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Observations at surface sites show an increase in global mean surface methane (CH4) of about 180 parts per billion (ppb) (above 10 %) over the period 1984-2012. Over this period there are large fluctuations in the annual growth rate. In this work, we investigate the atmospheric CH4 evolution over the period 1970-2012 with the Oslo CTM3 global Chemical Transport Model (CTM) in a bottom-up approach. We thoroughly assess data from surface measurement sites in international networks and select a subset suited for comparisons with the output from the CTM. We compare model results and observations to understand causes both for long-term trends and short-term variations. Employing the Oslo CTM3 model we are able to reproduce the seasonal and year to year variations and shifts between years with consecutive growth and stagnation, both at global and regional scales. The overall CH4 trend over the period is reproduced, but for some periods the model fails to reproduce the strength of the growth. The observed growth after 2006 is overestimated by the model in all regions. This seems to be explained by a too strong increase in anthropogenic emissions in Asia, having global impact. Our findings confirm other studies questioning the timing or strength of the emission changes in Asia in the EDGAR v4.2 emission inventory over the last decades. The evolution of CH4 is not only controlled by changes in sources, but also by changes in the chemical loss in the atmosphere and soil uptake. We model a large growth in atmospheric oxidation capacity over the period 1970-2012. In our simulations, the CH4 lifetime decreases by more than 8% from 1970 to 2012, a significant shortening of the residence time of this important greenhouse gas. This results in substantial growth in the chemical CH4 loss (relative to its burden) and dampens the CH4 growth. The change in atmospheric oxidation capacity is driven by complex interactions between a number of chemical components and meteorological factors. In our analysis, we are able to detach the key factors and provide simple prognostic equations for the relations between these and the atmospheric CH4 lifetime. [ABSTRACT FROM AUTHOR]

The ability of six global and one regional model to reproduce distributions of tropospheric ozone and its precursors, as well as aerosols over Asia in summer 2008 is evaluated using satellite and in-situ observations. Whilst ozone precursors (NO2 and CO) are generally underestimated by the models in the troposphere, surface NO2 concentrations are overestimated, suggesting that emissions of NOx are too high. Ozone integrated columns and vertical profiles are generally well modeled, but the global models face difficulties simulating the ozone gradient at the surface between urban and rural environments, pointing to the need to increase model resolution. The accuracy of simulated aerosol patterns over eastern China and northern India varies between the models, and although most of the models reproduce the observed pollution features over eastern China, significant biases are noted in the magnitude of optical properties (aerosol optical depth, aerosol backscatter). These results have important implications for accurate prediction of pollution episodes affecting air quality and the radiative effects of these short-lived climate pollutants over Asia. [ABSTRACT FROM AUTHOR]

Policies to control air quality focus on mitigating emissions of aerosols and their precursors, and other short-lived climate pollutants (SLCPs). On a local scale, these policies will have beneficial impacts on health and crop yields, by reducing particulate matter (PM) and surface ozone concentrations; however, the climate impacts of reducing emissions of SLCPs are less straightforward to predict. In this paper we consider a set of idealised, extreme mitigation strategies, in which the total anthropogenic emissions of individual SLCP emissions species are removed. This provides an upper bound on the potential climate impacts of such air quality strategies. We focus on evaluating the climate responses to changes in anthropogenic emissions of aerosol precursor species: black carbon (BC), organic carbon (OC) and sulphur dioxide (SO2).We perform climate integrations with four fully coupled atmosphereocean global climate models (AOGCMs), and examine the effects on global and regional climate of removing the total land-based anthropogenic emissions of each of the three aerosol precursor species. We find that the SO2 emissions reductions lead to the strongest response, with all three models showing an increase in surface temperature focussed in the northern hemisphere high latitudes, and a corresponding increase in global mean precipitation and run-off. Changes in precipitation and run-off patterns are driven mostly by a northward shift in the ITCZ, consistent with the hemispherically asymmetric warming pattern driven by the emissions changes. The BC and OC emissions reductions give a much weaker forcing signal, and there is some disagreement between models in the sign of the climate responses to these perturbations. These differences between models are due largely to natural variability in sea-ice extent, circulation patterns and cloud 25 changes. This large natural variability component to the signal when the ocean circulation and sea-ice are free-running means that the BC and OC mitigation measures do not necessarily lead to a discernible climate response. [ABSTRACT FROM AUTHOR]

Atmospheric black carbon (BC) absorbs solar radiation, and exacerbates global warming through exerting positive radiative forcing (RF). However, the contribution of BC to ongoing changes in global climate is under debate. Anthropogenic BC emissions, and the resulting distribution of BC concentration, are highly uncertain. In particular, long range transport and processes affecting BC atmospheric lifetime are poorly understood. Here we discuss whether recent assessments may have overestimated present day BC radiative forcing in remote regions. We compare vertical profiles of BC concentration from four recent aircraft measurement campaigns to simulations by 13 aerosol models participating in the AeroCom Phase II intercomparision. An atmospheric lifetime of BC of less than 5 days is shown to be essential for reproducing observations in remote ocean regions, in line with other recent studies. Adjusting model results to measurements in remote regions, and at high altitudes, leads to a 25% reduction in AeroCom Phase II median direct BC forcing, from fossil fuel and biofuel burning, over the industrial era. The sensitivity of modeled forcing to BC vertical profile and lifetime highlights an urgent need for further flight campaigns, close to sources and in remote regions, to provide improved quantification of BC effects for use in climate policy. [ABSTRACT FROM AUTHOR]

The Aerosol Direct Radiative Effect (ADRE) is defined as the change in the solar radiation flux, F, due to aerosol scattering and absorption. The difficulty in determining ADRE stems mainly from the need to estimate F without aerosols, F0, with either radiative transfer modelling and knowledge of the atmospheric state, or regression analysis of radiation data down to zero aerosol optical depth (AOD), if only F and AOD are observed. This paper examines the regression analysis method by using modeled surface data products provided by the AErosol RObotic NETwork (AERONET). We extrapolated F0 by two functions: a straight linear line and an exponential nonlinear decay. The exponential decay regression is expected to give a better estimation of ADRE with a few percents larger extrapolated F0 than the linear regression. We found that, contrary to the expectation, in most cases the linear regression gives better results than the nonlinear. In such cases the extrapolated F0 represents an unrealistically low WVC, resulting in underestimation of attenuation caused by the water vapour, and hence too large F0 and overestimation of the magnitude of ADRE. The nonlinear ADRE is generally 40-50% larger in magnitude than the linear ADRE due to the extrapolated F0 difference. Since for a majority of locations, AOD and water vapour column (WVC) have a positive correlation, the extrapolated F0 with the nonlinear regression fit represents an unrealistically low WVC, and hence too large F0. The systematic underestimation of F0 with the linear regression is compensated by the positive correlation between AOD and water vapour, providing the better result. [ABSTRACT FROM AUTHOR]

