Simple model of adsorption on external surface of carbon nanotubes: a new analytical approach basing on molecular simulation data

Nitrogen adsorption on carbon nanotubes is wide- ly studied because nitrogen adsorption isotherm measurement is a standard method applied for porosity characterization. A further reason is that carbon nanotubes are potential adsorbents for separation of nitrogen from oxygen in air. The study presented here describes the results of GCMC simulations of nitrogen (three site model) adsorption on single and multi walled closed nanotubes. The results obtained are described by a new adsorption isotherm model proposed in this study. The model can be treated as the tube analogue of the GAB isotherm taking into account the lateral adsorbate-adsorbate interactions. We show that the model describes the simulated data satisfactorily. Next this new approach is applied for a description of experimental data measured on different commercially available (and characterized using HRTEM) carbon nanotubes. We show that generally a quite good fit is observed and therefore it is suggested that the observed mechanism of adsorption in the studied materials is mainly determined by adsorption on tubes separated at large distances, so the tubes behave almost independently.

The basic ingredients of the North Atlantic Storm Track. Part II: Sea surface temperatures

The impact of North Atlantic SST patterns on the storm track is investigated using a hierarchy of GCM simulations using idealized (aquaplanet) and “semirealistic” boundary conditions in the atmospheric component (HadAM3) of the third climate configuration of the Met Office Unified Model (HadCM3). This framework enables the mechanisms determining the tropospheric response to North Atlantic SST patterns to be examined, both in isolation and in combination with continental-scale landmasses and orography. In isolation, a “Gulf Stream” SST pattern acts to strengthen the downstream storm track while a “North Atlantic Drift” SST pattern weakens it. These changes are consistent with changes in the extratropical SST gradient and near-surface baroclinicity, and each storm-track response is associated with a consistent change in the tropospheric jet structure. Locally enhanced near-surface horizontal wind convergence is found over the warm side of strengthened SST gradients associated with ascending air and increased precipitation, consistent with previous studies. When the combined SST pattern is introduced into the semirealistic framework (including the “North American” continent and the “Rocky Mountains”), the results suggest that the topographically generated southwest–northeast tilt in the North Atlantic storm track is enhanced. In particular, the Gulf Stream shifts the storm track south in the western Atlantic whereas the strong high-latitude SST gradient in the northeastern Atlantic enhances the storm track there.

Systematic winter sea-surface temperature biases in the northern Arabian Sea in HiGEM and the CMIP3 models

Analysis of 20th century simulations of the High resolution Global Environment Model (HiGEM) and the Third Coupled Model Intercomparison Project (CMIP3) models shows that most have a cold sea-surface temperature (SST) bias in the northern Arabian Sea during boreal winter. The association between Arabian Sea SST and the South Asian monsoon has been widely studied in observations and models, with winter cold biases known to be detrimental to rainfall simulation during the subsequent monsoon in coupled general circulation models (GCMs). However, the causes of these SST biases are not well understood. Indeed this is one of the first papers to address causes of the cold biases. The models show anomalously strong north-easterly winter monsoon winds and cold air temperatures in north-west India, Pakistan and beyond. This leads to the anomalous advection of cold, dry air over the Arabian Sea. The cold land region is also associated with an anomalously strong meridional surface temperature gradient during winter, contributing to the enhanced low-level convergence and excessive precipitation over the western equatorial Indian Ocean seen in many models.

Statistical analysis of eight surface ozone measurement series for various sites in Ireland

