Search

As the third most important greenhouse gas (GHG) after carbon dioxide (CO2) and methane (CH4), tropospheric ozone (O3) is also an air pollutant causing damage to human health and ecosystems. This study brings together recent research on observations and modeling of tropospheric O3 in the Arctic, a rapidly warming and sensitive environment. At different locations in the Arctic, the observed surface O3 seasonal cycles are quite different. Coastal Arctic locations, for example, have a minimum in the springtime due to O3 depletion events resulting from surface bromine chemistry. In contrast, other Arctic locations have a maximum in the spring. The 12 state-of-the-art models used in this study lack the surface halogen chemistry needed to simulate coastal Arctic surface O3 depletion in the springtime; however, the multi-model median (MMM) has accurate seasonal cycles at non-coastal Arctic locations. There is a large amount of variability among models, which has been previously reported, and we show that there continues to be no convergence among models or improved accuracy in simulating tropospheric O3 and its precursor species. The MMM underestimates Arctic surface O3 by 5 % to 15 % depending on the location. The vertical distribution of tropospheric O3 is studied from recent ozonesonde measurements and the models. The models are highly variable, simulating free-tropospheric O3 within a range of ±50 % depending on the model and the altitude. The MMM performs best, within ±8 % for most locations and seasons. However, nearly all models overestimate O3 near the tropopause (∼300 hPa or ∼8 km), likely due to ongoing issues with underestimating the altitude of the tropopause and excessive downward transport of stratospheric O3 at high latitudes. For example, the MMM is biased high by about 20 % at Eureka. Observed and simulated O3 precursors (CO, NOx, and reservoir PAN) are evaluated throughout the troposphere. Models underestimate wintertime CO everywhere, likely due to a combination of underestimating CO emissions and possibly overestimating OH. Throughout the vertical profile (compared to aircraft measurements), the MMM underestimates both CO and NOx but overestimates PAN. Perhaps as a result of competing deficiencies, the MMM O3 matches the observed O3 reasonably well. Our findings suggest that despite model updates over the last decade, model results are as highly variable as ever and have not increased in accuracy for representing Arctic tropospheric O3.

As the third most important greenhouse gas (GHG) after CO2 and methane, tropospheric ozone (O3) is also an air pollutant causing damage to human health and ecosystems. This study brings together recent research on observations and modeling of tropospheric O3 in the Arctic, a rapidly warming and sensitive environment. At different locations in the Arctic, the observed surface O3 seasonal cycles are quite different. Coastal Arctic locations, for example, have a minimum in the springtime due to O3 depletion events resulting from surface bromine chemistry. In contrast, other Arctic locations have a maximum in the spring. The 12 state-of-the-art models used in this study lack the surface halogen chemistry needed to simulate coastal Arctic surface O3 depletion in the springtime, however, the multi-model median (MMM) has accurate seasonal cycles at non-coastal Arctic locations. There is a large amount of variability among models, which has been reported previously, and we show that there continues to be no convergence among models, nor improved accuracy in simulating tropospheric O3 and its precursor species. The MMM underestimates Arctic surface O3 by 5 % to 15 % depending on the location. The vertical distribution of tropospheric O3 is studied from recent ozonesonde measurements and the models. The models are highly variable, simulating free-tropospheric O3 within a range of +/- 50 % depending on the model and the altitude. The MMM performs best, within +/- 8 % at most locations and seasons. However, nearly all models overestimate O3 near the tropopause (~300 hPa or ~8 km), likely due to ongoing issues with underestimating the altitude of the tropopause and excessive downward transport of stratospheric O3 at high latitudes. For example, the MMM is biased high by about 20 % at Eureka. Observed and simulated O3 precursors (CO, NOx and reservoir PAN) are evaluated throughout the troposphere. Models underestimate wintertime CO everywhere, likely due to a combination of underestimating CO emissions and possibly overestimating OH. Throughout the vertical profile (compared to aircraft measurements), the MMM underestimates both CO and NOx but overestimates PAN. Perhaps as a result of competing deficiencies, the MMM O3 matches the observed O3 reasonably well. Our findings suggest that despite model updates over the last decade , model results are as highly variable as ever, and have not increased in accuracy for representing Arctic tropospheric.

The Arctic atmosphere is warming rapidly and its relatively pristine environment is sensitive to the long-range transport of atmospheric pollutants. While carbon dioxide is the main cause for global warming, short-lived climate forcers (SLCFs) such as methane, ozone, and particles also play a role in Arctic climate on near-term time scales. Atmospheric modelling is critical for understanding the abundance and distribution of SLCFs throughout the Arctic atmosphere, and is used as a tool towards determining SLCF impacts on climate and health in the present and in future emissions scenarios. In this study, we evaluate 18 state-of-the-art atmospheric and Earth system models, assessing their representation of Arctic and Northern Hemisphere atmospheric SLCF distributions, considering a wide range of different chemical species (methane, tropospheric ozone and its precursors, black carbon, sulfate, organic aerosol, and particulate matter) and multiple observational datasets. Model simulations over four years (2008–2009 and 2014–2015) conducted for the 2021 Arctic Monitoring and Assessment Programme (AMAP) SLCF assessment report are thoroughly evaluated against satellite, ground, ship and aircraft-based observations. The results show a large range in model performance, with no one particular model or model type performing well for all regions and all SLCF species. The multi-model mean was able to represent the general features of SLCFs in the Arctic, though vertical mixing, long-range transport, deposition, and wildfire emissions remain highly uncertain processes. These need better representation within atmospheric models to improve their simulation of SLCFs in the Arctic environment.

Dust is one of the dominant aerosol types over Asia and the North Pacific Ocean, but quantitative estimation of dust distribution and its contribution to the total regional aerosol load from observations is challenging due to the presence of significant anthropogenic and natural aerosols and the frequent influence of clouds over the region. This study presents the dust aerosol distributions over Asia and the North Pacific using simulations from five global models that participated in the AeroCom phase II model experiments, and from multiple satellite remote-sensing and ground-based measurements of total aerosol optical depth (AOD) and dust optical depth (DOD). We examine various aspects of aerosol and dust presence in our study domain: (1) the horizontal distribution, (2) the longitudinal gradient during trans-Pacific transport, (3) seasonal variations, (4) vertical profiles, and (5) model-simulated dust life cycles. This study reveals that the diversity of DOD is mostly driven by the diversity of the dust source followed by residence time and mass extinction efficiency.

