Search

This study focuses on implications of differences between recent global emissions inventories for simulated trends in anthropogenic aerosol abundances and radiative forcing (RF) over the 1990–2019 period. We use the ECLIPSE version 6 (ECLv6) and CEDS year 2021 release (CEDS21) as input to the chemical transport model OsloCTM3 and compare the resulting aerosol evolution to corresponding results derived with the first CEDS release, as well as to observed trends in regional and global aerosol optical depth (AOD). Using CEDS21 and ECLv6 results in a 3 % and 6 % lower global mean AOD compared to CEDS in 2014, primarily driven by differences over China and India, where the area average AOD is up to 30 % lower. These differences are considerably larger than the satellite-derived interannual variability in AOD. A negative linear trend over 2005–2017 in global AOD following changes in anthropogenic emissions is found with all three inventories but is markedly stronger with CEDS21 and ECLv6. Furthermore, we confirm that the model better captures the sign and strength of the observed AOD trend over China with CEDS21 and ECLv6 compared to using CEDS, while the opposite is the case for South Asia. We estimate a net global mean aerosol-induced RF in 2014 relative to 1990 of 0.08 W m−2 for CEDS21 and 0.12 W m−2 for ECLv6, compared to 0.03 W m−2 with CEDS. Using CEDS21, we also estimate the RF in 2019 relative to 1990 to be 0.10 W m−2, reflecting the continuing decreasing trend in aerosol loads post-2014. Our results facilitate more rigorous comparison between existing and upcoming studies of climate and health effects of aerosols using different emission inventories.

Heterogeneous ice formation on aerosols is the main primary cloud ice formation process above temperatures of -38°C, and asa consequence it plays a major role in the formation of mixed-phase and ice clouds. Improving our understanding of iceprocesses could help better constrain the radiative forcing of cloud aerosol interactions, which remains a major source ofuncertainty in climate projections. Despite their importance, most atmospheric models do not represent aerosol-cloud iceprocesses explicitly.We extend in the WRF-Chem 3.9.1 model a recent parameterization of deposition-mode ice nucleation to also includeimmersion-mode nucleation, based on the classical nucleation theory (CNT) description. We also couple this parameterizationwith the aerosol-liquid cloud parameterization of Abdul Razzak and Ghan already included in WRF-Chem 3.9.1. This allows us tomodel the effect of aerosols on mixed-phase and ice clouds. We use volcanic eruptions as case studies, especially focusing onthe 2014/2015 Holuhraun/Bárðarbunga eruption in Iceland. Specifically, we investigate how volcanic aerosols influencemodeled cloud microphysical properties with and without the explicit ice nucleation parameterization, comparing the modelagainst MODIS satellite observations. We also investigate the effect of these processes on the cloud response in terms ofoptical properties, radiative fluxes, and precipitation during the eruptions

ETIN-MIP is a community-wide effort to improve dynamical understanding of the linkages between tropical precipitation and radiative biases in various regions, with implications for anthropogenic climate change and geoengineering.This article introduces the Extratropical-Tropical Interaction Model Intercomparison Project (ETIN-MIP), where a set of fully coupled model experiments are designed to examine the sources of longstanding tropical precipitation biases in climate models. In particular, we reduce insolation over three targeted latitudinal bands of persistent model biases: the southern extratropics, the southern tropics and the northern extratropics. To address the effect of regional energy bias corrections on the mean distribution of tropical precipitation, such as the double Intertropical Convergence Zone problem, we evaluate the quasi-equilibrium response of the climate system corresponding to a 50-year period after the 100 years of prescribed energy perturbation. Initial results show that, despite a large inter-model spread in each perturbation experiment due to differences in ocean heat uptake response and climate feedbacks across models, the southern tropics is most efficient at driving a meridional shift of tropical precipitation. In contrast, the extratropical energy perturbations are effectively damped by anomalous heat uptake over the subpolar oceans, thereby inducing a smaller meridional shift of tropical precipitation compared with the tropical energy perturbations. The ETIN-MIP experiments allow us to investigate the global implications of regional energy bias corrections, providing a route to guide the practice of model development, with implications for understanding dynamical responses to anthropogenic climate change and geoengineering.

