Aerosol Precursor Emissions Research Articles

Impact of aerosol emission controls on future Arctic sea ice cover

We examine the response of Arctic sea ice to projected aerosol and aerosol precursor emission changes under the Representative Concentration Pathway (RCP) scenarios in simulations of the Canadian Earth System Model. The overall decrease in aerosol loading causes a warming, largest over the Arctic, which leads to an annual mean reduction in sea ice extent of approximately 1 million km2 over the 21st century in all RCP scenarios. This accounts for approximately 25% of the simulated reduction in sea ice extent in RCP 4.5, and 40% of the reduction in RCP 2.5. In RCP 4.5, the Arctic ocean is projected to become ice-free during summertime in 2045, but it does not become ice-free until 2057 in simulations with aerosol precursor emissions held fixed at 2000 values. Thus, while reductions in aerosol emissions have significant health and environmental benefits, their substantial contribution to projected Arctic climate change should not be overlooked.

Development and application of the WRFPLUS-Chem online chemistry adjoint and WRFDA-Chem assimilation system

Abstract. Here we present the online meteorology and chemistry adjoint and tangent linear model, WRFPLUS-Chem (Weather Research and Forecasting plus chemistry), which incorporates modules to treat boundary layer mixing, emission, aging, dry deposition, and advection of black carbon aerosol. We also develop land surface and surface layer adjoints to account for coupling between radiation and vertical mixing. Model performance is verified against finite difference derivative approximations. A second-order checkpointing scheme is created to reduce computational costs and enable simulations longer than 6 h. The adjoint is coupled to WRFDA-Chem, in order to conduct a sensitivity study of anthropogenic and biomass burning sources throughout California during the 2008 Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) field campaign. A cost-function weighting scheme was devised to reduce the impact of statistically insignificant residual errors in future inverse modeling studies. Results of the sensitivity study show that, for this domain and time period, anthropogenic emissions are overpredicted, while wildfire emission error signs vary spatially. We consider the diurnal variation in emission sensitivities to determine at what time sources should be scaled up or down. Also, adjoint sensitivities for two choices of land surface model (LSM) indicate that emission inversion results would be sensitive to forward model configuration. The tools described here are the first step in conducting four-dimensional variational data assimilation in a coupled meteorology–chemistry model, which will potentially provide new constraints on aerosol precursor emissions and their distributions. Such analyses will be invaluable to assessments of particulate matter health and climate impacts.

Dominant role of greenhouse-gas forcing in the recovery of Sahel rainfall

Higher atmospheric greenhouse gases are shown to have driven the recovery of Sahelian rainfall since the 1980s. This study discounts the role of sea surface temperature changes that had previously been jointly credited as drivers of the recovery. Sahelian summer rainfall, controlled by the West African monsoon, exhibited large-amplitude multidecadal variability during the twentieth century. Particularly important was the severe drought of the 1970s and 1980s, which had widespread impacts1,2,3,4,5,6. Research into the causes of this drought has identified anthropogenic aerosol forcing3,4,7 and changes in sea surface temperatures (SSTs; refs 1, 2, 6, 8, 9, 10, 11) as the most important drivers. Since the 1980s, there has been some recovery of Sahel rainfall amounts2,3,4,5,6,11,12,13,14, although not to the pre-drought levels of the 1940s and 1950s. Here we report on experiments with the atmospheric component of a state-of-the-art global climate model to identify the causes of this recovery. Our results suggest that the direct influence of higher levels of greenhouse gases in the atmosphere was the main cause, with an additional role for changes in anthropogenic aerosol precursor emissions. We find that recent changes in SSTs, although substantial, did not have a significant impact on the recovery. The simulated response to anthropogenic greenhouse-gas and aerosol forcing is consistent with a multivariate fingerprint of the observed recovery, raising confidence in our findings. Although robust predictions are not yet possible, our results suggest that the recent recovery in Sahel rainfall amounts is most likely to be sustained or amplified in the near term.