Data from various stations having different measurement record periods between 1988 and 2007 are analyzed to investigate the surface ozone concentration, long-term trends, and seasonal changes in and around Ireland. Time series statistical analysis is performed on the monthly mean data using seasonal and trend decomposition procedures and the Box-Jenkins approach (autoregressive integrated moving average). In general, ozone concentrations in the Irish region are found to have a negative trend at all sites except at the coastal sites of Mace Head and Valentia. Data from the most polluted Dublin city site have shown a very strong negative trend of −0.33 ppb/yr with a 95% confidence limit of 0.17 ppb/yr (i.e., −0.33 ± 0.17) for the period 2002−2007, and for the site near the city of Cork, the trend is found to be −0.20 ± 0.11 ppb/yr over the same period. The negative trend for other sites is more pronounced when the data span is considered from around the year 2000 to 2007. Rural sites of Wexford and Monaghan have also shown a very strong negative trend of −0.99 ± 0.13 and −0.58 ± 0.12, respectively, for the period 2000−2007. Mace Head, a site that is representative of ozone changes in the air advected from the Atlantic to Europe in the marine planetary boundary layer, has shown a positive trend of about +0.16 ± 0.04 ppb per annum over the entire period 1988−2007, but this positive trend has reduced during recent years (e.g., in the period 2001−2007). Cluster analysis for back trajectories are performed for the stations having a long record of data, Mace Head and Lough Navar. For Mace Head, the northern and western clean air sectors have shown a similar positive trend (+0.17 ± 0.02 ppb/yr for the northern sector and +0.18 ± 0.02 ppb/yr for the western sector) for the whole period, but partial analysis for the clean western sector at Mace Head shows different trends during different time periods with a decrease in the positive trend since 1988 indicating a deceleration in the ozone trend for Atlantic air masses entering Europe.

The influence of stratospheric vortex displacements and splits on surface climate

A strong link exists between stratospheric variability and anomalous weather patterns at the earth’s surface. Specifically, during extreme variability of the Arctic polar vortex termed a “weak vortex event,” anomalies can descend from the upper stratosphere to the surface on time scales of weeks. Subsequently the outbreak of cold-air events have been noted in high northern latitudes, as well as a quadrupole pattern in surface temperature over the Atlantic and western European sectors, but it is currently not understood why certain events descend to the surface while others do not. This study compares a new classification technique of weak vortex events, based on the distribution of potential vorticity, with that of an existing technique and demonstrates that the subdivision of such events into vortex displacements and vortex splits has important implications for tropospheric weather patterns on weekly to monthly time scales. Using reanalysis data it is found that vortex splitting events are correlated with surface weather and lead to positive temperature anomalies over eastern North America of more than 1.5 K, and negative anomalies over Eurasia of up to −3 K. Associated with this is an increase in high-latitude blocking in both the Atlantic and Pacific sectors and a decrease in European blocking. The corresponding signals are weaker during displacement events, although ultimately they are shown to be related to cold-air outbreaks over North America. Because of the importance of stratosphere–troposphere coupling for seasonal climate predictability, identifying the type of stratospheric variability in order to capture the correct surface response will be necessary.

The role of anomalous SST and surface fluxes over the Southeastern North Atlantic in the explosive development of windstorm Xynthia

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.

Urban surface energy balance models: model characteristics and methodology for a comparison study

Many urban surface energy balance models now exist. These vary in complexity from simple schemes that represent the city as a concrete slab, to those which incorporate detailed representations of momentum and energy fluxes distributed within the atmospheric boundary layer. While many of these schemes have been evaluated against observations, with some models even compared with the same data sets, such evaluations have not been undertaken in a controlled manner to enable direct comparison. For other types of climate model, for instance the Project for Intercomparison of Land-Surface Parameterization Schemes (PILPS) experiments (Henderson-Sellers et al., 1993), such controlled comparisons have been shown to provide important insights into both the mechanics of the models and the physics of the real world. This paper describes the progress that has been made to date on a systematic and controlled comparison of urban surface schemes. The models to be considered, and their key attributes, are described, along with the methodology to be used for the evaluation.

Mixed layer lateral eddy fluxes mediated by air-sea interaction

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.

Sea surface temperature datasets for climate applications from Phase 1 of the European Space Agency Climate Change Initiative (SST CCI)

Sea surface temperature (SST) datasets have been generated from satellite observations for the period 1991–2010, intended for use in climate science applications. Attributes of the datasets specifically relevant to climate applications are: first, independence from in situ observations; second, effort to ensure homogeneity and stability through the time-series; third, context-specific uncertainty estimates attached to each SST value; and, fourth, provision of estimates of both skin SST (the fundamental measure- ment, relevant to air-sea fluxes) and SST at standard depth and local time (partly model mediated, enabling comparison with his- torical in situ datasets). These attributes in part reflect requirements solicited from climate data users prior to and during the project. Datasets consisting of SSTs on satellite swaths are derived from the Along-Track Scanning Radiometers (ATSRs) and Advanced Very High Resolution Radiometers (AVHRRs). These are then used as sole SST inputs to a daily, spatially complete, analysis SST product, with a latitude-longitude resolution of 0.05°C and good discrimination of ocean surface thermal features. A product user guide is available, linking to reports describing the datasets’ algorithmic basis, validation results, format, uncer- tainty information and experimental use in trial climate applications. Future versions of the datasets will span at least 1982–2015, better addressing the need in many climate applications for stable records of global SST that are at least 30 years in length.