The diurnal variability of aerosol optical depth (AOD) can be significant, depending on location and dominant aerosol type. However, these diurnal cycles have rarely been taken into account in measurement-based estimates of aerosol direct radiative forcing (ADRF) or aerosol direct radiative effect (ADRE). The objective of our study was to estimate the influence of diurnal aerosol variability on the top of the atmosphere ADRE estimates. By including all the possible AERONET sites, we wanted to assess the influence on global ADRE estimates, while by focusing also in more detail on some selected sites of strongest impact, our goal was to also see the possible impact regionally. We calculated ADRE with different assumptions about the daily AOD variability: taking the observed daily AOD cycle into account and assuming diurnally constant AOD. Moreover, we estimated the corresponding differences in ADREs, if the single AOD value for the daily mean was taken from the the Moderate Resolution Imaging Spectroradiometer (MODIS) Terra or Aqua overpass times, instead of accounting for the true observed daily variability. The mean impact of diurnal AOD variability on 24 h ADRE estimates, averaged over all AERONET sites, was rather small and it was relatively small even for the cases when AOD was chosen to correspond to the Terra or Aqua overpass time. This was true on average over all AERONET sites, while clearly there can be much stronger impact in individual sites. Examples of some selected sites demonstrated that the strongest observed AOD variability (the strongest morning afternoon contrast) does not typically result in a significant impact on 24 h ADRE. In those cases, the morning and afternoon AOD patterns are opposite and thus the impact on 24 h ADRE, when integrated over all solar zenith angles, is reduced. The most significant effect on daily ADRE was induced by AOD cycles with either maximum or minimum AOD close to local noon. In these cases, the impact on 24 h ADRE was typically around 0.1-0.2W m-2 (both positive and negative). [ABSTRACT FROM AUTHOR]

In this study we examine the performance of 31 global model radiative transfer schemes in cloud-free conditions with prescribed gaseous absorbers and no aerosols (Rayleigh atmosphere), with prescribed scattering-only aerosols, and with more absorbing aerosols. Results are compared to benchmark results from high-resolution, multi-angular line-by-line radiation models. For purely scattering aerosols, model bias relative to the line-by-line models in the top-of-the atmosphere aerosol radiative forcing ranges from roughly -10 to 20%, with over- and underestimates of radiative cooling at higher and lower sun elevation, respectively. Inter-model diversity (relative standard deviation) increases from ~10 to 15 % as sun elevation increases. Inter-model diversity in atmospheric and surface forcing decreases with increased aerosol absorption, indicating that the treatment of multiple-scattering is more variable than aerosol absorption in the models considered. Aerosol radiative forcing results from multi-stream models are generally in better agreement with the line-by-line results than the simpler two-stream schemes. Considering radiative fluxes, model performance is generally the same or slightly better than results from previous radiation scheme intercomparisons. However, the inter-model diversity in aerosol radiative forcing remains large, primarily as a result of the treatment of multiple-scattering. Results indicate that global models that estimate aerosol radiative forcing with two-stream radiation schemes may be subject to persistent biases introduced by these schemes, particularly for regional aerosol forcing. [ABSTRACT FROM AUTHOR]

The impact of black carbon (BC) aerosols on the global radiation balance is not well constrained. Here twelve global aerosol models are used to show that at least 20% of the present uncertainty in modeled BC direct radiative forcing (RF) is due to diversity in the simulated vertical profile of BC mass. Results are from phases 1 and 2 of the global aerosol model intercomparison project (AeroCom). Additionally, a significant fraction of the variability is shown to come from high altitudes, as, globally, more than 40% of the total BC RF is exerted above 5 km. BC emission regions and areas with transported BC are found to have differing characteristics. These insights into the importance of the vertical profile of BC lead us to suggest that observational studies are needed to better characterize the global distribution of BC, including in the upper troposphere. [ABSTRACT FROM AUTHOR]

Shipping is a growing sector in the global economy and it contributions to global CO2 emissions are expected to increase. CO2 emissions from the world shipping fleet will likely be regulated in the near future, and studies have shown that significant emission reductions can be achieved at low cost. Regulations are being discussed for both existing ships, as well as for future additions to the fleet. In this study a plausible CO2 emission reduction inventory is constructed for the cargo fleet existing in 2010, as well as for container ships, bulk ships and tankers separately. In the reduction inventories CO2 emissions are reduced by 25-32% relative to baseline by a ship type specific cost-effectiveness criterion, and 9 other emission compounds are changed as a technical implication of reducing CO2. The overall climate and environmental effects of the changes to all 10 emission components in the reduction inventory are assessed using a chemical transport model, radiative forcing (RF) models and a simple climate model. We find substantial environmental and health benefits with up to 5% reduction in surface ozone levels, 15% reductions in surface sulfate and 10% reductions in wet deposition of sulfate in certain regions exposed to heavy ship traffic. The major ship types show distinctly different contributions in specific locations. For instance, the container fleet contributes 50% of the sulfate decline on the west coast of North America. The global radiative forcing from a 1-yr emission equal to the difference between baseline and reduction inventory, show an initial strong positive forcing from non-CO2 compounds. This warming effect is due to reduced cooling by aerosols and methane. After approximately 25 yr, the non-CO2 forcing is balanced by the CO2 forcing. For the global mean temperature change we find a shift from warming to cooling after approximately 60 yr. The major ship types show significant differences in the short term radiative forcing; for instance the direct SO4 forcing from tankers is 30% higher than for container and bulk. The net long term effects on RF are similar due to similar CO2 forcing. We assess an emission scenario where the reduction inventory is sustained on the fleet as it steadily diminishes over time due to scrapping and disappears in 2040. We find a net temperature increase lasting until approximately 2080. We conclude that changes in non-CO2 emission does matter significantly if reductions of CO2 emissions are made on the year 2010 cargo shipping fleet. In sum, we find that emission changes motivated by CO2 reductions in shipping will be beneficial from a long-term climate perspective, and there are also positive environmental and health effects identified as concentrations of key short-lived pollutants are reduced. [ABSTRACT FROM AUTHOR]

We quantify the concentrations change of atmospheric pollutants and Radiative Forcing (RF) of short-lived components due to shipping emissions of NOx, SOx, CO, NMVOCs, BC and OC. A set of models is used to evaluate the period 2004-2030. This time period reflects expected increasing traffic in the Arctic region. Two datasets for ship emissions are used that may characterize the potential impact from shipping and the degree to which shipping controls may mitigate impacts: A high (HIGH) scenario and a low scenario with Maximum Feasible Reduction (MFR) of black carbon in the Arctic. In MFR, BC emissions in the Arctic are reduced with 70% representing a combination technology performance and/or reasonable advances in single-technology performance. Both scenarios result in moderate to substantial increases in concentrations of pollutants both globally and in the Arctic. Exceptions are black carbon in the MFR scenario, and sulfur species and organic carbon in both scenarios due to the future phase-in of current regulation that reduces fuel sulfur content. In the season with potential transit traffic through the Arctic in 2030 significant increases occur for all pollutants in large parts of the Arctic. Net global RFs from 2004-2030 of 53mWm-2 (HIGH) and 73mWm-2 (MFR) are similar to those found for preindustrial to present net global aircraft RF. The found warming contrasts the cooling from historical ship emissions. The reason for this difference and the higher global forcing for the MFR scenario is mainly the reduced future fuel sulfur content resulting in less cooling from sulfate aerosols. Arctic regional forcing is largest in the HIGH scenario because other components become locally more important in polar latitudes. In the HIGH scenario ozone dominates the RF during Arctic summer and the transit season. RF due to BC in air, and snow and ice becomes of significance in Arctic spring. For the HIGH scenario the net Arctic RF during spring is 5 times higher than in winter. [ABSTRACT FROM AUTHOR]