The COVID-19 lockdown measures gradually implemented in Lombardy (northern Italy) from 23 February 2020 led to a downturn in several economic sectors with possible impacts on air quality. Several communications claimed in the first weeks of March 2020 that the mitigation in air pollution observed at that time was actually related to these lockdown measures without considering that seasonal variations in emissions and meteorology also influence air quality. To determine the specific impact of lockdown measures on air quality in northern Italy, we compared observations from the European Commission Atmospheric Observatory of Ispra (regional background) and from the regional environmental protection agency (ARPA) air monitoring stations in the Milan conurbation (urban background) with expected values for these observations using two different approaches. On the one hand, intensive aerosol variables determined from specific aerosol characterisation observations performed in Ispra were compared to their 3-year averages. On the other hand, ground-level measured concentrations of atmospheric pollutants (NO2, PM10, O3, NO, SO2) were compared to expected concentrations derived from the Copernicus Atmosphere Monitoring Service Regional (CAMS) ensemble model forecasts, which did not account for lockdown measures. From these comparisons, we show that NO2 concentrations decreased as a consequence of the lockdown by −30 % and −40 % on average at the urban and regional background sites, respectively. Unlike NO2, PM10 concentrations were not significantly affected by lockdown measures. This could be due to any decreases in PM10 (and PM10 precursors) emissions from traffic being compensated for by increases in emissions from domestic heating and/or from changes in the secondary aerosol formation regime resulting from the lockdown measures. The implementation of the lockdown measures also led to an increase in the highest O3 concentrations at both the urban and regional background sites resulting from reduced titration of O3 by NO. The relaxation of the lockdown measures beginning in May resulted in close-to-expected NO2 concentrations in the urban background and to significant increases in PM10 in comparison to expected concentrations at both regional and urban background sites.

Cyanobacteria blooms are a worldwide concern for water bodies and may be promoted by eutrophication and climate change. The prediction of cyanobacterial blooms and identification of the main triggering factors are of paramount importance for water management. In this study, we analyzed a comprehensive dataset including ten-years measurements collected at Lake Varese, an eutrophic lake in Northern Italy. Microscopic analysis of the water samples was performed to characterize the community distribution and dynamics along the years. We observed that cyanobacteria represented a significant fraction of the phytoplankton community, up to 60% as biovolume, and a shift in the phytoplankton community distribution towards cyanobacteria dominance onwards 2010 was detected. The relationships between cyanobacteria biovolume, nutrients, and environmental parameters were investigated through simple and multiple linear regressions. We found that 14-days average air temperature together with total phosphorus may only partly explain the cyanobacteria biovolume variance at Lake Varese. However, weather forecasts can be used to predict an algal outbreak two weeks in advance and, eventually, to adopt management actions. The prediction of cyanobacteria algal blooms remains challenging and more frequent samplings, combined with the microscopy analysis and the metagenomics technique, would allow a more conclusive analysis.

The impact of air pollution on premature mortality in Europe and the United States (U.S.) in 2010 is modelled by a multi-model ensemble of regional models in the framework of the third phase of the Air Quality Model Evaluation International Initiative (AQMEII3). Introducing 20% emission reductions both globally and regionally in Europe, North America and East Asia were performed in order to calculate the domestic and foreign contributions to air quality and related premature mortality. Total premature mortality was estimated to be 414 000 in Europe and 160 000 in the U.S., using multi-model mean pollutant concentrations. The number of premature mortality cases calculated using concentration inputs from different air quality models can vary by up to a factor of three. Results show that the domestic emissions have the largest impacts on premature death, while foreign sources are a minor contributor to adverse impacts of air pollution.

Winter warming and sea-ice retreat observed in the Arctic in the last decades may be related to changes of large-scale atmospheric circulation pattern, which may impact the transport of black carbon (BC) to the Arctic and its deposition on the sea ice, with possible feedbacks on the regional and global climate forcing. In this study we developed and applied a statistical algorithm, based on the maximum likelihood estimate approach, to determine how the changes of three large-scale weather patterns associated with increasing temperatures in winter and sea-ice retreat in the Arctic impact the transport of BC to the Arctic and its deposition. We found that two atmospheric patterns together determine a decreasing winter deposition trend of BC between 1980 and 2015 in the eastern Arctic while they increase BC deposition in the western Arctic. The increasing BC trend is mainly due to a pattern characterized by a high-pressure anomaly near Scandinavia favouring the transport in the lower troposphere of BC from Europe and North Atlantic directly into to the Arctic. Another pattern with a high-pressure anomaly over the Arctic and low-pressure anomaly over the North Atlantic Ocean has a smaller impact on BC deposition but determines an increasing BC atmospheric load over the entire Arctic Ocean with increasing BC concentrations in the upper troposphere. The results show that changes in atmospheric circulation due to polar atmospheric warming and reduced winter sea ice significantly impacted BC transport and deposition. The anthropogenic emission reductions applied in the last decades were, therefore, crucial to counterbalance the most likely trend of increasing BC pollution in the Arctic.

Through the comparison of several regional-scale chemistry transport modeling systems that simulate meteorology and air quality over the European and North American continents, this study aims at (i) apportioning error to the responsible processes using timescale analysis, (ii) helping to detect causes of model error, and (iii) identifying the processes and temporal scales most urgently requiring dedicated investigations. The analysis is conducted within the framework of the third phase of the Air Quality Model Evaluation International Initiative (AQMEII) and tackles model performance gauging through measurement-to-model comparison, error decomposition, and time series analysis of the models biases for several fields (ozone, CO, SO2, NO, NO2, PM10, PM2. 5, wind speed, and temperature). The operational metrics (magnitude of the error, sign of the bias, associativity) provide an overall sense of model strengths and deficiencies, while apportioning the error to its constituent parts (bias, variance, and covariance) can help assess the nature and quality of the error. Each of the error components is analyzed independently and apportioned to specific processes based on the corresponding timescale (long scale, synoptic, diurnal, and intraday) using the error apportionment technique devised in the former phases of AQMEII. The application of the error apportionment method to the AQMEII Phase 3 simulations provides several key insights. In addition to reaffirming the strong impact of model inputs (emission and boundary conditions) and poor representation of the stable boundary layer on model bias, results also highlighted the high interdependencies among meteorological and chemical variables, as well as among their errors. This indicates that the evaluation of air quality model performance for individual pollutants needs to be supported by complementary analysis of meteorological fields and chemical precursors to provide results that are more insightful from a model development perspective. This will require evaluation methods that are able to frame the impact on error of processes, conditions, and fluxes at the surface. For example, error due to emission and boundary conditions is dominant for primary species (CO, particulate matter (PM)), while errors due to meteorology and chemistry are most relevant to secondary species, such as ozone. Some further aspects emerged whose interpretation requires additional consideration, such as the uniformity of the synoptic error being region- and model-independent, observed for several pollutants; the source of unexplained variance for the diurnal component; and the type of error caused by deposition and at which scale.

Past reductions of anthropogenic aerosol concentrations in Europe and North America could have amplified Arctic warming. In the future the impact of air pollution policies may differ, because the major anthropogenic sources of atmospheric aerosols are increasingly located in Asia. In this study numerical experiments evaluating only direct aerosol effects on atmospheric temperatures indicate that, while reduced carbon dioxide (CO2) emissions weaken Arctic warming, direct radiative forcing effects by reductions of anthropogenic aerosol concentrations, additional to those obtained by lower CO2 emissions, can either amplify or diminish it. Interactions between regionally modified radiation in Asia and internal climate variability may differently initiate and sustain atmospheric planetary waves propagating into the Arctic. In a nonlinear manner planetary waves may redistribute atmospheric and oceanic meridional heat fluxes at the high latitudes and either amplify or diminish Arctic warming in 2050. Lower CO2 concentrations might apparently contribute to reduce the interactions between the Arctic system and the lower latitudes, thus reducing the influence of strong air quality measures in Asia on the Arctic amplification of global warming. While past and present air pollution policies could have amplified Arctic warming, in the future the effects from atmospheric pollution reductions are less certain, depending on the future CO2 concentrations, and requiring improved simulations of changing aerosol concentrations and their interactions with clouds in Asia and the Arctic.