Meteorological forcing data for urban outdoor thermal comfort models from a coupled convective boundary layer and surface energy balance scheme

Site-specific meteorological forcing appropriate for applications such as urban outdoor thermal comfort simulations can be obtained using a newly coupled scheme that combines a simple slab convective boundary layer (CBL) model and urban land surface model (ULSM) (here two ULSMs are considered). The former simulates daytime CBL height, air temperature and humidity, and the latter estimates urban surface energy and water balance fluxes accounting for changes in land surface cover. The coupled models are tested at a suburban site and two rural sites, one irrigated and one unirrigated grass, in Sacramento, U.S.A. All the variables modelled compare well to measurements (e.g. coefficient of determination = 0.97 and root mean square error = 1.5 °C for air temperature). The current version is applicable to daytime conditions and needs initial state conditions for the CBL model in the appropriate range to obtain the required performance. The coupled model allows routine observations from distant sites (e.g. rural, airport) to be used to predict air temperature and relative humidity in an urban area of interest. This simple model, which can be rapidly applied, could provide urban data for applications such as air quality forecasting and building energy modelling, in addition to outdoor thermal comfort.

Improved seasonal prediction of the hot summer of 2003 over Europe through better representation of uncertainty in the land surface

Methods to explicitly represent uncertainties in weather and climate models have been developed and refined over the past decade, and have reduced biases and improved forecast skill when implemented in the atmospheric component of models. These methods have not yet been applied to the land surface component of models. Since the land surface is strongly coupled to the atmospheric state at certain times and in certain places (such as the European summer of 2003), improvements in the representation of land surface uncertainty may potentially lead to improvements in atmospheric forecasts for such events. Here we analyse seasonal retrospective forecasts for 1981–2012 performed with the European Centre for Medium-Range Weather Forecasts’ (ECMWF) coupled ensemble forecast model. We consider two methods of incorporating uncertainty into the land surface model (H-TESSEL): stochastic perturbation of tendencies, and static perturbation of key soil parameters. We find that the perturbed parameter approach considerably improves the forecast of extreme air temperature for summer 2003, through better representation of negative soil moisture anomalies and upward sensible heat flux. Averaged across all the reforecasts the perturbed parameter experiment shows relatively little impact on the mean bias, suggesting perturbations of at least this magnitude can be applied to the land surface without any degradation of model climate. There is also little impact on skill averaged across all reforecasts and some evidence of overdispersion for soil moisture. The stochastic tendency experiments show a large overdispersion for the soil temperature fields, indicating that the perturbation here is too strong. There is also some indication that the forecast of the 2003 warm event is improved for the stochastic experiments, however the improvement is not as large as observed for the perturbed parameter experiment.

The interaction of moist convection and mid-level dry air in the advance of the onset of the Indian monsoon

The advance of the onset of the Indian monsoon is here explained in terms of a balance between the low-level monsoon flow and an over-running intrusion of mid-tropospheric dry air. The monsoon advances, over a period of about 6 weeks, from the south of the country to the northwest. Given that the low-level monsoon winds are westerly or southwesterly, and the midlevel winds northwesterly, the monsoon onset propagates upwind relative to midlevel flow, and perpendicular to the low-level flow, and is not directly caused by moisture flux toward the northwest. Lacking a conceptual model for the advance means that it has been hard to understand and correct known biases in weather and climate prediction models. The mid-level northwesterlies form a wedge of dry air that is deep in the far northwest of India and over-runs the monsoon flow. The dry layer is moistened from below by shallow cumulus and congestus clouds, so that the profile becomes much closer to moist adiabatic, and the dry layer is much shallower in the vertical, toward the southeast of India. The profiles associated with this dry air show how the most favourable environment for deep convection occurs in the south, and onset occurs here first. As the onset advances across India, the advection of moisture from the Arabian Sea becomes stronger, and the mid-level dry air is increasingly moistened from below. This increased moistening makes the wedge of dry air shallower throughout its horizontal extent, and forces the northern limit of moist convection to move toward the northwest. Wetting of the land surface by rainfall will further reinforce the north-westward progression, by sustaining the supply of boundary layer moisture and shallow cumulus. The local advance of the monsoon onset is coincident with weakening of the mid-level northwesterlies, and therefore weakened mid-level dry advection.