Anthropogenic aerosol emissions over Asia are changing rapidly, both in composition and spatial distribution1. The Shared Socioeconomic Pathways (SSPs), potential narratives of development used by the Intergovernmental Panel for Climate Change in future projections, span a range of influences of aerosols on climate over the next decades. Several of these narratives project the continuation of a trend manifested in observations since 2010, with a clear dipole between South and East Asia. \ud \ud The patterns of radiative forcing that result from these distributions of aerosols will differ from those of the late 20th century. They may instigate large-scale atmospheric responses that could have wide ranging impacts on climate and society well beyond the aerosol source regions. South and East Asia are particularly vulnerable to climate change because of strong seasonal variations in precipitation, high average temperature, and very high population density. Therefore, any aerosol impacts on the strength or seasonal variations in monsoon rainfall, freshwater availability, or climate extremes, will incur large societal costs. We urge the scientific community to make definite progress towards understanding and quantifying the impacts of Asian aerosols and to tackle the potentially large regional and hemispheric implications of these emerging trends.

Atmospheric methane grew very rapidly in 2014 (12.7±0.5 ppb/yr), 2015 (10.1±0.7 ppb/yr), 2016 (7.0± 0.7 ppb/yr) and 2017 (7.7±0.7 ppb/yr), at rates not observed since the 1980s. The increase in the methane burden began in 2007, with the mean global mole fraction in remote surface background air rising from about 1775 ppb in 2006 to 1850 ppb in 2017. Simultaneously the 13C/12C isotopic ratio (expressed as δ13CCH4) has shifted, in a new trend to more negative values that have been observed worldwide for over a decade. The causes of methane's recent mole fraction increase are therefore either a change in the relative proportions (and totals) of emissions from biogenic and thermogenic and pyrogenic sources, especially in the tropics and sub‐tropics, or a decline in the atmospheric sink of methane, or both. Unfortunately, with limited measurement data sets, it is not currently possible to be more definitive. The climate warming impact of the observed methane increase over the past decade, if continued at >5 ppb/yr in the coming decades, is sufficient to challenge the Paris Agreement, which requires sharp cuts in the atmospheric methane burden. However, anthropogenic methane emissions are relatively very large and thus offer attractive targets for rapid reduction, which are essential if the Paris Agreement aims are to be attained.

Future projections of east Amazonian precipitation indicate drying, but they are uncertain and poorly understood. In this study we analyze the Amazonian precipitation response to individual atmospheric forcings using a number of global climate models. Black carbon is found to drive reduced precipitation over the Amazon due to temperature-driven circulation changes, but the magnitude is uncertain. CO2 drives reductions in precipitation concentrated in the east, mainly due to a robustly negative, but highly variable in magnitude, fast response. We find that the physiological effect of CO2 on plant stomata is the dominant driver of the fast response due to reduced latent heating and also contributes to the large model spread. Using a simple model, we show that CO2 physiological effects dominate future multimodel mean precipitation projections over the Amazon. However, in individual models temperature-driven changes can be large, but due to little agreement, they largely cancel out in the model mean. ©2018. The Authors.

Ethane and propane are the most abundant non-methane hydrocarbons in the atmosphere. However, their emissions, atmospheric distribution, and trends in their atmospheric concentrations are insufficiently understood. Atmospheric model simulations using standard community emission inventories do not reproduce available measurements in the Northern Hemisphere. Here, we show that observations of pre-industrial and present-day ethane and propane can be reproduced in simulations with a detailed atmospheric chemistry transport model, provided that natural geologic emissions are taken into account and anthropogenic fossil fuel emissions are assumed to be two to three times higher than is indicated in current inventories. Accounting for these enhanced ethane and propane emissions results in simulated surface ozone concentrations that are 5-13% higher than previously assumed in some polluted regions in Asia. The improved correspondence with observed ethane and propane in model simulations with greater emissions suggests that the level of fossil (geologic + fossil fuel) methane emissions in current inventories may need re-evaluation. © 2018 The Author(s).