The impact of air pollution on human health and the associated external costs in Europe and the United States (US) for the year 2010 are modeled by a multi-model ensemble of regional models in the frame of the third phase of the Air Quality Modelling Evaluation International Initiative (AQMEII3)

Source at https://doi.org/10.5194/acp-18-10199-2018. The evaluation and intercomparison of air quality models is key to reducing model errors and uncertainty. The projects AQMEII3 and EURODELTA-Trends, in the framework of the Task Force on Hemispheric Transport of Air Pollutants and the Task Force on Measurements and Modelling, respectively (both task forces under the UNECE Convention on the Long Range Transport of Air Pollution, LTRAP), have brought together various regional air quality models to analyze their performance in terms of air concentrations and wet deposition, as well as to address other specific objectives. This paper jointly examines the results from both project communities by intercomparing and evaluating the deposition estimates of reduced and oxidized nitrogen (N) and sulfur (S) in Europe simulated by 14 air quality model systems for the year 2010. An accurate estimate of deposition is key to an accurate simulation of atmospheric concentrations. In addition, deposition fluxes are increasingly being used to estimate ecological impacts. It is therefore important to know by how much model results differ and how well they agree with observed values, at least when comparison with observations is possible, such as in the case of wet deposition. This study reveals a large variability between the wet deposition estimates of the models, with some performing acceptably (according to previously defined criteria) and others underestimating wet deposition rates. For dry deposition, there are also considerable differences between the model estimates. An ensemble of the models with the best performance for N wet deposition was made and used to explore the implications of N deposition in the conservation of protected European habitats. Exceedances of empirical critical loads were calculated for the most common habitats at a resolution of 100 × 100m2 within the Natura 2000 network, and the habitats with the largest areas showing exceedances are determined. Moreover, simulations with reduced emissions in selected source areas indicated a fairly linear relationship between reductions in emissions and changes in the deposition rates of N and S. An approximate 20% reduction in N and S deposition in Europe is found when emissions at a global scale are reduced by the same amount. European emissions are by far the main contributor to deposition in Europe, whereas the reduction in deposition due to a decrease in emissions in North America is very small and confined to the western part of the domain. Reductions in European emissions led to substantial decreases in the protected habitat areas with critical load exceedances (halving the exceeded area for certain habitats), whereas no change was found, on average, when reducing North American emissions in terms of average values per habitat.

The impact of air pollution on human health and the associated external costs in Europe and the United States (U.S.) for the year 2010 is modelled by a multi-model ensemble of regional models in the frame of the third phase of the Air Quality Modelling Evaluation International Initiative (AQMEII3). This is the first study known to use a common health assessment approach across the two continents. The modelled surface concentrations of O3, CO, SO2 and PM2.5 from each model are used as input to the Economic Valuation of Air Pollution (EVA) system to calculate the resulting health impacts and the associated external costs. Along with a base case simulation, additional runs were performed introducing 20 % emission reductions both globally and regionally in Europe, North America and East Asia. Health impacts estimated by different models can vary up to a factor of three in Europe (twelve models) and the United States (three models). In Europe, the multi-model mean number of premature deaths is calculated to be 414 000 while in the U.S., it is estimated to be 160 000, in agreement with previous global and regional studies. In order to estimate the impact of biases coming from each model, two multi-model ensembles were produced, the first attributing an equal weight to each member of the ensemble, and the second where the subset of models that produce the smallest error compared to the surface observations at each time step. The latter results in increase of health impacts by up to 30 % in Europe, thus giving significantly higher mortality estimates compared to available literature. This is mostly due to a 27 % increase in the domain mean PM2.5 levels, along with a slight increase in O3 by ~ 1 %. Over the U.S., the mean PM2.5 and O3 levels decrease by 11 % and 2 %, respectively, when the optimal ensemble mean is used, leading to a decrease in the calculated health impacts by ~ 11 %. These differences encourage the use of optimal-reduced multi-model ensembles over traditional all model-mean ensembles, in particular for policy applications. Finally, the role of domestic versus foreign emission sources on the related health impacts is investigated using the 20 % emission reduction scenarios applied over the source regions as defined in the frame of HTAP2. The differences are calculated based on the models that are common in the basic multi-model ensemble and the perturbation scenarios, resulting in five models in Europe and all three models in the U.S. A 20 % reduction of global anthropogenic emissions avoids 54 000 and 27 500 premature deaths in Europe and the U.S., respectively. A 20 % reduction of North American emissions foreign emissions avoids ~ 1000 premature deaths in Europe and 25 000 premature deaths in the U.S. A 20 % decrease of emissions within the European source region avoids 47 000 premature deaths in Europe. Reducing the East Asian emission by 20 % avoids ~ 2000 premature deaths in the U.S. These results show that the domestic emissions make the largest impacts on premature death, while foreign sources make a minor contributing to adverse impacts of air pollution.

We analyze temporal trends of peroxyacetyl nitrate (PAN) retrievals from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) during 2002–2011 in the altitude range 8–23 km over the Asian summer monsoon (ASM) region. The greatest enhancements of PAN mixing ratios in the upper troposphere and lower stratosphere (UTLS) are seen during the summer monsoon season from June to September. During the monsoon season, the mole fractions of PAN show statistically significant (at 2σ) positive trends from 0.2 ± 0.05 to 4.6 ± 3.1 ppt yr−1 (except between 12 and 14 km) which is higher than the annual mean trends of 0.1 ± 0.05 to 2.7 ± 0.8 ppt yr−1. These rising concentrations point to increasing NOx (= NO + NO2) and volatile organic compound (VOC) emissions from developing nations in Asia, notably India and China. We analyze the influence of monsoon convection on the distribution of PAN in UTLS with simulations using the global chemistry–climate model ECHAM5-HAMMOZ. During the monsoon, transport into the UTLS over the Asian region primarily occurs from two convective zones, one the South China Sea and the other over the southern flank of the Himalayas. India and China host NOx-limited regimes for ozone photochemical production, and thus we use the model to evaluate the contributions from enhanced NOx emissions to the changes in PAN, HNO3 and O3 concentrations in the UTLS. From a set of sensitivity experiments with emission changes in particular regions, it can be concluded that Chinese emissions have a greater impact on the concentrations of these species than Indian emissions. According to SCanning Imaging Absorption SpectroMeter for Atmospheric CHartographY (SCIAMACHY) NO2 retrievals NOx emissions increases over India have been about half of those over China between 2002 and 2011.

