributions to the total budgets of heat over the BOREAS domain generated by mesoscale circulations. This effect is largest when the synoptic flow is relatively weak, yet it is present under less favorable conditions, as shown by the case study presented here. While further analysis is warranted to document this effect, the existence of mesoscale flow is not surprising, since it is related to the presence of landscape patches, including lakes, which are of a size on the order of the local Rossby radius and which have spatial differences in maximum sensible heat flux of about 300 W m−2. We have also analyzed the vertical temperature profile simulated in our case study as well as high-resolution soundings and we have found vertical profiles of temperature change above the boundary layer height, which we attribute in part to mesoscale contributions. Our conclusion is that in regions with organized landscapes, such as BOREAS, even with relatively strong synoptic winds, dynamical scaling criteria should be used to assess whether mesoscale effects should be parameterized or explicitly resolved in numerical models of the atmosphere.

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The analysis presented in this paper suggests that the larger heating over the boreal forest in the spring and summer, as contrasted with weaker heating over the adjacent tundra, results in a preferred position of the polar front along the northern edge of the boreal forest. This positioning is well documented in the literature (see, for example, Bryson, 1966; Barry and Hare, 1974; Kreps and Barry, 1970). This heating results from the lower albedo of the boreal forest which is not compensated by an increase in transpiration, even with the larger leaf area index of the forest. The warmer temperatures are mixed upward by the deep boundary layer over the forest and mesoscale circulations which result from the patchiness of heating associated with the heterogeneous landscapes of the forest. Thus in contrast to previous assumptions in which the arctic front position in the summer determines the northern limit of the boreal tree line, our study suggests the boreal forest itself significantly influences the preferred position of the front. This conclusion reinforces the findings of Bonan et al. (1992) and Foley et al. (1994) on the important role of boreal forest-tundra interactions with climate.

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In order to validate the reported precision of space‐based atmospheric composition measurements, validation studies often focus on measurements in the tropical stratosphere, where natural variability is weak. The scatter in tropical measurements can then be used as an upper limit on single‐profile measurement precision. Here we introduce a method of quantifying the scatter of tropical measurements which aims to minimize the effects of short‐term atmospheric variability while maintaining large enough sample sizes that the results can be taken as representative of the full data set. We apply this technique to measurements of O3, HNO3, CO, H2O, NO, NO2, N2O, CH4, CCl2F2, and CCl3F produced by the Atmospheric Chemistry Experiment–Fourier Transform Spectrometer (ACE‐FTS). Tropical scatter in the ACE‐FTS retrievals is found to be consistent with the reported random errors (RREs) for H2O and CO at altitudes above 20 km, validating the RREs for these measurements. Tropical scatter in measurements of NO, NO2, CCl2F2, and CCl3F is roughly consistent with the RREs as long as the effect of outliers in the data set is reduced through the use of robust statistics. The scatter in measurements of O3, HNO3, CH4, and N2O in the stratosphere, while larger than the RREs, is shown to be consistent with the variability simulated in the Canadian Middle Atmosphere Model. This result implies that, for these species, stratospheric measurement scatter is dominated by natural variability, not random error, which provides added confidence in the scientific value of single‐profile measurements.

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Approximately 1–2% of net primary production by land plants is re-emitted to the atmosphere as isoprene and monoterpenes. These emissions play major roles in atmospheric chemistry and air pollution–climate interactions. Phenomenological models have been developed to predict their emission rates, but limited understanding of the function and regulation of these emissions has led to large uncertainties in model projections of air quality and greenhouse gas concentrations. We synthesize recent advances in diverse fields, from cell physiology to atmospheric remote sensing, and use this information to propose a simple conceptual model of volatile isoprenoid emission based on regulation of metabolism in the chloroplast. This may provide a robust foundation for scaling up emissions from the cellular to the global scale.

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A detailed spectrally-resolved extraterrestrial solar spectrum (ESS) is important for line-by-line radiative transfer modeling in the near-infrared (near-IR). Very few observationally-based high-resolution ESS are available in this spectral region. Consequently the theoretically-calculated ESS by Kurucz has been widely adopted. We present the CAVIAR (Continuum Absorption at Visible and Infrared Wavelengths and its Atmospheric Relevance) ESS which is derived using the Langley technique applied to calibrated observations using a ground-based high-resolution Fourier transform spectrometer (FTS) in atmospheric windows from 2000–10000 cm-1 (1–5 μm). There is good agreement between the strengths and positions of solar lines between the CAVIAR and the satellite-based ACE-FTS (Atmospheric Chemistry Experiment-FTS) ESS, in the spectral region where they overlap, and good agreement with other ground-based FTS measurements in two near-IR windows. However there are significant differences in the structure between the CAVIAR ESS and spectra from semi-empirical models. In addition, we found a difference of up to 8 % in the absolute (and hence the wavelength-integrated) irradiance between the CAVIAR ESS and that of Thuillier et al., which was based on measurements from the Atmospheric Laboratory for Applications and Science satellite and other sources. In many spectral regions, this difference is significant, as the coverage factor k = 2 (or 95 % confidence limit) uncertainties in the two sets of observations do not overlap. Since the total solar irradiance is relatively well constrained, if the CAVIAR ESS is correct, then this would indicate an integrated “loss” of solar irradiance of about 30 W m-2 in the near-IR that would have to be compensated by an increase at other wavelengths.