We investigate the climate response to increased concentrations of black carbon (BC), as part of the Precipitation Driver Response Model Intercomparison Project (PDRMIP). A tenfold increase in BC is simulated by 9 global coupled-climate models, producing a model-median effective radiative forcing (ERF) of 0.82 (ranging from 0.41 to 2.91) Wm(−2), and a warming of 0.67 (0.16 to 1.66) K globally and 1.24 (0.26 to 4.31) K in the Arctic. A strong positive instantaneous radiative forcing (median of 2.10 Wm(−2) based on five of the models) is countered by negative rapid adjustments (−0.64 Wm(−2) for the same five models), which dampen the total surface temperature signal. Unlike other drivers of climate change, the response of temperature and cloud profiles to the BC forcing is dominated by rapid adjustments. Low-level cloud amounts increase for all models, while higher-level clouds are diminished. The rapid temperature response is particularly strong above 400 hPa, where increased atmospheric stabilization and reduced cloud cover contrast the response pattern of the other drivers. In conclusion, we find that this substantial increase in BC concentrations does have considerable impacts on important aspects of the climate system. However, some of these effects tend to offset one another, leaving a relatively small global warming of 0.47 K per Wm(−2) – about 20 % lower than the response to a doubling of CO(2). Translating the tenfold increase in BC to the present-day impact of anthropogenic BC (given the emissions used in this work) would leave a warming of merely 0.07 K.

Aerosols have a potentially large effect on climate, particularly through their interactions with clouds, but the magnitude of this effect is highly uncertain. Large volcanic eruptions produce sulfur dioxide, which in turn produces aerosols; these eruptions thus represent a natural experiment through which to quantify aerosol–cloud interactions. Here we show that the massive 2014–2015 fissure eruption in Holuhraun, Iceland, reduced the size of liquid cloud droplets—consistent with expectations—but had no discernible effect on other cloud properties. The reduction in droplet size led to cloud brightening and global-mean radiative forcing of around −0.2 watts per square metre for September to October 2014. Changes in cloud amount or cloud liquid water path, however, were undetectable, indicating that these indirect effects, and cloud systems in general, are well buffered against aerosol changes. This result will reduce uncertainties in future climate projections, because we are now able to reject results from climate models with an excessive liquid-water-path response.

We use simultaneous observations of tropospheric ozone and outgoing longwave radiation (OLR) sensitivity to tropospheric ozone from the Tropospheric Emission Spectrometer (TES) to evaluate model tropospheric ozone and its effect on OLR simulated by a suite of chemistry-climate models that participated in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The ensemble mean of ACCMIP models show a persistent but modest tropospheric ozone low bias (5–20 ppb) in the Southern Hemisphere (SH) and modest high bias (5–10 ppb) in the Northern Hemisphere (NH) relative to TES ozone for 2005–2010. These ozone biases have a significant impact on the OLR. Using TES instantaneous radiative kernels (IRK), we show that the ACCMIP ensemble mean tropospheric ozone low bias leads up to 120 mW m−2 OLR high bias locally but zonally compensating errors reduce the global OLR high bias to 39 ± 41 m Wm−2 relative to TES data. We show that there is a correlation (R2 = 0.59) between the magnitude of the ACCMIP OLR bias and the deviation of the ACCMIP preindustrial to present day (1750–2010) ozone radiative forcing (RF) from the ensemble ozone RF mean. However, this correlation is driven primarily by models whose absolute OLR bias from tropospheric ozone exceeds 100 m Wm−2. Removing these models leads to a mean ozone radiative forcing of 394 ± 42 m Wm−2. The mean is about the same and the standard deviation is about 30% lower than an ensemble ozone RF of 384 ± 60 m Wm−2 derived from 14 of the 16 ACCMIP models reported in a companion ACCMIP study. These results point towards a profitable direction of combining satellite observations and chemistry-climate model simulations to reduce uncertainty in ozone radiative forcing.