The Chernobyl Nuclear Power Plant (CNPP) accident occurred on April 26 of 1986, it is still an episode of interest, due to the large amount of radionuclides dispersed in the atmosphere. Caesium-137 ((137)Cs) is one of the main radionuclides emitted during the Chernobyl accident, with a half-life of 30years, which can be accumulated in humans and animals, and for this reason the impacts on population are still monitored today. One of the main parameters in order to estimate the exposure of population to (137)Cs is the concentration in the air, during the days after the accident, and the deposition at surface. The transport and deposition of (137)Cs over Europe occurred after the CNPP accident has been simulated using the WRF-HYSPLIT modeling system. Four different vertical and temporal emission rate profiles have been simulated, as well as two different dry deposition velocities. The model simulations could reproduce fairly well the observations of (137)Cs concentrations and deposition, which were used to generate the 'Atlas of Caesium deposition on Europe after the Chernobyl accident' and published in 1998. An additional focus was given on (137)Cs deposition and air concentrations over Turkey, which was one of the main affected countries, but not included in the results of the Atlas. We estimated a total deposition of 2-3.5 PBq over Turkey, with 2 main regions affected, East Turkey and Central Black Sea coast until Central Anatolia, with values between 10 kBq m(-2) and 100 kBq m(-2). Mean radiological effective doses from simulated air concentrations and deposition has been estimated for Turkey reaching 0.15 mSv/year in the North Eastern part of Turkey, even if the contribution from ingestion of contaminated food and water is not considered, the estimated levels are largely below the 1 mSv limit indicated by the International Commission on Radiological Protection.

Black carbon (BC) is an important component of particulate matter due to its effects on human health and climate. In this study, we present the first BC concentrations measured in the Istanbul megacity (similar to 15 million inhabitants). Two measurement campaigns have been conducted to measure BC and fine particulate matter (PM2.5) concentrations at four locations, characterized by different traffic densities. In the first campaign, BC daily mean concentrations have been found to be between 4 mu g/m(3) and 10 mu g/m(3). In the second campaign, BC and PM2.5 have been measured at the site with the highest traffic density for an entire year. Annually averaged BC contributes by 38 +/- 14% to the PM2.5 levels (annual average BC: 13 mu g/m(3) and PM2.5: 36 mu g/m(3)). Diurnal variations of BC concentrations followed those of traffic density (correlation coefficient of 0.87). These measurements are essential to identify the sources of BC and PM2.5 concentrations in Istanbul and develop mitigation measures. (C) 2013 Elsevier B.V. All rights reserved.

[1] This study investigates changes in extreme temperature and precipitation events under different future scenarios of anthropogenic aerosol emissions (i.e., SO2 and black and organic carbon) simulated with an aerosol-climate model (ECHAM5-HAM) with focus on Europe. The simulations include a maximum feasible aerosol reduction (MFR) scenario and a current legislation emission (CLEmod) scenario where Europe implements the MFR scenario, but the rest of the world follows the current legislation scenario and a greenhouse gas scenario. The strongest changes relative to the year 2000 are projected for the MFR scenario, in which the global aerosol reduction greatly enforces the general warming effect due to greenhouse gases and results in significant increases of temperature and precipitation extremes in Europe. Regional warming effects can also be identified from aerosol reductions under the CLEmodscenario. This becomes most obvious in the increase of the hottest summer daytime temperatures in Northern Europe.

Winter warming and sea ice retreat observed in the Arctic in the last decades determine changes of large scale atmospheric circulation pattern that may impact as well the transport of black carbon (BC) to the Arctic and its deposition on the sea ice, with possible feedbacks on the regional and global climate forcing. In this study we developed and applied a new statistical algorithm, based on the Maximum Likelihood Estimate approach, to determine how the changes of three large scale weather patterns (the North Atlantic Oscillation, the Scandinavian Blocking, and the El Nino-Southern Oscillation), associated with winter increasing temperatures and sea ice retreat in the Arctic, impact the transport of BC to the Arctic and its deposition. We found that the three atmospheric patterns together determine a decreasing winter deposition trend of BC between 1980 and 2015 in the Eastern Arctic while they increase BC deposition in the Western Arctic. The increasing trend is mainly due to the more frequent occurrences of stable high pressure systems (atmospheric blocking) near Scandinavia favouring the transport in the lower troposphere of BC from Europe and North Atlantic directly into to the Arctic. The North Atlantic Oscillation has a smaller impact on BC deposition in the Arctic, but determines an increasing BC atmospheric load over the entire Arctic Ocean with increasing BC concentrations in the upper troposphere. The El Nino-Southern Oscillation does not influence significantly the transport and deposition of BC to the Arctic. The results show that changes in atmospheric circulation due to polar atmospheric warming and reduced winter sea ice significantly impacted BC transport and deposition. The anthropogenic emission reductions applied in the last decades were, therefore, crucial to counterbalance the most likely trend of increasing BC pollution in the Arctic.

In this paper, we introduce the ECHAM5-HAMMOZ aerosol-chemistry-climate model that includes fully interactive simulations of Ox-NOx-hydrocarbons chemistry and of aerosol microphysics (including prognostic size distribution and mixing state of aerosols) implemented in the General Circulation Model ECHAM5. The photolysis rates used in the gas chemistry account for aerosol and cloud distributions and a comprehensive set of heterogeneous reactions is implemented. The model is evaluated with trace gas and aerosol observations provided by the TRACE-P aircraft experiment. Sulfate concentrations are well captured but black carbon concentrations are underestimated. The number concentrations, surface areas, and optical properties are reproduced fairly well near the surface but underestimated in the upper troposphere. CO concentrations are well reproduced in general while O3 concentrations are overestimated by 10-20 ppbv. We find that heterogeneous chemistry significantly influences the regional and global distributions of a number of key trace gases. Heterogeneous reactions reduce the ozone surface concentrations by 18-23% over the TRACE-P region and the global annual mean O3 burden by 7%. The annual global mean OH concentration decreases by 10% inducing a 7% increase in the global CO burden. Annual global mean HNO3 surface concentration decreases by 15% because of heterogenous reaction on mineral dust. A comparison of our results to those from previous studies suggests that the choice of uptake coefficients for a given species is the critical parameter that determines the global impact of heterogeneous chemistry on a trace gas (rather than the description of aerosol properties and distributions). A prognostic description of the size distribution and mixing state of the aerosols is important, however, to account for the effect of heterogeneous chemistry on aerosols as further discussed in the second part of this two-part series. Copyright 2008 by the American Geophysical Union.