Ozone (O3) from 17 atmospheric chemistry models taking part in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) has been used to calculate tropospheric ozone radiative forcings (RFs). We calculate a value for the pre-industrial (1750) to present-day (2010) tropospheric ozone RF of 0.40Wm-2. The model range of pre-industrial to present-day changes in O3 produces a spread (±1 standard deviation) in RFs of ±17%. Three different radiation schemes were used -- we find differences in RFs between schemes (for the same ozone fields) of ±10%. Applying two different tropopause definitions gives differences in RFs of ±3%. Given additional (unquantified) uncertainties associated with emissions, climate-chemistry interactions and land-use change, we estimate an overall uncertainty of ±30% for the tropospheric ozone RF. Experiments carried out by a subset of six models attribute tropospheric ozone RF to increased emissions of methane (47%), nitrogen oxides (29%), carbon monoxide (15%) and non-methane volatile organic compounds (9%); earlier studies attributed more of the tropospheric ozone RF to methane and less to nitrogen oxides. Normalising RFs to changes in tropospheric column ozone, we find a global mean normalised RF of 0.042Wm-2 DU-1 , a value similar to previous work. Using normalised RFs and future tropospheric column ozone projections we calculate future tropospheric ozone RFs (Wm-2 ; relative to 1850 -- add 0.04Wm-2 to make relative to 1750) for the Representative Concentration Pathways in 2030 (2100) of: RCP2.6: 0.31 (0.16); RCP4.5: 0.38 (0.26); RCP6.0: 0.33 (0.24); and RCP8.5: 0.42 (0.56). Models show some coherent responses of ozone to climate change: decreases in the tropical lower troposphere, associated with increases in water vapour; and increases in the sub-tropical to mid-latitude upper troposphere, associated with increases in lightning and stratosphere-to-troposphere transport. [ABSTRACT FROM AUTHOR]

Simulated multi-model "diversity" in aerosol direct radiative forcing estimates is often perceived as measure of aerosol uncertainty. However, current models used for aerosol radiative forcing calculations vary considerably in model components relevant for forcing calculations and the associated "host-model uncertainties" are generally convoluted with the actual aerosol uncertainty. In this AeroCom Prescribed intercomparison study we systematically isolate and quantify host model uncertainties on aerosol forcing experiments through prescription of identical aerosol radiative properties in nine participating models. Even with prescribed aerosol radiative properties, simulated clear-sky and all-sky aerosol radiative forcings show significant diversity. For a purely scattering case with globally constant optical depth of 0.2, the global-mean all-sky top-of-atmosphere radiative forcing is -4.51Wm-2 and the inter-model standard deviation is 0.70Wm-2, corresponding to a relative standard deviation of 15 %. For a case with partially absorbing aerosol with an aerosol optical depth of 0.2 and single scattering albedo of 0.8, the forcing changes to 1.26Wm-2, and the standard deviation increases to 1.21W-2, corresponding to a significant relative standard deviation of 96 %. However, the top-ofatmosphere forcing variability owing to absorption is low, with relative standard deviations of 9% clear-sky and 12% all-sky. Scaling the forcing standard deviation for a purely scattering case to match the sulfate radiative forcing in the AeroCom Direct Effect experiment, demonstrates that host model uncertainties could explain about half of the overall sulfate forcing diversity of 0.13Wm-2 in the AeroCom Direct Radiative Effect experiment. Host model errors in aerosol radiative forcing are largest in regions of uncertain host model components, such as stratocumulus cloud decks or areas with poorly constrained surface albedos, such as sea ice. Our results demonstrate that host model uncertainties are an important component of aerosol forcing uncertainty that require further attention. [ABSTRACT FROM AUTHOR]

We use simultaneous observations of ozone and outgoing longwave radiation (OLR) from the Tropospheric Emission Spectrometer (TES) to evaluate ozone distributions and radiative forcing simulated by a suite of chemistry-climate models that participated in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The ensemble mean of ACCMIP models show a persistent but modest tropospheric ozone low bias (5-20 ppb) in the Southern Hemisphere (SH) and modest high bias (5-10 ppb) in the Northern Hemisphere (NH) relative to TES for 2005-2010. These biases lead to substantial differences in ozone instantaneous radiative forcing between TES and the ACCMIP simulations. Using TES instantaneous radiative kernels (IRK), we show that the ACCMIP ensemble mean has a low bias in the SH tropics of up to 100mWm-2 locally and a global low bias of 35±44mWm-2 relative to TES. Combining ACCMIP preindustrial ozone and the TES present-day ozone, we calculate an observationally constrained estimate of tropospheric ozone radiative forcing (RF) of 399±70mWm-2, which is about 7% higher than using the ACCMIP models alone but with the same standard deviation (Stevenson et al., 2012). In addition, we explore an alternate approach to constraining radiative forcing estimates by choosing a subset of models that best match TES ozone, which leads to an ozone RF of 369±42mWm-2. This estimate is closer to the ACCMIP ensemble mean RF but about a 40% reduction in standard deviation. These results point towards a profitable direction of combining observations and chemistry-climate model simulations to reduce uncertainty in ozone radiative forcing. [ABSTRACT FROM AUTHOR]

We report on the AeroCom Phase II direct aerosol effect (DAE) experiment where 15 detailed global aerosol models have been used to simulate the changes in the aerosol distribution over the industrial era. All 15 models have estimated the radiative forcing (RF) of the anthropogenic DAE, and have taken into account anthropogenic sulphate, black carbon (BC) and organic aerosols (OA) from fossil fuel, biofuel, and biomass burning emissions. In addition several models have simulated the DAE of anthropogenic nitrate and anthropogenic influenced secondary organic aerosols (SOA). The model simulated all-sky RF of the DAE from total anthropogenic aerosols has a range from -0.58 to -0.02W m-2, with a mean of -0.30W m-2 for the 15 models. Several models did not include nitrate or SOA and modifying the estimate by accounting for this with information from the other AeroCom models reduces the range and slightly strengthens the mean. Modifying the model estimates for missing aerosol components and for the time period 1750 to 2010 results in a mean RF for the DAE of -0.39W m-2. Compared to AeroCom Phase I (Schulz et al., 2006) we find very similar spreads in both total DAE and aerosol component RF. However, the RF of the total DAE is stronger negative and RF from BC from fossil fuel and biofuel emissions are stronger positive in the present study than in the previous AeroCom study. We find a tendency for models having a strong (positive) BC RF to also have strong (negative) sulphate or OA RF. This relationship leads to smaller uncertainty in the total RF of the DAE compared to the RF of the sum of the individual aerosol components. The spread in results for the individual aerosol components is substantial, and can be divided into diversities in burden, mass extinction coefficient (MEC), and normalized RF with respect to AOD. We find that these three factors give similar contributions to the spread in results. [ABSTRACT FROM AUTHOR]