Effects of declining aerosols on projections of zonally averaged tropical precipitation

All of the representative concentration pathways (RCPs) assume that future emissions of aerosols and aerosol precursors will decline sharply. There is considerable evidence that historically increasing aerosols have substantially affected tropical precipitation, but the effects of projected aerosol declines have received little attention. We compare projections forced by the medium-low RCP4.5 pathway in two subsets of models from the Coupled Model Intercomparison Project Phase 5 (CMIP5): one group (HiForc) includes treatments of indirect aerosol effects on cloud albedo and cloud lifetime as well as direct aerosol effects, while the other group (LoForc) only treats direct aerosol effects. In this scenario we find that models in the HiForc group consistently project larger increases in both the mean and inter-hemispheric (north minus south) asymmetry of tropical sea-surface temperature (SST) and precipitation than do models in the LoForc group. Earlier projections from CMIP3, in which future aerosol declines were assumed to be smaller, behave more like the CMIP5 LoForc group. These results show that projected tropical SST and precipitation changes are sensitive to assumptions about aerosol emissions and indirect aerosol effects. If the real world resembles the HiForc group, then future aerosol changes are likely to be an important (even dominant) driver of tropical precipitation changes under low to moderate forcing scenarios.

High secondary aerosol contribution to particulate pollution during haze events in China.

Rapid industrialization and urbanization in developing countries has led to an increase in air pollution, along a similar trajectory to that previously experienced by the developed nations. In China, particulate pollution is a serious environmental problem that is influencing air quality, regional and global climates, and human health. In response to the extremely severe and persistent haze pollution experienced by about 800 million people during the first quarter of 2013 (refs 4, 5), the Chinese State Council announced its aim to reduce concentrations of PM2.5 (particulate matter with an aerodynamic diameter less than 2.5micrometres) by up to 25 per cent relative to 2012 levels by 2017 (ref. 6). Such efforts however require elucidation of the factors governing the abundance and composition of PM2.5, which remain poorly constrained in China. Here we combine a comprehensive set of novel and state-of-the-art offline analytical approaches and statistical techniques to investigate the chemical nature and sources of particulate matter at urban locations in Beijing, Shanghai, Guangzhou and Xi'an during January 2013. We find that the severe haze pollution event was driven to a large extent by secondary aerosol formation, which contributed 30-77 per cent and 44-71 per cent (average for all four cities) of PM2.5 and of organic aerosol, respectively. On average, the contribution of secondary organic aerosol (SOA) and secondary inorganic aerosol (SIA) are found to be of similar importance (SOA/SIA ratios range from 0.6 to 1.4). Our results suggest that, in addition to mitigating primary particulate emissions, reducing the emissions of secondary aerosol precursors from, for example, fossil fuel combustion and biomass burning is likely to be important for controlling China's PM2.5 levels and for reducing the environmental, economic and health impacts resulting from particulate pollution.

Origin and sources of dissolved organic matter in snow on the East Antarctic ice sheet.

Polar ice sheets hold a significant pool of the world's carbon reserve and are an integral component of the global carbon cycle. Yet, organic carbon composition and cycling in these systems is least understood. Here, we use ultrahigh resolution mass spectrometry to elucidate, at an unprecedented level, molecular details of dissolved organic matter (DOM) in Antarctic snow. Tens of thousands of distinct molecular species are identified, providing clues to the nature and sources of organic carbon in Antarctica. We show that many of the identified supraglacial organic matter formulas are consistent with material from microbial sources, and terrestrial inputs of vascular plant-derived materials are likely more important sources of organic carbon to Antarctica than previously thought. Black carbon-like material apparently originating from biomass burning in South America is also present, while a smaller fraction originated from soil humics and appears to be photochemically or microbially modified. In addition to remote continental sources, we document signals of oceanic emissions of primary aerosols and secondary organic aerosol precursors. The new insights on the diversity of organic species in Antarctic snowpack reinforce the importance of studying organic carbon associated with the Earth's polar regions in the face of changing climate.