Ozone pollution represents a serious health and environmental problem. While ozone pollution is mostly produced by photochemistry in summer, elevated ozone concentrations can also be influenced by long range transport driven by the atmospheric circulation and stratospheric ozone intrusions. We analyze the role of large scale atmospheric circulation variability in the North Atlantic basin in determining surface ozone concentrations. Here, we show, using ground station measurements and a coupled atmosphere-chemistry model simulation for the period 1980–2005, that the North Atlantic Oscillation (NAO) does affect surface ozone concentrations – on average, over 10 ppbv on the monthly mean in southwest central and northern Europe – during all seasons except fall. The commonly used NAO index is able to capture the link existing between atmospheric dynamics and surface ozone concentrations in winter and spring but it fails in summer. We find that the first Principal Component, computed from the time variation of the sea level pressure (SLP) field, detects the atmosphere circulation/ozone relationship not only in winter and spring but also during summer, when the atmospheric circulation weakens and regional photochemical processes peak. The first Principal Component of the SLP field could be used as a tool to identify areas more exposed to forthcoming ozone pollution events. Finally, our results suggest that the increasing baseline ozone in western and northern Europe during the 1990s could be related to the prevailing phase of the NAO in that period., JRC.H.7-Climate Risk Management

The degree of non-linearity in DMS-cloud-climate interactions is assessed using the ECHAM5-HAMMOZ model by taking into account end-to-end aerosol chemistry-cloud microphysics link. The evaluation is made over the Southern oceans in austral summer, a region of minimal anthropogenic influence. In this study, we compare the DMS-derived changes in the aerosol and cloud microphysical properties between a baseline simulation with the ocean DMS emissions from a prescribed climatology, and a scenario where the DMS emissions are doubled. Our results show that doubling the DMS emissions in the current climate results in a non-linear response in atmospheric DMS burden and subsequently, in SO2 and H2SO4 burdens due to inadequate OH oxidation. The aerosol optical depth increases by only ~20 % in the 30° S–75° S belt in the SH summer months. This increases the vertically integrated cloud droplet number concentrations (CDNC) by 25 %. Since the vertically integrated liquid water vapor is constant in our model simulations, an increase in CDNC leads to a reduction in cloud droplet radius of 3.4 % over the Southern oceans in summer. The equivalent increase in cloud liquid water path is 10.7 %. The above changes in cloud microphysical properties result in a change in global annual mean radiative forcing at the TOA of −1.4 W m−2. The results suggest that the DMS-cloud microphysics link is highly non-linear. This has implications for future studies investigating the DMS-cloud climate feedbacks in a warming world and for studies evaluating geoengineering options to counteract warming by modulating low level marine clouds.

Among the atmospheric emission sources, wildfires are episodic events characterized by large spatial and temporal variability. Therefore, accurate information on gaseous and aerosol emissions from fires for specific regions and seasons is critical for air quality forecasts. The Spinning Enhanced Visible and Infrared Imager (SEVIRI) in geostationary orbit provides fire observations over Africa and the Mediterranean with a temporal resolution of 15 min. It thus resolves the complete fire life cycle and captures the fires' peak intensities, which is not possible in Moderate Resolution Imaging Spectroradiometer (MODIS) fire emission inventories like the Global Fire Assimilation System (GFAS). We evaluate two different operational fire radiative power (FRP) products derived from SEVIRI, by studying a large forest fire in Antalya, Turkey, in July-August 2008. The EUMETSAT Land Surface Analysis Satellite Applications Facility (LSA SAF) has higher FRP values during the fire episode than the Wildfire Automated Biomass Burning Algorithm (WF-ABBA). It is also in better agreement with the co-located, gridded MODIS FRP. Both products miss small fires that frequently occur in the region and are detected by MODIS. Emissions are derived from the FRP products. They are used along-side GFAS emissions in smoke plume simulations with the Weather Research and Forecasting (WRF) model and the Community Multiscale Air Quality (CMAQ) model. In comparisons with MODIS aerosol optical thickness (AOT) and Infrared Atmospheric Sounding Interferometer (IASI), CO and NH3 observations show that including the diurnal variability of fire emissions improves the spatial distribution and peak concentrations of the simulated smoke plumes associated with this large fire. They also show a large discrepancy between the currently available operational FRP products, with the LSA SAF being the most appropriate., SCOPUS: ar.j, info:eu-repo/semantics/published

13 pages, 5 figures, supporting information http://dx.doi.org/10.1002/2014JD022687, One of the critical parameters in assessing the global impacts of dimethyl sulfide (DMS) on cloud properties and the radiation budget is the estimation of phytoplankton-induced ocean emissions, which are derived from prescribed, climatological surface seawater DMS concentrations. The most widely used global ocean DMS climatology was published 15 years ago and has recently been updated using a much larger database of observations. The updated climatology displays significant differences in terms of the global distribution and regional monthly averages of sea surface DMS. In this study, we use the ECHAM5-HAMMOZ aerosol-chemistry-climate general circulation model to quantify the influence of the updated DMS climatology in computed atmospheric properties, namely, the spatial and temporal distributions of atmospheric DMS concentration, sulfuric acid concentration, sulfate aerosols, number of activated aerosols, cloud droplet number concentration, and the aerosol radiative forcing at the top of the atmosphere. Significant differences are observed for all the modeled variables. Comparison with observations of atmospheric DMS and total sulfate also shows that in places with large DMS emissions, the updated climatology shows a better match with the observations. This highlights the importance of using the updated climatology for projecting future impacts of oceanic DMS emissions, especially considering that the relative importance of the natural sulfur fluxes is likely to increase due to legislation to “clean up” anthropogenic emissions. The largest estimated differences are in the Southern Ocean, Indian Ocean, and parts of the Pacific Ocean, where the climatologies differ in seasonal concentrations over large geographical areas. The model results also indicate that the former DMS climatology underestimated the effect of DMS on the globally averaged annual aerosol radiative forcing at the top of the atmosphere by about 20%, The Indian Institute of Tropical Meteorology is supported by the Ministry of Earth Sciences, Government of India. S.-J.R. and R.S. acknowledge support from the former Spanish Ministry of Science and Innovation through projects PRISMA and Malaspina 2010

Among the atmospheric emission sources, wildfires are episodic events characterized by large spatial and temporal variability. Therefore, accurate information on fire gaseous and aerosol emissions for specific regions and seasons is critical for air quality forecasts. The Spinning Enhanced Visible and Infrared Imager (SEVIRI) in geostationary orbit provides fire observations over Africa and the Mediterranean with a unique temporal resolution of 15min. It thus resolves the complete fire life cycle and captures the fires' peak intensities, which is not possible in MODIS-based fire emission inventories like GFAS. We evaluate two different operational Fire Radiative Power (FRP) products derived from SEVIRI, by studying the case of a large forest fire in Antalya, Turkey, in July-August 2008. The EUMETSAT LSA SAF product has higher FRP values during the fire episode than the WF-ABBA product. It is also in better agreement with the colocated, gridded MODIS FRP. Both products miss small fires that frequently occur in the region and are detected by MODIS. Emissions are derived from the FRP products. They are used along-side GFAS emissions in smoke plume simulations with WRF and the Community Multiscale Air Quality model (CMAQ). Comparisons with MODIS AOT and IASI CO and NH3 observations show that including the diurnal variability of fire emissions improves the spatial distribution and peak concentrations of the simulated smoke plumes associated to the large fire. They also show a large discrepancy between the currently available operational FRP products, with the LSA SAF one being the most appropriate., SCOPUS: re.j, info:eu-repo/semantics/published