International audience; Atmospheric aerosols from anthropogenic and natural sources reach the polar regions through long-range transport and affect the local radiation balance. Such transport is, however, poorly constrained in present-day global climate models, and few multi-model evaluations of polar an-thropogenic aerosol radiative forcing exist. Here we compare the aerosol optical depth (AOD) at 550 nm from simulations with 16 global aerosol models from the AeroCom Phase II model intercomparison project with available observations at both poles. We show that the annual mean multi-model median is representative of the observations in Arctic, but that the intermodel spread is large. We also document the geographical distribution and seasonal cycle of the AOD for the individual aerosol species: black carbon (BC) from fossil fuel and biomass burning, sulfate, organic aerosols (OAs), dust, and sea-salt. For a subset of models that represent nitrate and secondary organic aerosols (SOAs), we document the role of these aerosols at high latitudes. The seasonal dependence of natural and anthropogenic aerosols differs with natural aerosols peaking in winter (sea-salt) and spring (dust), whereas AOD from anthropogenic aerosols peaks in late spring and summer. The models produce a median annual mean AOD of 0.07 in the Arctic (de-fined here as north of 60 • N). The models also predict a noteworthy aerosol transport to the Antarctic (south of 70 • S) with a resulting AOD varying between 0.01 and 0.02. The Published by Copernicus Publications on behalf of the European Geosciences Union. 12198 M. Sand et al.: Aerosols at the poles: an AeroCom Phase II multi-model evaluation models have estimated the shortwave anthropogenic radia-tive forcing contributions to the direct aerosol effect (DAE) associated with BC and OA from fossil fuel and biofuel (FF), sulfate, SOAs, nitrate, and biomass burning from BC and OA emissions combined. The Arctic modelled annual mean DAE is slightly negative (−0.12 W m −2), dominated by a positive BC FF DAE in spring and a negative sulfate DAE in summer. The Antarctic DAE is governed by BC FF. We perform sensitivity experiments with one of the AeroCom models (GISS modelE) to investigate how regional emissions of BC and sulfate and the lifetime of BC influence the Arctic and Antarctic AOD. A doubling of emissions in eastern Asia results in a 33 % increase in Arctic AOD of BC. A doubling of the BC lifetime results in a 39 % increase in Arctic AOD of BC. However, these radical changes still fall within the AeroCom model range.

PDRMIP investigates the role of various drivers of climate change for mean and extreme precipitation changes, based on multiple climate model output and energy budget analyses.\ud \ud As the global temperature increases with changing climate, precipitation rates and patterns are affected through a wide range of physical mechanisms. The globally averaged intensity of extreme precipitation also changes more rapidly than the globally averaged precipitation rate. While some aspects of the regional variation in precipitation predicted by climate models appear robust, there is still a large degree of inter-model differences unaccounted for. Individual drivers of climate change initially alter the energy budget of the atmosphere leading to distinct rapid adjustments involving changes in precipitation. Differences in how these rapid adjustment processes manifest themselves within models are likely to explain a large fraction of the present model spread and needs better quantifications to improve precipitation predictions. Here, we introduce the Precipitation Driver and Response Model Intercomparison Project (PDRMIP), where a set of idealized experiments designed to understand the role of different climate forcing mechanisms were performed by a large set of climate models. PDRMIP focuses on understanding how precipitation changes relating to rapid adjustments and slower responses to climate forcings are represented across models. Initial results show that rapid adjustments account for large regional differences in hydrological sensitivity across multiple drivers. The PDRMIP results are expected to dramatically improve our understanding of the causes of the present diversity in future climate projections.

New calculations of the radiative forcing (RF) are presented for the three main well‐mixed\ud greenhouse gases, methane, nitrous oxide, and carbon dioxide. Methane’s RF is particularly impacted\ud because of the inclusion of the shortwave forcing; the 1750–2011 RF is about 25% higher (increasing from\ud 0.48 W m−2 to 0.61 W m−2) compared to the value in the Intergovernmental Panel on Climate Change (IPCC)\ud 2013 assessment; the 100 year global warming potential is 14% higher than the IPCC value. We present new\ud simplified expressions to calculate RF. Unlike previous expressions used by IPCC, the new ones include the\ud overlap between CO2 and N2O; for N2O forcing, the CO2 overlap can be as important as the CH4 overlap. The\ud 1750–2011 CO2 RF is within 1% of IPCC’s value but is about 10% higher when CO2 amounts reach 2000 ppm, a\ud value projected to be possible under the extended RCP8.5 scenario.