Impacts of land use and land cover changes on biogenic emissions of volatile organic compounds in China from the late 1980s to the mid-2000s: implications for tropospheric ozone and secondary organic aerosol

Based on the MEGAN (Model of Emissions of Gases and Aerosols from Nature) module embedded within the global chemical transport model (GEOS-Chem), we estimate the changes in emissions of biogenic volatile organic compounds (BVOCs) and their impacts on surface-layer O3 and secondary organic aerosols (SOA) in China between the late 1980s and the mid-2000s by using the land cover dataset derived from remote sensing images and land use survey. The land cover change in China from the late 1980s to the mid-2000s can be characterised by an expansion of urban areas (the total urban area in the mid-2000s was four times that in the late 1980s) and a reduction in total vegetation coverage by 4%. Regionally, the fractions of land covered by forests exhibited increases in southeastern and northeastern China by 10–30 and 5–15%, respectively, those covered by cropland decreased in most regions except that the farming–pastoral zone in northern China increased by 5–20%, and the factions of grassland in northern China showed a large reduction of 5–30%. With changes in both land cover and meteorological fields, annual BVOC emission in China is estimated to increase by 11.4% in the mid-2000s relative to the late 1980s. With anthropogenic emissions of O3 precursors, aerosol precursors and aerosols fixed at year 2005 levels, the changes in land cover and meteorological parameters from the late 1980s to the mid-2000s are simulated to change the seasonal mean surface-layer O3 concentrations by −4 to +6 ppbv (−10 to +20%) and to change the seasonal mean surface-layer SOA concentrations by −0.4 to +0.6 µg m−3 (−20 to +30%) over China. We find that the decadal changes in meteorological parameters had larger collective effects on BVOC emissions and surface-layer concentrations of O3 and SOA than those in land cover and land use alone. We also perform a sensitivity simulation to compare the impacts of changes in anthropogenic emissions on concentrations of O3 and SOA with those of the changes in meteorological parameters and land cover.

Determination of the uncertainties of the German emission inventories for particulate matter and aerosol precursors using Monte-Carlo analysis

This paper presents the application of a Monte-Carlo simulation for assessing the uncertainties of German 2005 emissions of particulate matter (PM10 & PM2.5) and aerosol precursors (SO2, NOx, NH3 and NMVOC) carried out in the PAREST (PArticle REduction STrategies) research project. For the uncertainty analysis the German Federal Environment Agency’s emission inventory was amended and integrated with a model on the disaggregation of energy balance data. A series of algorithms was developed in order to make efficient and pragmatic use of available literature and expert judgement data for uncertainties of emission model input data. The inventories for PM10 (95 %-confidence interval: −16 %/+ 23 %), PM2.5 (−15 %/+19 %) and NOx (−10 %/+23 %) appear most uncertain, while the inventories for SO2 (−9 %/+9 %), NMVOC (−10 %/+12 %) and NH3 (−13 %/+13 %) show a higher accuracy. The source categories adding the most relevant contributions to overall uncertainty vary across the pollutants and comprise agriculture, mobile machinery in agriculture and forestry, construction sites, small businesses/carpentries, cigarette smoke and fireworks, road traffic, solvent use and stationary combustion. The PAREST results on relative uncertainties have been quoted in the German Informative Inventory Reports since 2012. A comparison shows that the PAREST results for Germany are within the range of (for NH3: close below) other European countries’ results on air pollutant inventory uncertainties as reported in the 2013 Informative Inventory Reports.

Assessing remote polarimetric measurement sensitivities to aerosol emissions using the geos-chem adjoint model

Abstract. Uncertainties in aerosol sources, microphysical properties, and global distributions undermine efforts to evaluate the radiative impacts of atmospheric aerosols. In this work, we investigate the feasibility of using remote polarimetric measurements for constraining aerosol and aerosol precursor emissions in light of these uncertainties. A model that incorporates a radiative transfer model with forward and adjoint chemical transport models has been applied to quantify the sensitivity of the reflectance at the top of atmosphere over land to aerosol emissions and microphysical properties. A set of simulated satellite observations, one intensity based and one capable of polarimetric measurements, are used to illustrate differences in the assimilation potential between the two. It is found that the sensitivity of the polarized reflectance to aerosol and aerosol precursor emissions tends to be significantly higher than that of the intensity for cases of non-absorbing aerosols. This is true even when the polarimetric sampling scheme is spatially sparser than that of the intensity sampling. This framework allows us to quantify upper limits on the uncertainties in the aerosol microphysical properties for which a 50% change in aerosol emissions is detectable using these simulated observations. It was found that although typical current remote sensing instrumentation provides retrievals of the refractive index and effective radius with accuracies within acceptable limits to detect a 50% change in emissions, retrievals of the effective variance contain uncertainties too large to detect these changes in emissions. These results may guide new applications of polarimetric measurements to constrain aerosol sources, and thus reduce uncertainty in our broader understanding of the impacts of aerosols on climate.