The purpose of this study is to investigate a dust transport episode using atmospheric 3D modeling, satellite data, and in-situ observations. 3D simulations have been used to determine the aerosol optical properties and direct radiative effects of dust particles. In this study, the number of daily exceedances due to dust transport is estimated and, performance of RegCM4.1 model tested quantitatively with the aid of AOD data from AERONET network and PM10) ground measurements. The impact of dust on radiation estimated by the model for the 4-day period. PM10, values for Istanbul for the period between 2004-2010, and Marmara and Aegean Region for March 2008 provided by the Turkish Ministry of Environment were used to select an important episode. Exceedance days were evaluated according to the BSC-DREAM8b model output. We have used the RegCM4.1 model to further investigate the Saharan dust transport in the selected episode 21-24 March 2008. First, observed daily mean PM10 concentrations reach up to 180 mu g/m(3) in Marmara Region and 160 mu g/m(3) in Aegean Region, respectively. According to the RegCM4.1 model outputs, station Erdemli presents the highest AOD on 23rd March 2008, around 12, which is found to be highest than AERONET observations (ADD of 0.7). In parallel, daily mean AOD in Marmara Region is around 1.0 on the same day. Corresponding simulated column burden is about 1000 mg/m(2) in Marmara Region and 750 mg/m(2) in Aegean Region, respectively. In terms of radiative effect, daily mean shortwave (all-sky) radiative effect at surface (ToA) is -62 W/m(2) (-29 W/m(2)) in Marmara and -71 W/m(2) (-33 W/m(2)) in Aegean Region, respectively. In parallel, longwave all-sky direct forcing at surface (ToA) is + 7 W/m(2) and (+4 W/m(2)) in Marmara, +11 W/m(2) (+4 W/m(2)) in Aegean Region. (C) 2014 Elsevier B.V. All rights reserved.

The Asian summer monsoon involves complex transport patterns with large-scale redistribution of trace gases in the upper troposphere and lower stratosphere (UTLS). We employ the global chemistry–climate model ECHAM5–HAMMOZ in order to evaluate the transport pathways and the contributions of nitrogen oxide species peroxyacetyl nitrate (PAN), NOx and HNO3 from various monsoon regions, to the UTLS over southern Asia and vice versa. Simulated long-term seasonal mean mixing ratios are compared with trace gas retrievals from the Michelson Interferometer for Passive Atmospheric Sounding aboard ENVISAT(MIPAS-E) and aircraft campaigns during the monsoon season (June–September) in order to evaluate the model's ability to reproduce these transport patterns. The model simulations show that there are three regions which contribute substantial pollution to the South Asian UTLS: the Asian summer monsoon (ASM), the North American monsoon (NAM) and the West African monsoon (WAM). However, penetration due to ASM convection reaches deeper into the UTLS compared to NAM and WAM outflow. The circulation in all three monsoon regions distributes PAN into the tropical latitude belt in the upper troposphere (UT). Remote transport also occurs in the extratropical UT where westerly winds drive North American and European pollutants eastward where they can become part of the ASM convection and lifted into the lower stratosphere. In the lower stratosphere the injected pollutants are transported westward by easterly winds. Sensitivity experiments with ECHAM5–HAMMOZ for simultaneous NOx and non-methane volatile organic compounds (NMVOCs) emission change (−10 %) over ASM, NAM and WAM confirm similar transport. Our analysis shows that a 10 % change in Asian emissions transports ~ 5–30 ppt of PAN in the UTLS over Asia, ~ 1–10 ppt of PAN in the UTLS of northern subtropics and mid-latitudes, ~ 7–10 ppt of HNO3 and ~ 1–2 ppb of ozone in UT over Asia. Comparison of emission change over Asia, North America and Africa shows that the highest transport of HNO3 and ozone occurs in the UT over Asia and least over Africa. The intense convective activity in the monsoon regions is associated with lightning and thereby the formation of additional NOx. This also affects the distribution of PAN in the UTLS. Simulations with and without lightning show an increase in the concentrations of PAN (~ 40 %), HNO3 (75 %), NOx (70 %) and ozone (30 %) over the regions of convective transport. Lightning-induced production of these species is higher over equatorial Africa and America compared to the ASM region. This indicates that the contribution of anthropogenic emissions to PAN in the UTLS over the ASM is higher than that of lightning.

Atmospheric pollution over South Asia attracts special attention due to its effects on regional climate, the water cycle, and human health. These effects are potentially growing owing to rising trends of anthropogenic aerosol emissions found there. In this study, the spatio-temporal aerosol distributions over South Asia from 7 global models, for the period of 2000–2007, are evaluated systematically against aerosol retrievals of NASA satellite sensors and ground-based measurements. Overall, substantial underestimations of aerosol loading over South Asia are found systematically in 6 out of 7 models. Averaged over the entire South Asia, the annual mean Aerosol Optical Depth (AOD) is underestimated by a range of 18–45 % across models compared to MISR, which is the lowest bound among various satellite AOD retrievals (from MISR, SeaWiFS, MODIS Aqua and Terra). In particular at Kanpur located in northern India, AOD is underestimated even more by a factor of 4, and annual mean Aerosol Absorption Optical Depth (AAOD) is underestimated by about a factor of 2 in comparison with AERONET, during the post-monsoon and the wintertime periods (i.e. October–January) when agricultural waste burning and anthropogenic emissions dominate. The largest model underestimation of aerosol loading occurs in the lowest boundary layer (from surface to 2 km) based on the comparisons with aerosol extinction vertical distribution from CALIPSO. The possible causes for the common problems of model aerosol underestimation over south Asia are identified here, which are suggested as the following. During the winter, not only the columnar aerosol loading in models, but also surface concentrations of all aerosol components (sulfate, nitrate, organic aerosol and black carbon) are found lower than observations (ISRO-GBP, ICARB and CALIPSO), indicating that anthropogenic emissions, especially biofuel, are likely underestimated in this season. Nitrate, a major component of aerosols in South Asia, is either not considered in 4 out of 7 models or significantly lower than observations in other 2 models. Surprisingly, the near-surface relative humidity in these models is found significantly lower than observations in the winter, resulting in suppression of the hygroscopic growth of soluble aerosols and formations of sulfate and nitrate, and thereby underestimation of AOD. During the post-monsoon season, the deficiency of agricultural waste burning emissions in GFED2 biomass burning emission inventory, used by the models, partly contributes to the model underestimation of aerosol loading over South Asia in burning seasons.