Precipitation is expected to respond differently to various drivers of anthropogenic climate change. We present the first results from the Precipitation Driver and Response Model Intercomparison Project (PDRMIP), where nine global climate models have perturbed CO2, CH4, black carbon, sulfate, and solar insolation. We divide the resulting changes to global mean and regional precipitation into fast responses that scale with changes in atmospheric absorption and slow responses scaling with surface temperature change. While the overall features are broadly similar between models, we find significant regional intermodel variability, especially over land. Black carbon stands out as a component that may cause significant model diversity in predicted precipitation change. Processes linked to atmospheric absorption are less consistently modeled than those linked to top-of-atmosphere radiative forcing. We identify a number of land regions where the model ensemble consistently predicts that fast precipitation responses to climate perturbations dominate over the slow, temperature-driven responses.

We analyse cirrus cloud data over congested air traffic corridors during the period 1984–2007 and look into manmade changes in cirrus clouds due to air traffic. The analysis is based on the International Satellite Cloud Climatology Project (ISCCP) D2 data set for the period 1984–2007. Manmade changes in cirrus clouds were determined from the comparison of cirrus clouds over higher traffic regions and over lower traffic regions. These comparisons were done by calculating the differences between adjacent high and low air traffic areas over North America, Europe, North Atlantic and North Pacific. In all cases the differences show a positive trend which is consistent with the increasing trend of global air traffic in the past 20 years. Over North America, Europe, North Atlantic and North Pacific cirrus clouds increased by 0.9 % per decade over high air traffic regions relative to their low traffic counterparts. The result of manmade cirrus increase of 0.9 % over the western air traffic corridors is expected to have a measurable effect in radiative forcing. © 2016, Springer International Publishing Switzerland.

The usefulness of previous Coupled Model Intercomparison Project (CMIP) exercises has been hampered by a lack of radiative forcing information. This has made it difficult to understand reasons for differences between model responses. Effective radiative forcing (ERF) is easier to diagnose than traditional radiative forcing in global climate models (GCMs) and is more representative of the eventual temperature response. Here we examine the different methods of computing ERF in two GCMs. We find that ERF computed from a fixed sea-surface temperature (SST) method (ERF_fSST) has much more certainty than regression based methods. Thirty-year integrations are sufficient to reduce the 5-95% confidence interval in global ERF_fSST to 0.1 W m-2. For 2xCO2 ERF, 30 year integrations are needed to ensure that the signal is larger than the local confidence interval over more than 90% of the globe. Within the ERF_fSST method there are various options for prescribing SSTs and sea-ice. We explore these and find that ERF is only weakly dependent on the methodological choices. Prescribing the monthly-averaged seasonally varying model’s preindustrial climatology is recommended for its smaller random error and easier implementation. As part of CMIP6, the Radiative Forcing Model Intercomparison Project (RFMIP) asks models to conduct 30-year ERF_fSST experiments using the model’s own preindustrial climatology of SST and sea-ice. The Aerosol and Chemistry Model Intercomparison Project (AerChemMIP) will also mainly use this approach. We propose this as a standard method for diagnosing ERF and recommend that it be used across the climate modelling community to aid future comparisons.

Aerosol properties above clouds have been retrieved over the South East Atlantic Ocean during the fire season 2006 using satellite observations from POLDER (Polarization and Directionality of Earth Reflectances). From June to October, POLDER has observed a mean Above-Cloud Aerosol Optical Thickness (ACAOT) of 0.28 and a mean Above-Clouds Single Scattering Albedo (ACSSA) of 0.87 at 550nm. These results have been used to evaluate the simulation of aerosols above clouds in five Aerosol Comparisons between Observations and Models (Goddard Chemistry Aerosol Radiation and Transport (GOCART), Hadley Centre Global Environmental Model 3 (HadGEM3), European Centre Hamburg Model 5-Hamburg Aerosol Module 2 (ECHAM5-HAM2), Oslo-Chemical Transport Model 2 (OsloCTM2), and Spectral Radiation-Transport Model for Aerosol Species (SPRINTARS)). Most models do not reproduce the observed large aerosol load episodes. The comparison highlights the importance of the injection height and the vertical transport parameterizations to simulate the large ACAOT observed by POLDER. Furthermore, POLDER ACSSA is best reproduced by models with a high imaginary part of black carbon refractive index, in accordance with recent recommendations. ©2016. American Geophysical Union.