A steady-state analysis of the temperature responses of water vapor and aerosol lifetimes

Abstract. The dominant removal mechanism of soluble aerosol is wet deposition. The atmospheric lifetime of aerosol, relevant for aerosol radiative forcing, is therefore coupled to the atmospheric cycling time of water vapor. This study investigates the coupling between water vapor and aerosol lifetimes in a well-mixed atmosphere. Based on a steady-state study by Pruppacher and Jaenicke (1995) we describe the coupling in terms of the processing efficiency of air by clouds and the efficiencies of water vapor condensation, of aerosol activation, and of the transfer from cloud water to precipitation. We extend this to expressions for the temperature responses of the water vapor and aerosol lifetimes. Previous climate model results (Held and Soden, 2006) suggest a water vapor lifetime temperature response of +5.3 ± 2.0% K−1. This can be used as a first guess for the aerosol lifetime temperature response, but temperature sensitivities of the aerosol lifetime simulated in recent aerosol–climate model studies extend beyond this range and include negative values. This indicates that other influences probably have a larger impact on the computed aerosol lifetime than its temperature response, more specifically changes in the spatial distributions of aerosol (precursor) emissions and precipitation patterns, and changes in the activation efficiency of aerosol. These are not quantitatively evaluated in this study but we present suggestions for model experiments that may help to understand and quantify the different factors that determine the aerosol atmospheric lifetime.

The role of reduced aerosol precursor emissions in driving near-term warming

The representative concentration pathway (RCP) scenarios all assume stringent emissions controls on aerosols and their precursors, and hence include progressive decreases in aerosol and aerosol precursor emissions through the 21st century. Recent studies have suggested that the resultant decrease in aerosols could drive rapid near-term warming, which could dominate the effects of greenhouse gas (GHG) increases in the coming decades. In CanESM2 simulations, we find that under the RCP 2.6 scenario, which includes the fastest decrease in aerosol and aerosol precursor emissions, the contribution of aerosol reductions to warming between 2000 and 2040 is around 30%. Moreover, the rate of warming in the RCP 2.6 simulations declines gradually from its present-day value as GHG emissions decrease. Thus, while aerosol emission reductions contribute to gradual warming through the 21st century, we find no evidence that aerosol emission reductions drive particularly rapid near-term warming in this scenario. In the near-term, as in the long-term, GHG increases are the dominant driver of warming.

Constraints on aerosol sources using GEOS‐Chem adjoint and MODIS radiances, and evaluation with multisensor (OMI, MISR) data

We present a new top‐down approach that spatially constrains the amount of aerosol emissions using satellite (Moderate Resolution Imaging Spectroradiometer (MODIS)) observed radiances with the adjoint of a chemistry transport model (GEOS‐Chem). This paper aims to demonstrate the approach through applying it to a case study that yields the following emission estimates over China for April 2008: 1.73 Tg for SO2, 0.72 Tg for NH3, 1.38 Tg for NOx, 0.10 Tg for black carbon, and 0.18 Tg for organic carbon from anthropogenic sources, which reflects, respectively, a reduction of 33.5%, 34.5%, 18.8%, 9.1%, and 15% in comparison to the prior bottom‐up inventories of INTEX‐B 2006. The mineral dust emission from the online dust entrainment and mobilization module is reduced by 56.4% of 19.02 to 8.30 Tg. Compared to the prior simulation, the posterior simulation shows a much better agreement with the following independent measurements: aerosol optical depth (AOD) measured by AERONET sun‐spectrophotometers and retrieved from Multi‐angle Imaging SpectroRadiometer (MISR), atmospheric NO2 and SO2 columnar amount retrieved from Ozone Monitoring Instrument (OMI), and in situ data of sulfate‐nitrate‐ammonium and PM10 (particular matter with aerodynamic diameter less than 10 µm) mass concentrations over both anthropogenic pollution and dust source regions. Assuming the bottom‐up (prior) anthropogenic emissions are the best estimates for their base year of 2006, the overwhelming reduction in the posterior (top‐down) estimate indicates less emission in April 2008 especially for the SO2 tracer in the central and eastern parts of China, and/or an overestimation in the prior emission. The former is supported by the AOD change detected by MODIS and MISR sensors, while the latter is likely the case for NOx and NH3 emissions because no evidence shows that their atmospheric concentration has declined over China. With the promising results shown in this study, continuous efforts are needed toward a holistic and comprehensive inversion of emission using multisensor remote sensing data (of trace gases and aerosols) for constraining aerosol primary and precursor emissions at various temporal and spatial scales.