As part of the Atmospheric Chemistry and Climate Model Intercomparison Project (AC-CMIP), we evaluate the historical black carbon (BC) aerosols simulated by 8 ACCMIP models against observations including 12 ice core records, long-term surface mass concentrations and recent Arctic BC snowpack measurements. We also estimate BC albedo forcing by performing additional simulations using offline models with prescribed meteorology from 1996-2000. We evaluated the vertical profile of BC snow concentrations from these offline simulations using the recent BC snowpack measurements. Despite using the same BC emissions, the global BC burden differs by approximately a factor of 3 among models due to differences in aerosol removal parameterizations and simulated meteorology: 34 Gg to 103 Gg in 1850 and 82 Gg to 315 Gg in 2000. However, the global BC burden from preindustrial to present-day increases by 2.5-3 times with little variation among models, roughly matching the 2.5-fold increase in total BC emissions during the same period. We find a large divergence among models at both Northern Hemisphere (NH) and Southern Hemisphere (SH) high latitude regions for BC burden and at SH high latitude regions for deposition fluxes. The ACCMIP simulations match the observed BC surface mass concentrations well in Europe and North America except at Jungfraujoch and Ispra. However, the models fail to predict the Arctic BC seasonality due to severe underestimations during winter and spring. The simulated vertically resolved BC snow concentrations are, on average, within a factor of 2-3 of the BC snowpack measurements except for Greenland and the Arctic Ocean. For the ice core evaluation, models tend to capture both the observed temporal trends and the magnitudes well at Greenland sites. However, models fail to predict the decreasing trend of BC depositions/ice-core concentrations from the 1950s to the 1970s in most Tibetan Plateau ice cores. The distinct temporal trend at the Tibetan Plateau ice cores indicates a strong influence from Western Europe, but the modeled BC increases in that period are consistent with the emission changes in Eastern Europe, the Middle East, South and East Asia. At the Alps site, the simulated BC suggests a strong influence from Europe, which agrees with the Alps ice core observations. Models successfully simulate higher BC concentrations observed at Zuoqiupu during the non-monsoon season than monsoon season, but models underpredict BC in both seasons. Despite a large divergence in BC deposition at two Antarctic ice core sites, models are able to capture the relative increase from preindustrial to present-day seen in the ice cores. In 2000 relative to 1850, globally annually averaged BC surface albedo forcing from the offline simulations ranges from 0.014 to 0.019 W m-2 among the ACCMIP models. Comparing offline and online BC albedo forcings computed by some of the same models, we find that the global annual mean can vary by up to a factor of two because of different aerosol models or different BC-snow parameterizations and snow cover. The spatial distributions of the offline BC albedo forcing in 2000 show especially high BC forcing (i.e. over 0.1 W m-2) over Manchuria, Karakoram, and most of the Former USSR. Models predict the highest global annual mean BC forcing in 1980 rather than 2000, mostly driven by the high fossil fuel and biofuel emissions in the Former USSR in 1980. [ABSTRACT FROM AUTHOR]

A primary goal of the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) was to characterize the short-lived drivers of preindustrial to 2100 climate change in the current generation of climate models. Here we evaluate historical and future radiative forcing in the 10 ACCMIP models that included aerosols, 8 of which also participated in the Coupled Model Intercomparison Project phase 5 (CMIP5). The models generally reproduce present-day climatological total aerosol optical depth (AOD) relatively well. They have quite different contributions from various aerosol components to this total, however, and most appear to underestimate AOD over East Asia. The models generally capture 1980-2000 AOD trends fairly well, though they underpredict AOD increases over the Yellow/Eastern Sea. They appear to strongly underestimate absorbing AOD, especially in East Asia, South and Southeast Asia, South America and Southern Hemisphere Africa. We examined both the conventional direct radiative forcing at the tropopause (RF) and the forcing including rapid adjustments (adjusted forcing; AF, including direct and indirect effects). The models' calculated all aerosol all-sky 1850 to 2000 global mean annual average RF ranges from -0.06 to -0.49W m-2, with a mean of -0.26W m-2 and a median of -0.27W m-2. Adjusting for missing aerosol components in some models brings the range to -0.12 to -0.62W m-2, with a mean of -0.39W m-2. Screening the models based on their ability to capture spatial patterns and magnitudes of AOD and AOD trends yields a quality-controlled mean of -0.42W m-2 and range of -0.33 to -0.50W m-2 (accounting for missing components). The CMIP5 subset of AC-CMIP models spans -0.06 to -0.49W m-2, suggesting some CMIP5 simulations likely have too little aerosol RF. A substantial, but not well quantified, contribution to historical aerosol RF may come from climate feedbacks (35 to -58%). The mean aerosol AF during this period is -1.12W m-2 (median value -1.16W m-2, range -0.72 to -1.44W m-2), indicating that adjustments to aerosols, which include cloud, water vapor and temperature, lead to stronger forcing than the aerosol direct RF. Both negative aerosol RF and AF are greatest over and near Europe, South and East Asia and North America during 1850 to 2000. AF, however, is positive over both polar regions, the Sahara, and the Karakoram. Annual average AF is stronger than 0.5W m-2 over parts of the Arctic and more than 1.5W m-2 during boreal summer. Examination of the regional pattern of RF and AF shows that the multi-model spread relative to the mean of AF is typically the same or smaller than that for RF over areas with substantial forcing. Historical aerosol RF peaks in nearly all models around 1980, declining thereafter. Aerosol RF declines greatly in most models over the 21st century and is only weakly sensitive to the particular Representative Concentration Pathway (RCP). One model, however, shows approximate stabilization at current RF levels under RCP 8.5, while two others show increasingly negative RF due to the influence of nitrate aerosols (which are not included in most models). Aerosol AF, in contrast, continues to become more negative during 1980 to 2000 despite the turnaround in RF. Total anthropogenic composition forcing (RF due to well-mixed greenhouse gases (WMGHGs) and ozone plus aerosol AF) shows substantial masking of greenhouse forcing by aerosols towards the end of the 20th century and in the early 21st century at the global scale. Regionally, net forcing is negative over most industrialized and biomass burning regions through 1980, but remains strongly negative only over East and Southeast Asia by 2000 and only over a very small part of Southeast Asia by 2030 (under RCP8.5). Net forcing is strongly positive by 1980 over the Sahara, Arabian peninsula, the Arctic, Southern Hemisphere South America, Australia and most of the oceans. Both the magnitude of and area covered by positive forcing expand steadily thereafter. There is no clear relationship between aerosol AF and climate sensitivity in the CMIP5 subset of ACCMIP models. There is a clear link between the strength of aerosol+ozone forcing and the global mean historical climate response to anthropogenic non-WMGHG forcing (ANWF). The models show ~20-35% greater climate sensitivity to ANWF than to WMGHG forcing, at least in part due to geographic differences in climate sensitivity. These lead to ~50% more warming in the Northern Hemisphere in response to increasing WMGHGs. This interhemispheric asymmetry is enhanced for ANWF by an additional 10-30%. At smaller spatial scales, response to ANWF and WMGHGs show distinct differences. [ABSTRACT FROM AUTHOR]