Evaluating the climate and air quality impacts of short-lived pollutants

This paper presents a summary of the work done within the European Union's Seventh Framework Programme project ECLIPSE (Evaluating the Climate and Air Quality Impacts of Short-Lived Pollutants). ECLIPSE had a unique systematic concept for designing a realistic and effective mitigation scenario for short-lived climate pollutants (SLCPs; methane, aerosols and ozone, and their precursor species) and quantifying its climate and air quality impacts, and this paper presents the results in the context of this overarching strategy. The first step in ECLIPSE was to create a new emission inventory based on current legislation (CLE) for the recent past and until 2050. Substantial progress compared to previous work was made by including previously unaccounted types of sources such as flaring of gas associated with oil production, and wick lamps. These emission data were used for present-day reference simulations with four advanced Earth system models (ESMs) and six chemistry transport models (CTMs). The model simulations were compared with a variety of ground-based and satellite observational data sets from Asia, Europe and the Arctic. It was found that the models still underestimate the measured seasonality of aerosols in the Arctic but to a lesser extent than in previous studies. Problems likely related to the emissions were identified for northern Russia and India, in particular. To estimate the climate impacts of SLCPs, ECLIPSE followed two paths of research: the first path calculated radiative forcing (RF) values for a large matrix of SLCP species emissions, for different seasons and regions independently. Based on these RF calculations, the Global Temperature change Potential metric for a time horizon of 20 years (GTP20) was calculated for each SLCP emission type. This climate metric was then used in an integrated assessment model to identify all emission mitigation measures with a beneficial air quality and short-term (20-year) climate impact. These measures together defined a SLCP mitigation (MIT) scenario. Compared to CLE, the MIT scenario would reduce global methane (CH4) and black carbon (BC) emissions by about 50 and 80 %, respectively. For CH4, measures on shale gas production, waste management and coal mines were most important. For non-CH4 SLCPs, elimination of high-emitting vehicles and wick lamps, as well as reducing emissions from gas flaring, coal and biomass stoves, agricultural waste, solvents and diesel engines were most important. These measures lead to large reductions in calculated surface concentrations of ozone and particulate matter. We estimate that in the EU, the loss of statistical life expectancy due to air pollution was 7.5 months in 2010, which will be reduced to 5.2 months by 2030 in the CLE scenario. The MIT scenario would reduce this value by another 0.9 to 4.3 months. Substantially larger reductions due to the mitigation are found for China (1.8 months) and India (11–12 months). The climate metrics cannot fully quantify the climate response. Therefore, a second research path was taken. Transient climate ensemble simulations with the four ESMs were run for the CLE and MIT scenarios, to determine the climate impacts of the mitigation. In these simulations, the CLE scenario resulted in a surface temperature increase of 0.70 ± 0.14 K between the years 2006 and 2050. For the decade 2041–2050, the warming was reduced by 0.22 ± 0.07 K in the MIT scenario, and this result was in almost exact agreement with the response calculated based on the emission metrics (reduced warming of 0.22 ± 0.09 K). The metrics calculations suggest that non-CH4 SLCPs contribute ~ 22 % to this response and CH4 78 %. This could not be fully confirmed by the transient simulations, which attributed about 90 % of the temperature response to CH4 reductions. Attribution of the observed temperature response to non-CH4 SLCP emission reductions and BC specifically is hampered in the transient simulations by small forcing and co-emitted species of the emission basket chosen. Nevertheless, an important conclusion is that our mitigation basket as a whole would lead to clear benefits for both air quality and climate. The climate response from BC reductions in our study is smaller than reported previously, possibly because our study is one of the first to use fully coupled climate models, where unforced variability and sea ice responses cause relatively strong temperature fluctuations that may counteract (and, thus, mask) the impacts of small emission reductions. The temperature responses to the mitigation were generally stronger over the continents than over the oceans, and with a warming reduction of 0.44 K (0.39–0.49) K the largest over the Arctic. Our calculations suggest particularly beneficial climate responses in southern Europe, where surface warming was reduced by about 0.3 K and precipitation rates were increased by about 15 (6–21) mm yr−1 (more than 4 % of total precipitation) from spring to autumn. Thus, the mitigation could help to alleviate expected future drought and water shortages in the Mediterranean area. We also report other important results of the ECLIPSE project.