Using a global aerosol model adjoint to unravel the footprint of spatially‐distributed emissions on cloud droplet number and cloud albedo

The adjoints of the GEOS‐Chem Chemical Transport Model and a comprehensive cloud droplet parameterization are coupled to study the sensitivity of cloud droplet number concentration (Nd) over US regions and Central Europe to global emissions of anthropogenic fine mode aerosol precursors. Simulations reveal that the Nd over the midwestern and southeastern US is mostly sensitive to SO2 emissions during August, and to NH3 emissions during February. Over the western US, Nd is mostly sensitivity to SO2 and primary organic aerosol emissions. In Central Europe, Nd is most sensitive to NH3 and NOx emissions. As expected, local emissions strongly affect Nd; long‐range transport, however, is also important for the western US and Europe. Emissions changes projected for the year 2050 are estimated to have the largest impacts on cloud albedo andNd over Central Europe during August (42% and 82% change, respectively) and western US during February (12% and 36.5% change, respectively).

Trend analysis in aerosol optical depths and pollutant emission estimates between 2000 and 2009

We evaluated global and regional aerosol optical depth (AOD) trends in view of aerosol (precursor) emission changes between 2000 and 2009. We used AOD data products from MODIS, MISR and AERONET and emission estimates from the EMEP, REAS and IPCC inventories. The trends in global monthly AOD of MODIS (L3), MISR (L3) and AERONET (L2) are significantly negative over Europe and North America, whereas over South and East Asia they are mostly positive. The calculated 2000e2009 trends from the monthly L3 products correspond well with the more detailed daily MODIS L2 AODs for three selected regions (Central Mediterranean, North-East America and East Asia). Furthermore, daily and monthly AERONET L2 AOD trends agree well. The trends in AOD are compared to estimated emission changes of SO2 ,N Ox ,N H3 and black carbon. We associate the downward trends in AOD over Europe and North America with decreasing emissions of SO2 ,N Ox and other pollutants. Over East Asia the MODIS L2 trends are generally positive, consistent with increasing pollutant emissions by fossil energy use and growing industrial and urban activities. It appears that SO2 emission changes dominate the AOD trends, although especially in Asia NOx emissions may become increasingly important. Our results suggest that solar brightening due to decreasing SO2 emissions and the resulting downward AOD trends over Europe may have weakened in the 2000s compared to the 1990s.

Future projections of surface UV-B in a changing climate

[1] Results of comprehensive long-term simulations of surface all-sky and clear-sky ultraviolet (UV) radiation through 1960–2100 are presented. A new earth system model, MIROC-ESM-CHEM, is used for the simulation, which considers key processes that change the surface UV radiation: atmospheric dynamics and chemistry affecting ozone in the stratosphere and troposphere, aerosols and clouds in the troposphere, and changes in surface albedo with sea ice and snow cover. In contrast to previous assessments considering only the effect of long-term change in stratospheric ozone, the simulated long-term behavior of UV radiation in this study is strongly affected by other processes. In one of two simulations, all-sky UV radiation in the northern midlatitudes is projected to increase in the 21st century despite the expected recovery of the stratospheric ozone layer. Reductions in aerosols and clouds are expected to overcompensate for the effect of ozone recovery. The results are sensitive to the future socioeconomic scenario, describing GHG concentrations and emissions of aerosol and ozone precursors in the troposphere. The interannual variability of UV radiation associated with the 11 year solar cycle and local processes is also discussed.