Accurate prediction of future methane abundances following a climate scenario requires understanding the lifetime changes driven by anthropogenic emissions, meteorological factors, and chemistry-climate feedbacks. Uncertainty in any of these influences or the underlying processes implies uncertainty in future abundance and radiative forcing. We simulate methane lifetime in multiple models over the period 1997-2009, adding sensitivity tests to determine key variables that drive the year- to-year variability. Across three atmospheric chemistry and transport models -- UCI CTM, GEOS-Chem, and Oslo CTM3 -- we find that temperature, water vapor, ozone column, biomass burning and lightning NOx are the dominant sources of interannual changes in methane lifetime. We also evaluate the model responses to forcings that have impacts on decadal time scales, such as methane feedback, and anthropogenic NOx emissions. In general, these different CTMs show similar sensitivities to the driving variables. We construct a parametric model that reproduces most of the interannual variability of each CTM and use it to predict methane lifetime from 1980 through 2100 following a specified emissions and climate scenario (RCP 8.5). The parametric model propagates uncertainties through all steps and provides a foundation for predicting methane abundances in any climate scenario. Our sensitivity tests also enable a new estimate of the methane global warming potential (GWP), accounting for stratospheric ozone effects, including those mediated by water vapor. We estimate the 100-yr GWP to be 32. [ABSTRACT FROM AUTHOR]

The future impact of traffic emissions on atmospheric ozone and OH has been investigated separately for the three sectors AIRcraft, maritime SHIPping and ROAD traffic. To reduce uncertainties we present results from an ensemble of six different atmospheric chemistry models, each simulating the atmospheric chemical composition in a possible high emission scenario (A1B), and with emissions from each transport sector reduced by 5% to estimate sensitivities. Our results are compared with optimistic future emission scenarios (B1 and B1 ACARE), presented in a companion paper, and with the recent past (year 2000). Present-day activity indicates that anthropogenic emissions so far evolve closer to A1B than the B1 scenario. As a response to expected changes in emissions, AIR and SHIP will have increased impacts on atmospheric O3 and OH in the future while the impact of ROAD traffic will decrease substantially as a result of technological improvements. In 2050, maximum aircraft-induced O3 occurs near 80° N in the UTLS region and could reach 9 ppbv in the zonal mean during summer. Emissions from ship traffic have their largest O3 impact in the maritime boundary layer with a maximum of 6 ppbv over the North Atlantic Ocean during summer in 2050. The O3 impact of road traffic emissions in the lower troposphere peaks at 3 ppbv over the Arabian Peninsula, much lower than the impact in 2000. Radiative Forcing (RF) calculations show that the net effect of AIR, SHIP and ROAD combined will change from a marginal cooling of -0.38±13 mW m-2 in 2000 to a relatively strong cooling of -32±8.9 (B1) or -31±20 mW m-2 (A1B) in 2050, when taking into account RF due to changes in O3, CH4 and CH4-induced O3. This is caused both by the enhanced negative net RF from SHIP, which will change from -20±5.4 mW m-2 in 2000 to -31±4.8 (B1) or -40±11 mW m-2 (A1B) in 2050, and from reduced O3 warming from ROAD, which is likely to turn from a positive net RF of 13±7.9mWm-2 in 2000 to a slightly negative net RF of -2.9±1.7 (B1) or -3.3±3.8 (A1B) mW m-2 in the middle of this century. The negative net RF from ROAD is temporary and induced by the strong decline in ROAD emissions prior to 2050, which only affects the methane cooling term due to the longer lifetime of CH4 compared to O3. The O3 RF from AIR in 2050 is strongly dependent on scenario and ranges from 19±6.8 (B1 ACARE) to 62±13.6 mW m-2 (A1B). There is also a considerable span in the net RF from AIR in 2050, ranging from -0.54±4.6 (B1 ACARE) to 12±11 (A1B) mW m-2 compared to 6.5±2.1 mW m-2 in 2000. [ABSTRACT FROM AUTHOR]

In order to use knowledge of past climate change to improve our understanding of the sensitivity of the climate system, detailed knowledge about the time development of radiative forcing (RF) of the earth atmosphere system is crucial. In this study, time series of anthropogenic forcing of climate from pre-industrial times until 2010, for all well established forcing agents, are estimated. This includes presentation of RF histories of well mixed greenhouse gases, tropospheric ozone, direct- and indirect aerosol effects, surface albedo changes, stratospheric ozone and stratospheric water vapour. For long lived greenhouse gases, standard methods are used for calculating RF, based on global mean concentration changes. For short lived climate forcers, detailed chemical transport modelling and radiative transfer modelling using historical emission inventories is performed. For the direct aerosol effect, sulphate, black carbon, organic carbon, nitrate and secondary organic aerosols are considered. For aerosol indirect effects, time series of both the cloud lifetime effect and the cloud albedo effect are presented. Radiative forcing time series due to surface albedo changes are calculated based on prescribed changes in land use and radiative transfer modelling. For the stratospheric components, simple scaling methods are used. Long lived greenhouse gases (LLGHGs) are the most important radiative forcing agent with a RF of 2.83±0.28Wm-2 in year 2010 relative to 1750. The two main aerosol components contributing to the direct aerosol effect are black carbon and sulphate, but their contributions are of opposite sign. The total direct aerosol effect was -0.48±0.14Wm-2 in year 2010. Since preindustrial times the RF of LLGHGs has been offset by the direct and indirect aerosol effects, especially in the second half of the 20th century, which possibly lead to a decrease in the total anthropogenic RF in the middle of the century. We find a total anthropogenic RF in year 2010 of 1.4Wm-2. However, the uncertainties in the negative RF from aerosols are large, especially for the cloud lifetime effect. [ABSTRACT FROM AUTHOR]

Atmospheric concentration changes and the resulting radiative forcing (RF) due to emissions from shipping and petroleum activity in the Arctic have been studied, using three-dimensional chemistry transport (OsloCTM2) and radiative transfer models. The present work focuses on short-lived climate forcers, based on a coherent dataset of present day emissions from petroleum and shipping activities in the Arctic region. We find that the net forcing effect of Arctic shipping emissions of short-lived climate forcers (SLCFs) is negative, while the net effect from Arctic petroleum emissions of SLCFs is positive. The negative RF from Arctic shipping arises mainly from direct aerosol -- and first indirect effects of sulphate. Positive RF from Arctic petroleum is mainly due to black carbon in air and deposited on snow and ice. Normalized forcing (RF per change in atmospheric burden) and global warming potentials (GWP) suggest that Arctic conditions (high solar angle, high surface albedo, summer season with midnight sun and polar night during winter) lead to different sensitivity to emissions here compared to lower latitudes. [ABSTRACT FROM AUTHOR]