International audience; This study evaluates model-simulated dust aerosols over North Africa and the North Atlantic from five global models that participated in the Aerosol Comparison between Observations and Models phase II model experiments. The model results are compared with satellite aerosol optical depth (AOD) data from Moderate Resolution Imaging Spectroradiometer (MODIS), Multiangle Imaging Spectroradiometer (MISR), and Sea-viewing Wide Field-of-view Sensor, dust optical depth (DOD) derived from MODIS and MISR, AOD and coarse-mode AOD (as a proxy of DOD) from ground-based Aerosol Robotic Network Sun photometer measurements, and dust vertical distributions/centroid height from Cloud Aerosol Lidar with Orthogonal Polarization and Atmospheric Infrared Sounder satellite AOD retrievals. We examine the following quantities of AOD and DOD: (1) the magnitudes over land and over ocean in our study domain, (2) the longitudinal gradient from the dust source region over North Africa to the western North Atlantic, (3) seasonal variations at different locations, and (4) the dust vertical profile shape and the AOD centroid height (altitude above or below which half of the AOD is located). The different satellite data show consistent features in most of these aspects; however, the models display large diversity in all of them, with significant differences among the models and between models and observations. By examining dust emission, removal, and mass extinction efficiency in the five models, we also find remarkable differences among the models that all contribute to the discrepancies of model-simulated dust amount and distribution. This study highlights the challenges in simulating the dust physical and optical processes, even in the best known dust environment, and stresses the need for observable quantities to constrain the model processes. Key Points North African dust is studied using observations and models Observations agree in the magnitude, distribution, and seasonality of dust Models show large differences to observations and they show large diversity ©2014. American Geophysical Union. All Rights Reserved.

This paper evaluates the current status of global modeling of the organic aerosol (OA) in the troposphere and analyzes the differences between models as well as between models and observations. Thirty-one global chemistry transport models (CTMs) and general circulation models (GCMs) have participated in this intercomparison, in the framework of AeroCom phase II. The simulation of OA varies greatly between models in terms of the magnitude of primary emissions, secondary OA (SOA) formation, the number of OA species used (2 to 62), the complexity of OA parameterizations (gas-particle partitioning, chemical aging, multiphase chemistry, aerosol microphysics), and the OA physical, chemical and optical properties. The diversity of the global OA simulation results has increased since earlier AeroCom experiments, mainly due to the increasing complexity of the SOA parameterization in models, and the implementation of new, highly uncertain, OA sources. Diversity of over one order of magnitude exists in the modeled vertical distribution of OA concentrations that deserves a dedicated future study. Furthermore, although the OA / OC ratio depends on OA sources and atmospheric processing, and is important for model evaluation against OA and OC observations, it is resolved only by a few global models. The median global primary OA (POA) source strength is 56 Tg a−1 (range 34–144 Tg a−1) and the median SOA source strength (natural and anthropogenic) is 19 Tg a−1 (range 13–121 Tg a−1). Among the models that take into account the semi-volatile SOA nature, the median source is calculated to be 51 Tg a−1 (range 16–121 Tg a−1), much larger than the median value of the models that calculate SOA in a more simplistic way (19 Tg a−1; range 13–20 Tg a−1, with one model at 37 Tg a−1). The median atmospheric burden of OA is 1.4 Tg (24 models in the range of 0.6–2.0 Tg and 4 between 2.0 and 3.8 Tg), with a median OA lifetime of 5.4 days (range 3.8–9.6 days). In models that reported both OA and sulfate burdens, the median value of the OA/sulfate burden ratio is calculated to be 0.77; 13 models calculate a ratio lower than 1, and 9 models higher than 1. For 26 models that reported OA deposition fluxes, the median wet removal is 70 Tg a−1 (range 28–209 Tg a−1), which is on average 85% of the total OA deposition. Fine aerosol organic carbon (OC) and OA observations from continuous monitoring networks and individual field campaigns have been used for model evaluation. At urban locations, the model–observation comparison indicates missing knowledge on anthropogenic OA sources, both strength and seasonality. The combined model–measurements analysis suggests the existence of increased OA levels during summer due to biogenic SOA formation over large areas of the USA that can be of the same order of magnitude as the POA, even at urban locations, and contribute to the measured urban seasonal pattern. Global models are able to simulate the high secondary character of OA observed in the atmosphere as a result of SOA formation and POA aging, although the amount of OA present in the atmosphere remains largely underestimated, with a mean normalized bias (MNB) equal to −0.62 (−0.51) based on the comparison against OC (OA) urban data of all models at the surface, −0.15 (+0.51) when compared with remote measurements, and −0.30 for marine locations with OC data. The mean temporal correlations across all stations are low when compared with OC (OA) measurements: 0.47 (0.52) for urban stations, 0.39 (0.37) for remote stations, and 0.25 for marine stations with OC data. The combination of high (negative) MNB and higher correlation at urban stations when compared with the low MNB and lower correlation at remote sites suggests that knowledge about the processes that govern aerosol processing, transport and removal, on top of their sources, is important at the remote stations. There is no clear change in model skill with increasing model complexity with regard to OC or OA mass concentration. However, the complexity is needed in models in order to distinguish between anthropogenic and natural OA as needed for climate mitigation, and to calculate the impact of OA on climate accurately.

Sahara-originated dust is the most significant natural source of particulate matter; however, this contribution is still unclear in the Eastern Mediterranean especially in Western Turkey, where significant industrial sources and metropolitan areas are located. The Real-time Air Quality Modeling System (RAQMS) is utilized to explore the possible effects of Saharan dust on high levels of PM10 measured in Turkey. RAQMS model is compared with 118-air quality stations distributed throughout Turkey (81 cities) for April 2008. MODIS aerosol product (MOD04 for Terra and MYD04 for Aqua) is used to see columnar aerosol loading of the atmosphere at 550 nm (Aerosol optical depth (AOD) values found to be between 0.6 and 0.8 during the episode). High-resolution vertical profiles of clouds and aerosols are provided from CALIOP, on board of CALISPO satellite. The results suggest a significant contribution of Sahara dust to high levels of PM10 in Turkey with RAQMS and in situ time series showing similar patterns. The two data sets are found to be in agreement with a correlation of 0.87. (C) 2013 Elsevier B.V. All rights reserved.

International audience; Major gaseous and particulate pollutant levels over Europe in 2008 have been simulated using the offline-coupled WRFCMAQ chemistry and transport modeling system. The simulations are compared with surface observations from the EMEP stations, ozone (O3) soundings, ship-borne O3 and nitrogen dioxide (NO2) observations in the western Mediterranean, tropospheric NO2 vertical column densities from the SCIAMACHY instrument, and aerosol optical depths (AOD) from the AERONET. The results show that on average, surface O3 levels are underestimated by 4 to 7% over the northern European EMEP stations while they are overestimated by 7-10% over the southern European EMEP stations and underestimated in the tropospheric column (by 10-20%). Particulate matter (PM) mass concentrations are underestimated by up to 60%, particularly in southern and eastern Europe, suggesting underestimated PM sources. Larger differences are calculated for individual aerosol components, particularly for organic and elemental carbon than for the total PM mass, indicating uncertainty in the combustion sources. Better agreement has been obtained for aerosol species over urban areas of the eastern Mediterranean, particularly for nss-SO4 2, attributed to the implementation of higher quality emission inventories for that area. Simulated AOD levels are lower than the AERONET observations by 10% on average, with average underestimations of 3% north of 40°N, attributed to the low anthropogenic emissions in the model and 22% south of 40°N, suggesting underestimated natural and resuspended dust emissions. Overall, the results reveal differences in the model performance between northern and southern Europe, suggesting significant differences in the representation of both anthropogenic and natural emissions in these regions. Budget analyses indicate that O3 and peroxyacetyl nitrate (PAN) are transported from the free troposphere (FT) to the planetary boundary layer over Europe, while other species follow the reverse path and are then advected away from the source region. © 2013 Elsevier B.V.