Modelled and observed changes in aerosols and surface solar radiation over Europe between 1960 and 2009

Substantial changes in anthropogenic aerosols and precursor gas emissions have occurred over recent decades due to the implementation of air pollution control legislation and economic growth. The response of atmospheric aerosols to these changes and the impact on climate are poorly constrained, particularly in studies using detailed aerosol chemistry–climate models. Here we compare the HadGEM3-UKCA (Hadley Centre Global Environment Model-United Kingdom Chemistry and Aerosols) coupled chemistry–climate model for the period 1960–2009 against extensive ground-based observations of sulfate aerosol mass (1978–2009), total suspended particle matter (SPM, 1978–1998), PM10 (1997–2009), aerosol optical depth (AOD, 2000–2009), aerosol size distributions (2008–2009) and surface solar radiation (SSR, 1960–2009) over Europe. The model underestimates observed sulfate aerosol mass (normalised mean bias factor (NMBF) = −0.4), SPM (NMBF = −0.9), PM10 (NMBF = −0.2), aerosol number concentrations (N30 NMBF = −0.85; N50 NMBF = −0.65; and N100 NMBF = −0.96) and AOD (NMBF = −0.01) but slightly overpredicts SSR (NMBF = 0.02). Trends in aerosol over the observational period are well simulated by the model, with observed (simulated) changes in sulfate of −68 % (−78 %), SPM of −42 % (−20 %), PM10 of −9 % (−8 %) and AOD of −11 % (−14 %). Discrepancies in the magnitude of simulated aerosol mass do not affect the ability of the model to reproduce the observed SSR trends. The positive change in observed European SSR (5 %) during 1990–2009 ("brightening") is better reproduced by the model when aerosol radiative effects (ARE) are included (3 %), compared to simulations where ARE are excluded (0.2 %). The simulated top-of-the-atmosphere aerosol radiative forcing over Europe under all-sky conditions increased by > 3.0 W m−2 during the period 1970–2009 in response to changes in anthropogenic emissions and aerosol concentrations.

Global climatology of surface water temperatures of large lakes by remote sensing

Lake surface water temperatures (LSWTs) of 246 globally distributed large lakes were derived from Along-Track Scanning Radiometers (ATSR) for the period 1991–2011. The climatological cycles of mean LSWT derived from these data quantify on a global scale the responses of large lakes' surface temperatures to the annual cycle of forcing by solar radiation and the ambient meteorological conditions. LSWT cycles reflect the twice annual peak in net solar radiation for lakes between 1°S to 12°N. For lakes without a lake-mean seasonal ice cover, LSWT extremes exceed air temperatures by 0.5–1.7 °C for maximum and 0.7–1.9 °C for minimum temperature. The summer maximum LSWTs of lakes from 25°S to 35°N show a linear decrease with increasing altitude; −3.76 ± 0.17 °C km−1 (inline image = 0.95), marginally lower than the corresponding air temperature decrease with altitude −4.15 ± 0.24 °C km−1 (inline image = 0.95). Lake altitude of tropical lakes account for 0.78–0.83 (inline image) of the variation in the March to June LSWT–air temperature differences, with differences decreasing by 1.9 °C as the altitude increases from 500 to 1800 m above sea level (a.s.l.) We define an ‘open water phase’ as the length of time the lake-mean LSWT remains above 4 °C. There is a strong global correlation between the start and end of the lake-mean open water phase and the spring and fall 0 °C air temperature transition days, (inline image = 0.74 and 0.80, respectively), allowing for a good estimation of timing and length of the open water phase of lakes without LSWT observations. Lake depth, lake altitude and distance from coast further explain some of the inter-lake variation in the start and end of the open water phase.