The impact of future emissions from aviation and shipping on the atmospheric chemical composition has been estimated using an ensemble of six different atmospheric chemistry models. This study considers an optimistic emission scenario (B1) taking into account e.g. rapid introduction of clean and resource-efficient technologies, and a mitigation option for the aircraft sector (B1 ACARE), assuming further technological improvements. Results from sensitivity simulations, where emissions from each of the transport sectors were reduced by 5 %, show that emissions from both aircraft and shipping will have a larger impact on atmospheric ozone and OH in near future (2025; B1) and for longer time horizons (2050; B1) compared to recent time (2000). However, the ozone and OH impact from aircraft can be reduced substantially in 2050 if the technological improvements considered in the B1 ACARE will be achieved. Shipping emissions have the largest impact in the marine boundary layer and their ozone contribution may exceed 4 ppb (scaled to 100 %) over the North Atlantic Ocean in the future (2050; B1) during northern summer (July). In the zonal mean, ship-induced ozone relative to the background levels may exceed 12% near the surface. Corresponding numbers for OH are 6.0 x 105 molecules cm-3 and 30 %, respectively. This large impact on OH from shipping leads to a relative methane lifetime reduction of 3.92(±0.48)% on the global average in 2050 B1 (ensemble mean CH4 lifetime is 8.0(±1.0) yr), compared to 3.68(±0.47)% in 2000. Aircraft emissions have about 4 times higher ozone enhancement efficiency (ozone molecules enhanced relative to NOx molecules emitted) than shipping emissions, and the maximum impact is found in the UTLS region. Zonal mean aircraft-induced ozone could reach up to 5 ppb at northern mid- and high latitudes during future summer (July 2050; B1), while the relative impact peaks during northern winter (January) with a contribution of 4.2 %. Although the aviation-induced impact on OH is lower than for shipping, it still causes a reduction in the relative methane lifetime of 1.68(±0.38)% in 2050 B1. However, for B1 ACARE the perturbation is reduced to 1.17(±0.28) %, which is lower than the year 2000 estimate of 1.30(±0.30) %. [ABSTRACT FROM AUTHOR]

Recent laboratory measurements have shown the existence of a HNO3 forming branch of the HO2 + NO reaction. This reaction is the main source of atmospheric O3, through the subsequent photolysis of NO2, as well as being a major source of OH. The branching of the reaction to HNO3 reduces the formation of these species significantly, affecting O3 abundances, climate and the oxidation capacity of the troposphere. The Oslo CTM2, a three-dimensional chemistry transport model, is used to calculate atmospheric composition and trends with and without the new reaction branch. Results for the present day atmosphere, when both temperature and pressure effects on the branching ratio are accounted for, show an increase of the global, annual mean methane lifetime by 10.9 %, resulting from a 14.1% reduction in the global, annual mean OH concentration. Comparisons with measurements show that including the new branch improves the modelled O3, but that it is not possible to conclude whether the NOy distribution improves. We model an approximately 11% reduction in the tropical tropospheric O3 increase since pre-industrial times, as well as an 8% decrease in the trend of OH concentration, when the new branch is accounted for. The radiative forcing due to changes in O3 over the industrial era was calculated as 0.33 W m-2, reducing to 0.26 W m-2 with the new reaction branch. These results are significant, and it is important that this reaction branching is confirmed by other laboratory groups. [ABSTRACT FROM AUTHOR]

The distribution of black carbon (BC) in the atmosphere and the deposition of BC on snow surfaces since pre-industrial time until present are modelled with the Oslo CTM2 model. The model results are compared with observations including recent measurements of BC in snow in the Arctic. The global mean burden of BC from fossil fuel and biofuel sources increased during two periods. The first period, until 1920, is related to increases in emissions in North America and Europe, and the last period after 1970 are related mainly to increasing emissions in East Asia. Although the global burden of BC from fossil fuel and biofuel increases, in the Arctic the maximum atmospheric BC burden as well as in the snow was reached in 1960s, with a slight reduction thereafter. The global mean burden of BC from open biomass burning sources has not changed significantly since 1900. With current inventories of emissions from open biomass sources, the modelled burden of BC in snow and in the atmosphere north of 65° N is small compared to the BC burden of fossil fuel and biofuel origin. From the concentration changes radiative forcing time series due to the direct aerosol effect as well as the snow-albedo effect is calculated for BC from fossil fuel and biofuel. The calculated radiative forcing in 2000 for the direct aerosol effect is 0.35 Wm-2 and for the snow-albedo effect 0.016 W m~2. Due to a southward shift in the emissions there is an increase in the lifetime of BC as well as an increase in normalized radiative forcing, giving a change in forcing per unit of emissions of 26% since 1950. [ABSTRACT FROM AUTHOR]

Black carbon, light-absorbing organic carbon (often called "brown carbon") and mineral dust are the major light-absorbing aerosols. Currently the sources and formation of brown carbon aerosol in particular are not well understood. In this study we estimated globally the amount of light-absorbing organic carbon and black carbon from AERONET measurements. We find that the columnar absorbing organic carbon (brown carbon) levels in biomass burning regions of South-America and Africa are relatively high (about 15-20 mg/m² during biomass burning season), while the concentrations are significantly lower in urban areas in US and Europe. However, we estimated significant absorbing organic carbon amounts from the data of megacities of newly industrialized countries, particularly in India and China, showing also clear seasonality with peak values up to 30-35 mg/m² during the coldest season, likely caused by the coal and biofuel burning used for heating. We also compared our retrievals with the modeled organic carbon by global Oslo CTM for several sites. Model values are higher in biomass burning regions than AERONET-based retrievals, while opposite is true in urban areas in India and China. [ABSTRACT FROM AUTHOR]

Aerosols and their precursors are emitted abundantly by transport activities. Transportation constitutes one of the fastest growing activities and its growth is predicted to increase significantly in the future. Previous studies have estimated the aerosol direct radiative 5 forcing from one transport sub-sector, but only one study to our knowledge estimated the range of radiative forcing from the main aerosol components (sulphate, black carbon (BC) and organic carbon) for the whole transportation sector. In this study, we compare results from two different chemical transport models and three radiation codes under different hypothesis of mixing: internal and external mixing using 10 emission inventories for the year 2000. The main results from this study is a positive direct radiative forcing for aerosols emitted by road traffic of +20±11mWm-2 for an externally mixed aerosol, and of +32±13mWm-2 when BC is internally mixed . These direct radiative forcings are much higher than the previously published estimate of +3±11mWm-2. For transport activities from shipping, the net direct aerosol radia15 tive forcing is negative. This forcing is dominated by the contribution of the sulphate. For both an external and an internal mixture, the radiative forcing from shipping is estimated at -26±4mWm-2. These estimates are in very good agreement with the range of a previously published one (from -46 to -13mWm-2) but with a much narrower range. By contrast, the direct aerosol forcing from aviation is estimated to be small, 20 and in the range -0.9 to +0.3mWm-2. [ABSTRACT FROM AUTHOR]