An eight-member ensemble of ECHAM5-HAMMOZ simulations for a boreal summer season is analysed to study the transport of aerosols in the upper troposphere and lower stratosphere (UTLS) during the Asian summer monsoon (ASM). The simulations show persistent maxima in black carbon, organic carbon, sulfate, and mineral dust aerosols within the anticyclone in the UTLS throughout the ASM (period from July to September), when convective activity over the Indian subcontinent is highest, indicating that boundary layer aerosol pollution is the source of this UTLS aerosol layer. The simulations identify deep convection and the associated heat-driven circulation over the southern flanks of the Himalayas as the dominant transport pathway of aerosols and water vapour into the tropical tropopause layer (TTL). Comparison of model simulations with and without aerosols indicates that anthropogenic aerosols are central to the formation of this transport pathway. Aerosols act to increase cloud ice, water vapour, and temperature in the model UTLS. Evidence of ASM transport of aerosols into the stratosphere is also found, in agreement with aerosol extinction measurements from the Halogen Occultation Experiment (HALOE) and Stratospheric Aerosol and Gas Experiment (SAGE) II. As suggested by the observations, aerosols are transported into the Southern Hemisphere around the tropical tropopause by large-scale mixing processes. Aerosol-induced circulation changes also include a weakening of the main branch of the Hadley circulation and a reduction of monsoon precipitation over India.

An eight member ensemble of ECHAM5-HAMMOZ simulations for the year 2003 is analyzed to study the transport of aerosols in the Upper Troposphere and Lower Stratosphere (UTLS) during the Asian Summer Monsoon (ASM). Simulations show persistent maxima in black carbon, organic carbon, sulfate, and mineral dust aerosols within the anticyclone in the UTLS throughout the ASM (period from July to September) when convective activity over the Indian subcontinent is highest. Model simulations indicate boundary layer aerosol pollution as the source of this UTLS aerosol layer and identify ASM convection as the dominant transport process. Evidence of ASM transport of aerosols into the stratosphere is observed in HALogen Occultation Experiment (HALOE) and Stratospheric Aerosol and Gas Experiment (SAGE) II aerosol extinction. The impact of aerosols in the UTLS region is analyzed by evaluating the differences between simulations with (CTRL) and without aerosol (HAM-off) loading. The transport of anthropogenic aerosols in the UTLS increases cloud ice, water vapour and temperature, indicating that aerosols play an important role in enhancement of cloud ice in the Upper-Troposphere (UT). Aerosol induced circulation changes include a weakening of the main branch of the Hadley circulation and increased vertical transport around the southern flank of the Himalayas and reduction in monsoon precipitation over the India region.

Tropospheric ozone and black carbon (BC) contribute to both degraded air quality and global warming. We considered ~400 emission control measures to reduce these pollutants by using current technology and experience. We identified 14 measures targeting methane and BC emissions that reduce projected global mean warming ~0.5°C by 2050. This strategy avoids 0.7 to 4.7 million annual premature deaths from outdoor air pollution and increases annual crop yields by 30 to 135 million metric tons due to ozone reductions in 2030 and beyond. Benefits of methane emissions reductions are valued at $700 to $5000 per metric ton, which is well above typical marginal abatement costs (less than $250). The selected controls target different sources and influence climate on shorter time scales than those of carbon dioxide–reduction measures. Implementing both substantially reduces the risks of crossing the 2°C threshold., JRC.H.2-Air and Climate

Understanding historical trends of trace gas and aerosol distributions in the troposphere is essential to evaluate the efficiency of the existing strategies to reduce air pollution and to design more efficient future air quality and climate policies. We per- formed coupled photochemistry and aerosol microphysics simulations for the period 1980¿2005 using the aerosol-chemistry-climate model ECHAM5-HAMMOZ, to assess our understanding of long term changes and inter-annual variability of the chemical composition of the troposphere, and in particular of O3 and sulphate concentrations, for which long-term surface observations are available. In order to separate the impact of the anthropogenic emissions and meteorology on atmospheric chemistry, we compare two model experiments, driven by the same ECMWF re-analysis data, but with varying and constant anthropogenic emissions, respectively. Our model analysis indicates an average increase of 1 ppbv (corresponding to 0.04 ppbv yr-1) in global average surface O3 concentrations due to anthropogenic emissions, but this trend is largely masked by natural variability (0.63 ppbv), corresponding to 75% of the total variability (0.83 ppbv). Regionally, annual mean surface O3 concentrations increased by 1.3 and 1.6 ppbv over Europe and North America, respectively, despite the large anthropogenic emission reductions between 1980 and 2005. A comparison of winter and summer O3 trends with measurements shows a qualitative agreement, except in North America, where our model erroneously computed a positive trend. O3 increases of more than 4 ppbv in East Asia and 5 ppbv in South Asia can not be corroborated with long-term observations. Global average sulphate surface concentrations are largely controlled by anthropogenic emissions. Globally natural emissions are an important driver determining AOD variations, regionally AOD decreased by 28% over Europe, while it increased by 19% and 26% in East and South Asia. The global radiative perturbation calculated in our model for the period 1980¿2005 was rather small (0.05Wm-2 for O3 and 0.02Wm-2 for total aerosol direct effect), but larger perturbations ranging from -0.54 to 1.26Wm-2 are estimated in those regions where anthropogenic emissions largely varied., JRC.H.2-Air and Climate

The contribution of ocean dimethyl sulfide (DMS) emissions to changes in cloud microphysical properties is quantified seasonally and globally for present day climate conditions using an aerosol-chemistry-climate general circulation model, ECHAM5-HAMMOZ, coupled to a cloud microphysics scheme. We evaluate DMS aerosol-cloud-climate linkages over the southern oceans where anthropogenic influence is minimal. The changes in the number of activated particles, cloud droplet number concentration (CDNC), cloud droplet effective radius, cloud cover and the radiative forcing are examined by analyzing two simulations: a baseline simulation with ocean DMS emissions derived from a prescribed climatology and one in which the ocean DMS emissions are switched off. Our simulations show that the model realistically simulates the seasonality in the number of activated particles and CDNC, peaking during Southern Hemisphere (SH) summer coincident with increased phytoplankton blooms and gradually declining with a minimum in SH winter. In comparison to a simulation with no DMS, the CDNC level over the southern oceans is 128% larger in the baseline simulation averaged over the austral summer months. Our results also show an increased number of smaller sized cloud droplets during this period. We estimate a maximum decrease of up to 15–18% in the droplet radius and a mean increase in cloud cover by around 2.5% over the southern oceans during SH summer in the simulation with ocean DMS compared to when the DMS emissions are switched off. The global annual mean top of the atmosphere DMS aerosol all sky radiative forcing is −2.03 W/m2, whereas, over the southern oceans during SH summer, the mean DMS aerosol radiative forcing reaches −9.32 W/m2.