Aerosol modelling in Europe with a focus on Switzerland during summer and winter episodes

Abstract. This paper describes aerosol modelling in Europe with a focus on Switzerland during summer and winter periods. We modelled PM2.5 (particles smaller than 2.5 μm in aerodynamic diameter) for one summer and two winter periods in years 2006 and 2007 using the CAMx air quality model. The meteorological fields were obtained from MM5 simulations. The modelled wind speeds during some low-wind periods, however, had to be calibrated with measurements to use realistic input for the air quality model. The detailed AMS (aerosol mass spectrometer) measurements at specific locations were used to evaluate the model results. In addition to the base case simulations, we carried out sensitivity tests with modified aerosol precursor emissions, air temperature and deposition. Aerosol concentrations in winter 2006 were twice as high as those in winter 2007, however, the chemical compositions were similar. CAMx could reproduce the relative composition of aerosols very well both in the winter and summer periods. Absolute concentrations of aerosol species were underestimated by about 20 %. Both measurements and model results suggest that organic aerosol (30–38 %) and particulate nitrate (30–36 %) are the main aerosol components in winter. In summer, organic aerosol dominates the aerosol composition (55–57 %) and is mainly of secondary origin. The contribution of biogenic volatile organic compound (BVOC) emissions to the formation of secondary organic aerosol (SOA) was predicted to be very large (>95 %) in Switzerland. The main contributors to the modelled SOA concentrations were oxidation products of monoterpenes and sesquiterpenes as well as oligomerization of oxidized compounds. The fraction of primary organic aerosol (POA) derived from measurements was lower than the model predictions indicating the importance of volatility of POA, which has not yet been taken into account in CAMx. Sensitivity tests with reduced NOx and NH3 emissions suggest that aerosol formation is more sensitive to ammonia emissions in winter in a large part of Europe. In Switzerland however, aerosol formation is predicted to be NOx-sensitive. In summer, effects of NOx and NH3 emission reductions on aerosol concentrations are predicted to be lower mostly due to lower ammonium nitrate concentrations. In general, the sensitivity to NH3 emissions is weaker in summer due to higher NH3 emissions.

Ultrafine particle formation in the inland sea breeze airflow in Southwest Europe

Abstract. Studies on ultrafine particles (diameter < 100nm) and air quality have mostly focused on vehicle exhaust emissions and on new particle formation in "clean" ambient air. Here we present a study focused on the processes contributing to ultrafine particle concentrations in a city (Huelva, SW Spain) placed close to a coastal area where significant anthropogenic emissions of aerosol precursors occur. The overall data analysis shows that two processes predominantly contribute to the number of particles coarser than 2.5 nm: vehicle exhaust emissions and new particle formation due to photo-chemical activity. As typically occurs in urban areas, vehicle exhaust emissions result in high concentrations of black carbon (BC) and particles coarser than 2.5 nm (N) during the morning rush hours. The highest N concentrations were recorded during the 11:00–17:00 h period, under the sea breeze regime, when low BC concentrations were registered and photochemical activity resulted in high O3 levels and in new particle formation in the aerosol precursors' rich inland airflow. In this period, it is estimated that about 80% of the number of particles are linked to sulfur dioxide emissions. The contributions to N of "carbonaceous material and those compounds nucleating/condensing immediately after emission" and of the "new particle formation processes in air masses rich gaseous precursors (e.g. SO2)" were estimated by means of a relatively novel method based on simultaneous measurements of BC and N. A comparison with two recent studies suggests that the daily cycles of "new particle formation" during the inland sea breeze is blowing period seem to be a feature of ultrafine particles in coastal areas of South-west Europe.