Human activity influences a wide range of components that affect the surface UV radiation levels, among them ozone at high latitudes. We calculate the effect of humaninduced changes in the surface erythemally weighted ultra-violet radiation (UV-E) since 1750. We compare results from a radiative transfer model to surface UV-E radiation for year 2000 derived by satellite observations (from Total Ozone Mapping Spectroradiometer) and to ground based measurements at 14 sites. The model correlates well with the observations; the correlation coefficients are 0.97 and 0.98 for satellite and ground based measurements, respectively. In addition to the effect of changes in ozone, we also investigate the effect of changes in SO2, NO2, the direct and indirect effects of aerosols, albedo changes and aviation-induced contrails and cirrus. The results show an increase of surface UV-E in polar regions, most strongly in the Southern Hemisphere. Furthermore, our study also shows an extensive surface UV-E reduction over most land areas; a reduction up to 20% since 1750 is found in some industrialized regions. [ABSTRACT FROM AUTHOR]

The pre-industrial and present day distributions and burdens of Secondary Organic Aerosol (SOA) have been calculated using the off-line aerosol chemistry transport model Oslo CTM2. The production of SOA was found to have increased from about 43 Tg yr-1 to 69 Tg yr-1 since pre-industrial times, leading to an increase in the global annual mean SOA burden from 0.44 Tg to 0.70 Tg, or about 59%. The increases are greatest over industrialised areas, as well as over regions with high biogenic precursor emissions. The contribution of emissions from different sources to the larger SOA burdens has been calculated. The results suggest that the majority of the increase is caused by emissions of primary organic aerosols (POA), from fossil fuel and bio fuel combustion. When SOA partitioning to ammonium sulphate aerosol was not accounted for, the increase in SOA burden between pre-industrial times and the present was found to be lower (51%), with a production increase of 55%. As yet, very few radiative forcing estimates of SOA exist, and no such estimates were provided in the latest IPCC report. In this study, we find that the change in SOA burden caused a radiative forcing of -0.09Wm-2, when SOA was allowed to partition to both organic and sulphate aerosols, and -0.06Wm-2 when only partitioning to organic aerosols was assumed. Therefore, the radiative forcing of SOA is found to be substantially stronger than the best estimate for POA in the latest IPCC assessment. [ABSTRACT FROM AUTHOR]

The response of clouds to sudden decreases in the flux of galactic cosmic rays (Forbush decrease events) has been investigated using cloud products from the space-borne MODIS instrument, which has been in operation since 2000. By focusing on pristine Southern Hemisphere ocean regions we examine areas which are particularly susceptible to changes in cloud condensation nuclei (CCN) concentrations, and where a cosmic ray signal should be easier to detect than elsewhere. While previous studies on the subject have mainly considered cloud cover, the high spatial and spectral resolution of MODIS allows for a more thorough study of microphysical parameters such as cloud droplet size, cloud water content and cloud optical depth, in addition to cloud cover. Averaging the results from the 13 Forbush decrease events that were considered, no systematic correlation was found between any of the four cloud parameters and galactic cosmic radiation, with a seemingly random distribution of positive and negative correlations. When only the three Forbush decrease events with the largest amplitude are studied, the correlations fit the hypothesis better, with 8 out of 12 correlations having the expected sign. Splitting the area of study into several sub-regions, one sub-region in the Atlantic Ocean showed statistically significant correlations compatible with a cosmic ray-induced enhancement of CCN and cloud droplet number concentrations. However, the lack of correlation in any of the other 5 sub-regions suggests that this may be a statistical co-incidence. Introducing a time lag of a few days for clouds to respond to the cosmic ray signal did not change the overall results. Singling out low clouds of intermediate optical depth with large susceptibility did not lead to higher correlations. In conclusion, no response to variations in cosmic rays associated with Forbush decrease events was found in marine low clouds in remote regions using MODIS data. [ABSTRACT FROM AUTHOR]

A high-resolution global aerosol model (Oslo CTM2) driven by meteorological data and allowing a comparison with a variety of aerosol observations is used to simulate radiative forcing (RF) of the direct aerosol effect. The model simulates all main aerosol components, including several secondary components such as nitrate and secondary organic carbon. The model reproduces the main chemical composition and size features observed during large aerosol campaigns. Although the chemical composition compares best with ground-based measurement over land for modelled sulphate, no systematic differences are found for other compounds. The modelled aerosol optical depth (AOD) is compared to remote sensed data from AERONET ground and MODIS and MISR satellite retrievals. To gain confidence in the aerosol modelling, we have tested its ability to reproduce daily variability in the aerosol content, and this is performing well in many regions; however, we also identified some locations where model improvements are needed. The annual mean regional pattern of AOD from the aerosol model is broadly similar to the AERONET and the satellite retrievals (mostly within 10-20%). We notice a significant improvement from MODIS Collection 4 to Collection 5 compared to AERONET data. Satellite derived estimates of aerosol radiative effect over ocean for clear sky conditions differs significantly on regional scales (almost up to a factor two), but also in the global mean. The Oslo CTM2 has an aerosol radiative effect close to the mean of the satellite derived estimates. We derive a radiative forcing (RF) of the direct aerosol effect of -0.35Wm-2 in our base case. Implementation of a simple approach to consider internal black carbon (BC) mixture results in a total RF of -0.28Wm-2. Our results highlight the importance of carbonaceous particles, producing stronger individual RF than considered in the recent IPCC estimate; how ever, net RF is less different. A significant RF from secondary organic aerosols (SOA) is estimated (close to -0.1Wm-2). The SOA also contributes to a strong domination of secondary aerosol species for the aerosol composition over land. A combination of sensitivity simulations and model evaluation show that the RF is rather robust and unlikely to be much stronger than in our best estimate. [ABSTRACT FROM AUTHOR]

Three analyses of satellite observations and two sets of model studies are used to estimate changes in the stratospheric ozone distribution from solar minimum to solar maximum and are presented for three different latitudinal bands: Poleward of 30° north, between 30° north and 30° south and poleward of 30° south. In the model studies the solar cycle impact is limited to changes in UV fluxes. There is a general agreement between satellite observation and model studies, particular at middle and high northern latitudes. Ozone increases at solar maximum with peak values around 40 km. The profiles are used to calculate the radiative forcing (RF) from solar minimum to solar maximum. The ozone RF, calculated with two different radiative transfer schemes is found to be negligible (a magnitude of 0.01Wm-2 or less), compared to the direct RF due to changes in solar irradiance, since contributions from the longwave and shortwave nearly cancel each other. The largest uncertainties in the estimates come from the lower stratosphere, where there is significant disagreement between the different ozone profiles. [ABSTRACT FROM AUTHOR]