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In order to evaluate the future potential benefits of emission regulation on regional air quality, while taking into account the effects of climate change, off-line air quality projection simulations are driven using weather forcing taken from regional climate models. These regional models are themselves driven by simulations carried out using global climate models (GCM) and economical scenarios. Uncertainties and biases in climate models introduce an additional “climate modeling” source of uncertainty that is to be added to all other types of uncertainties in air quality modeling for policy evaluation. In this article we evaluate the changes in air quality-related weather variables induced by replacing reanalyses-forced by GCM-forced regional climate simulations. As an example we use GCM simulations carried out in the framework of the ERA-interim programme and of the CMIP5 project using the Institut Pierre-Simon Laplace climate model (IPSLcm), driving regional simulations performed in the framework of the EURO-CORDEX programme. In summer, we found compensating deficiencies acting on photochemistry: an overestimation by GCM-driven weather due to a positive bias in short-wave radiation, a negative bias in wind speed, too many stagnant episodes, and a negative temperature bias. In winter, air quality is mostly driven by dispersion, and we could not identify significant differences in either wind or planetary boundary layer height statistics between GCM-driven and reanalyses-driven regional simulations. However, precipitation appears largely overestimated in GCM-driven simulations, which could significantly affect the simulation of aerosol concentrations. The identification of these biases will help interpreting results of future air quality simulations using these data. Despite these, we conclude that the identified differences should not lead to major difficulties in using GCM-driven regional climate simulations for air quality projections.

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We investigate the role of the anthropogenic heat flux on the urban heat island of London. To do this, the time-varying anthropogenic heat flux is added to an urban surface-energy balance parametrization, the Met Office–Reading Urban Surface Exchange Scheme (MORUSES), implemented in a 1 km resolution version of the UK Met Office Unified Model. The anthropogenic heat flux is derived from energy-demand data for London and is specified on the model's 1 km grid; it includes variations on diurnal and seasonal time-scales. We contrast a spring case with a winter case, to illustrate the effects of the larger anthropogenic heat flux in winter and the different roles played by thermodynamics in the different seasons. The surface-energy balance channels the anthropogenic heat into heating the urban surface, which warms slowly because of the large heat capacity of the urban surface. About one third of this additional warming goes into increasing the outgoing long-wave radiation and only about two thirds goes into increasing the sensible heat flux that warms the atmosphere. The anthropogenic heat flux has a larger effect on screen-level temperatures in the winter case, partly because the anthropogenic flux is larger then and partly because the boundary layer is shallower in winter. For the specific winter case studied here, the anthropogenic heat flux maintains a well-mixed boundary layer through the whole night over London, whereas the surrounding rural boundary layer becomes strongly stably stratified. This finding is likely to have important implications for air quality in winter. On the whole, inclusion of the anthropogenic heat flux improves the comparison between model simulations and measurements of screen-level temperature slightly and indicates that the anthropogenic heat flux is beginning to be an important factor in the London urban heat island.

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The atmospheric circulation over the North Atlantic-European sector experienced exceptional but highly contrasting conditions in the recent 2010 and 2012 winters (November-March; with the year dated by the relevant January). Evidence is given for the remarkably different locations of the eddy-driven westerly jet over the North Atlantic. In the 2010 winter the maximum of the jet stream was systematically between 30ºN and 40ºN (in the ‘south jet regime’), while in the 2012 winter it was predominantly located around 55ºN (north jet regime). These jet features underline the occurrence of either weak flow (2010) or strong and persistent ridges throughout the troposphere (2012). This is confirmed by the very different occurrence of blocking systems over the North Atlantic, associated with episodes of strong cyclonic (anticyclonic) Rossby wave breaking in 2010 (2012) winters. These dynamical features underlie strong precipitation and temperature anomalies over parts of Europe, with detrimental impacts on many socioeconomic sectors. Despite the highly contrasting atmospheric states, mid and high-latitude boundary conditions do not reveal strong differences in these two winters. The two winters were associated with opposite ENSO phases, but there is no causal evidence of a remote forcing from the Pacific sea surface temperatures. Finally, the exceptionality of the two winters is demonstrated in relation to the last 140 years. It is suggested that these winters may be seen as archetypes of North Atlantic jet variability under current climate conditions.