Simplified aerosol modeling for variational data assimilation

Abstract. We have developed a simplified aerosol model together with its tangent linear and adjoint versions for the ultimate aim of optimizing global aerosol and aerosol precursor emission using variational data assimilation. The model was derived from the general circulation model LMDz; it groups together the 24 aerosol species simulated in LMDz into 4 species, namely gaseous precursors, fine mode aerosols, coarse mode desert dust and coarse mode sea salt. The emissions have been kept as in the original model. Modifications, however, were introduced in the computation of aerosol optical depth and in the processes of sedimentation, dry and wet deposition and sulphur chemistry to ensure consistency with the new set of species and their composition. The simplified model successfully manages to reproduce the main features of the aerosol distribution in LMDz. The largest differences in aerosol load are observed for fine mode aerosols and gaseous precursors. Differences between the original and simplified models are mainly associated to the new deposition and sedimentation velocities consistent with the definition of species in the simplified model and the simplification of the sulphur chemistry. Furthermore, simulated aerosol optical depth remains within the variability of monthly AERONET observations for all aerosol types and all sites throughout most of the year. Largest differences are observed over sites with strong desert dust influence. In terms of the daily aerosol variability, the model is less able to reproduce the observed variability from the AERONET data with larger discrepancies in stations affected by industrial aerosols. The simplified model however, closely follows the daily simulation from LMDz. Sensitivity analyses with the tangent linear version show that the simplified sulphur chemistry is the dominant process responsible for the strong non-linearity of the model.

Anthropogenic and natural contributions to regional trends in aerosol optical depth, 1980–2006

Understanding the roles of human and natural sources in contributing to aerosol concentrations around the world is an important step toward developing efficient and effective mitigation measures for local and regional air quality degradation and climate change. In this study we test the hypothesis that changes in aerosol optical depth (AOD) over time are caused by the changing patterns of anthropogenic emissions of aerosols and aerosol precursors. We present estimated trends of contributions to AOD for eight world regions from 1980 to 2006, built upon a full run of the Goddard Chemistry Aerosol Radiation and Transport model for the year 2001, extended in time using trends in emissions of man‐made and natural sources. Estimated AOD trends agree well (R > 0.5) with observed trends in surface solar radiation in Russia, the United States, south Asia, southern Africa, and East Asia (before 1992) but less well for Organization for Economic Co‐operative Development (OECD) Europe (R < 0.5). The trends do not agree well for southeast Asia and for East Asia (after 1992) where large‐scale inter‐ and intraannual variations in emissions from forest fires, volcanic eruptions, and dust storms confound our approach. Natural contributions to AOD, including forest and grassland fires, show no significant long‐term trends (<1%/a), except for a small increasing trend in OECD Europe and a small decreasing trend in South America. Trends in man‐made contributions to AOD follow the changing patterns of industrial and economic activity. We quantify the average contributions of key source types to regional AOD over the entire time period.

Transport impacts on atmosphere and climate: Shipping

Emissions of exhaust gases and particles from oceangoing ships are a significant and growing contributor to the total emissions from the transportation sector. We present an assessment of the contribution of gaseous and particulate emissions from oceangoing shipping to anthropogenic emissions and air quality. We also assess the degradation in human health and climate change created by these emissions. Regulating ship emissions requires comprehensive knowledge of current fuel consumption and emissions, understanding of their impact on atmospheric composition and climate, and projections of potential future evolutions and mitigation options. Nearly 70% of ship emissions occur within 400 km of coastlines, causing air quality problems through the formation of ground-level ozone, sulphur emissions and particulate matter in coastal areas and harbours with heavy traffic. Furthermore, ozone and aerosol precursor emissions as well as their derivative species from ships may be transported in the atmosphere over several hundreds of kilometres, and thus contribute to air quality problems further inland, even though they are emitted at sea. In addition, ship emissions impact climate. Recent studies indicate that the cooling due to altered clouds far outweighs the warming effects from greenhouse gases such as carbon dioxide (CO 2) or ozone from shipping, overall causing a negative present-day radiative forcing (RF). Current efforts to reduce sulphur and other pollutants from shipping may modify this. However, given the short residence time of sulphate compared to CO 2, the climate response from sulphate is of the order decades while that of CO 2 is centuries. The climatic trade-off between positive and negative radiative forcing is still a topic of scientific research, but from what is currently known, a simple cancellation of global mean forcing components is potentially inappropriate and a more comprehensive assessment metric is required. The CO 2 equivalent emissions using the global temperature change potential (GTP) metric indicate that after 50 years the net global mean effect of current emissions is close to zero through cancellation of warming by CO 2 and cooling by sulphate and nitrogen oxides.