In spring 2006 a special meteorological situation occurred in the European Arctic region giving record high levels of air pollution. The synoptic situation resulted in extensive transport of pollution predominantly from agricultural fires in Eastern Europe into the Arctic region and record high air-pollution levels were measured at the Zeppelin observatory at Ny-Ålesund (78°54′ N, 11°53′ E) in the period from 25 April to 12 May. In the present study we investigate the optical properties of the aerosols from this extreme event and we estimate the radiative forcing of this episode. We examine the aerosol optical properties from the source region and into the European Arctic and explore the evolution of the episode and the changes in the optical properties. A number of sites in Eastern Europe, Northern Scandinavia and Svalbard are included in the study. In addition to AOD measurements, we explored lidar measurements from Minsk, ALOMAR (Arctic Lidar Observatory for Middle Atmosphere Research at Andenes) and Ny-Ålesund. For the AERONET sites included (Minsk, Toravere, Hornsund) we have further studied the evolution of the aerosol size. Importantly, at Svalbard it is consistency between the AERONET measurements and calculations of single scattering albedo based on aerosol chemical composition. We have found strong agreement between the satellite daily MODIS AOD and the ground-based AOD observations. This agreement is crucial for the radiative forcing calculations. We calculate a strong negative radiative forcing for the most polluted days employing the analysed ground based data, MODIS AOD and a multi-stream model for radiative transfer of solar radiation. [ABSTRACT FROM AUTHOR]

During the last twenty-five years European emission data have been compiled and reported under the Cooperative Programme for Monitoring and Evaluation of the Longrange Transmission of Air Pollutants in Europe (EMEP) as part of the work under the UNECE Convention on Long-range Transboundary Air Pollution (LRTAP). This paper presents emission trends of SO2 reported to EMEP and validated within the programme for the period 1980-2004. These European anthropogenic sulphur emissions have been steadily decreasing over the last twenty-five years, amounting from about 55 Tg SO2 in 1980 to 15 Tg SO2 in 2004. The uncertainty in sulphur emission estimates for individual countries and years are documented to range between 3% and 25%. The relative contribution of European emissions to global anthropogenic sulphur emissions has been halved during this period. Based on annual emission reports from European countries, three emission reduction regimes have been identified. The period 1980-1989 is characterized by low annual emission reductions (below 5% reduction per year and 20% for the whole period) and is dominated by emission reductions in Western Europe. The period 1990-1999 is characterised by high annual emission reductions (up to 11% reduction per year and 54% for the whole period), most pronounced in Central and Eastern Europe. The annual emission reductions in the period 2000-2004 are medium to low and reflect the unified Europe, with equally large reductions in both East and West. The sulphur emission reduction has been largest in the sector Combustion in energy and transformation industries, but substantial decreases are also seen in the Non-industrial combustion plants together with the sectors Industrial Combustion and Industrial Production Processes. The majority of European countries have reduced their emissions by more than 60% between 1990 and 2004, and one quarter have already achieved sulphur emission reductions higher than 80%. At European level, the 25 total sulphur target for 2010 set in the Gothenburg Protocol (16 Tg) has apparently already been met by 2004. However, still half of the Parties to the Gothenburg Protocol have to reduce further their sulphur emissions in order to attain their individual country total emission targets for 2010. It is also noteworthy that, contrasting the Gothenburg Protocol requirements, a growing number of countries have recently been reporting increasing sulphur emissions, while others report only minor further decreases. The emission trends presented here are supported by different studies of air concentrations and depositions carried out within and outside the framework of the LRTAP Convention. [ABSTRACT FROM AUTHOR]

Nine different global models with detailed aerosol modules have independently produced instantaneous direct radiative forcing due to anthropogenic aerosols. The anthropogenic impact is derived from the difference of two model simulations with identically prescribed aerosol emissions, one for present-day and one for pre-industrial conditions. The difference in the energy budget at the top of the atmosphere (ToA) yields a new harmonized estimate for the aerosol direct radiative forcing (RF) under all-sky conditions. On a global annual basis RF is -0.2Wm-2, with a standard deviation of ±0.2Wm-2. Anthropogenic nitrate and dust are not included in this estimate. No model shows a significant positive all-sky RF. The corresponding clear-sky RF is -0.6Wm-2. The cloud-sky RF was derived based on all-sky and clear-sky RF and modelled cloud cover. It was significantly different from zero and ranged between -0.16 and +0.34Wm-2. A sensitivity analysis shows that the total aerosol RF is influenced by considerable diversity in simulated residence times, mass extinction coefficients and most importantly forcing efficiencies (forcing per unit optical depth). Forcing efficiency differences among models explain most of the variability, mainly because all-sky forcing estimates require proper representation of cloud fields and the correct relative altitude placement between absorbing aerosol and clouds. The analysis of the sulphate RF shows that differences in sulphate residence times are compensated by opposite mass extinction coefficients. This is explained by more sulphate particle humidity growth and thus higher extinction in models with short-lived sulphate present at lower altitude and vice versa. Solar absorption within the atmospheric column is estimated at +0.85Wm-2. The local annual average maxima of atmospheric forcing exceed +5Wm-2 confirming the regional character of aerosol impacts on climate. The annual average surface forcing is -1.03Wm-2. [ABSTRACT FROM AUTHOR]

A thermo dynamical model for treatment of gas/aerosol partitioning of semi volatile inorganic aerosols has been implemented in a global chemistry and aerosol transport model (Oslo CTM2). The sulphur cycle and sea salt particles have been implemented earlier in the Oslo CTM2 and the focus of this study is on whether nitrate particles are formed as fine mode ammonium nitrate or react on existing sea salt particles. The model results show that ammonium nitrate particles play a non-negligible role in the total aerosol composition in certain industrialized regions and therefore have a significant local radiative forcing. On a global scale the aerosol optical depth of ammonium nitrate is relatively small due to limited availability of ammonia and reaction with sea salt particles. Inclusion of sea salt in the calculations reduces the aerosol optical depth and burden of ammonium nitrate particles by 25% on a global scale but with large regional variations. [ABSTRACT FROM AUTHOR]

Changes in atmospheric ozone have occurred since the preindustrial era as a result of increasing anthropogenic emissions. Within ACCENT, a European Network of Excellence, ozone changes between 1850 and 2000 are assessed for the troposphere and the lower stratosphere (up to 30 km) by a variety of seven chemistry-climate models and three chemical transport models. The modeled ozone changes are taken as input for detailed calculations of radiative forcing. When only changes in chemistry are considered (constant climate) the modeled global-mean tropospheric ozone column increase since preindustrial times ranges from 7.9DU to 13.8DU among the ten participating models, while the stratospheric column reduction lies between 14.1DU and 47.9DU in the models considering stratospheric chemistry. The resulting radiative forcing is strongly dependent on the location and altitude of the modeled ozone change and varies between 0.26Wm-2 and 0.53Wm-2 due to ozone change in the troposphere and -0.25Wm-2 and +0.12Wm-2 due to the stratospheric ozone change. Changes in ozone and other greenhouse gases since preindustrial times have altered climate. Six out of the ten participating models have performed an additional calculation taking into account both chemical and climate change. The isolated effect of climate change is an enhancement of the tropospheric ozone column increase in all models, ranging from 1% to 37%, while the stratospheric reduction becomes slightly less severe in most models. In the three climate-chemistry models with detailed tropospheric and stratospheric chemistry the inclusion of climate change increases the resulting radiative forcing due to tropospheric ozone change by up to 0.08Wm-2, while the radiative forcing due to stratospheric ozone change is reduced by up to 0.14Wm-2. Considering tropospheric and stratospheric change combined, the total ozone column change is negative while the resulting net radiative forcing is positive. [ABSTRACT FROM AUTHOR]