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

Carbon dioxide has exerted the largest portion of radiative forcing and surface temperature change over the industrial era, but other anthropogenic influences have also contributed. However, large uncertainties in total forcing make it difficult to derive climate sensitivity from historical observations. Anthropogenic forcing has increased between the Fourth and Fifth Assessment Reports of the Intergovernmental Panel of Climate Change (IPCC; refs,), although its relative uncertainty has decreased. Here we show, based on data from the two reports, that this evolution towards lower uncertainty can be expected to continue into the future. Because it is easier to reduce air pollution than carbon dioxide emissions and because of the long lifetime of carbon dioxide, the less uncertain carbon dioxide forcing is expected to become increasingly dominant. Using a statistical model, we estimate that the relative uncertainty in anthropogenic forcing of more than 40% quoted in the latest IPCC report for 2011 will be almost halved by 2030, even without better scientific understanding. Absolute forcing uncertainty will also decline for the first time, provided projected decreases in aerosols occur. Other factors being equal, this stronger constraint on forcing will bring a significant reduction in the uncertainty of observation-based estimates of the transient climate response, with a 50% reduction in its uncertainty range expected by 2030.

The collation and applications of a comprehensive database of infrared cross-sections of 200 halocarbons and related molecules is described. The first phase of this research was published by Hodnebrog et al. (Reviews of Geophysics, 2013, doi:10.1002/rog.20013) in which cross-sections were drawn from a wide range of laboratory studies in the published literature and, when these were not available, from ab initio calculations. The criteria for selection of particular cross-section data sets will be described. The primary purpose of the database is for use in the calculation of radiative forcing and climate metrics such as the Global Warming Potential, and illustrations of their usage will be given. The work on the database is intended to be an ongoing exercise and the plan is to revise and expand the database as new data become available.

A wide range of anthropogenic as well as natural forcing mechanisms may lead to climate change. We present calculations of the radiative forcing due to anthropogenic emissions leading to changes in the concentrations of several trace gases and aerosols. Increase in all major well mixed greenhouse gases are included as well as changes in tropospheric and stratospheric ozone. The radiative forcing due to certain aerosols is also estimated. The calculations have been performed for the Northern Hemisphere, and the main focus in this scientific note is on high latitudes.

International audience

Clouds and aerosols continue to contribute the largest uncertainty to estimates and interpretations of the Earth's changing energy budget. This chapter focuses on process understanding and considers observations, theory and models to assess how clouds and aerosols contribute and respond to climate change. The following conclusions are drawn.

In the mid-1970s it was recognized that, as well as being substances that deplete stratospheric ozone, chlorofluorocarbons (CFCs) were strong greenhouse gases that could have substantial impacts on radiative forcing of climate change. Around a decade later, this group of radiatively active compounds was expanded to include a large number of replacements for ozone-depleting substances such as chlorocarbons, hydrochlorocarbons, hydrochlorofluorocarbons (HCFCs), hydrofluorocarbons (HFCs), perfluorocarbons (PFCs), bromofluorocarbons, and bromochlorofluorocarbons.\ud This paper systematically reviews the published literature concerning the radiative efficiencies (REs) of CFCs, bromofluorocarbons and bromochlorofluorocarbons (halons), HCFCs, HFCs, PFCs, SF6, NF3, and related halogen containing compounds. In addition we provide a comprehensive and self-consistent set of new calculations of REs and global warming potentials (GWPs) for these compounds, mostly employing atmospheric lifetimes taken from the available literature. We also present Global Temperature change Potentials (GTPs) for selected gases. Infrared absorption spectra used in the RE calculations were taken from databases and individual studies, and from experimental and ab initio computational studies. Evaluations of REs and GWPs are presented for more than 200 compounds. Our calculations yield REs significantly (> 5%) different from those in the Intergovernmental Panel on Climate Change Fourth Assessment Report (AR4) for 49 compounds. We present new RE values for more than 100 gases which were not included in AR4. A widely-used simple method to calculate REs and GWPs from absorption spectra and atmospheric lifetimes is assessed and updated. This is the most comprehensive review of the radiative efficiencies and global warming potentials of halogenated compounds performed to date.

The CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) layer product is used for a multimodel evaluation of the vertical distribution of aerosols. Annual and seasonal aerosol extinction profiles are analyzed over 13 sub-continental regions representative of industrial, dust, and biomass burning pollution, from CALIOP 2007-2009 observations and from AeroCom (Aerosol Comparisons between Observations and Models) 2000 simulations. An extinction mean height diagnostic (Z) is defined to quantitatively assess the models' performance. It is calculated over the 0-6 km and 0-10 km altitude ranges by weighting the altitude of each 100 m altitude layer by its aerosol extinction coefficient. The mean extinction profiles derived from CALIOP layer products provide consistent regional and seasonal specificities and a low inter-annual variability. While the outputs from most models are significantly correlated with the observed Z climatologies, some do better than others, and 2 of the 12 models perform particularly well in all seasons. Over industrial and maritime regions, most models show higher Z than observed by CALIOP, whereas over the African and Chinese dust source regions, Z is underestimated during Northern Hemisphere Spring and Summer. The positive model bias in Z is mainly due to an overestimate of the extinction above 6 km. Potential CALIOP and model limitations, and methodological factors that might contribute to the differences are discussed. Copyright 2012 by the American Geophysical Union.

The effect of anthropogenic emissions from China on global burdens of ozone, sulphate, organic carbon (OC) and black carbon (BC) aerosols is examined, using the three-dimensional chemistry transport model Oslo CTM2. Two model simulations were performed, the first with global present-day emissions and the second with the anthropogenic emissions from China set to their pre-industrial levels. The global radiative forcing for these species is then calculated. Industrial emissions from China are found to account for a 4–5% increase in the global burden of OC aerosol, the change in secondary organic aerosol being slightly less than that of primary organic aerosol. A 10% increase in the global sulphate aerosol burden is calculated, and the increase in BC is 23%. The global radiative forcing of aerosols from China was calculated to be −62, −3.7, −13 and 89 mW m-2, for sulphate, secondary organic, primary organic and BC aerosols, respectively. The increase in ozone causes a forcing of 77 mW m-2.DOI: 10.1111/j.1600-0889.2009.00424.x

To estimate the impact of emissions by road, aircraft and ship traffic on ozone and OH in the present-day atmosphere six different atmospheric chemistry models have been used. Based on newly developed global emission inventories for road, ship and aircraft emission data sets each model performed sensitivity simulations reducing the emissions of each transport sector by 5%. The model results indicate that on global annual average lower tropospheric ozone responds most sensitive to ship emissions (50.6%±10.9% of the total traffic induced perturbation), followed by road (36.7%±9.3%) and aircraft exhausts (12.7%±2.9%), respectively. In the northern upper troposphere between 200–300 hPa at 30–60° N the maximum impact from road and ship are 93% and 73% of the maximum effect of aircraft, respectively. The latter is 0.185 ppbv for ozone (for the 5% case) or 3.69 ppbv when scaling to 100%. On the global average the impact of road even dominates in the UTLS-region. The sensitivity of ozone formation per NOx molecule emitted is highest for aircraft exhausts. The local maximum effect of the summed traffic emissions on the ozone column predicted by the models is 0.2 DU and occurs over the northern subtropical Atlantic extending to central Europe. Below 800 hPa both ozone and OH respond most sensitively to ship emissions in the marine lower troposphere over the Atlantic. Based on the 5% perturbation the effect on ozone can exceed 0.6% close to the marine surface (global zonal mean) which is 80% of the total traffic induced ozone perturbation. In the southern hemisphere ship emissions contribute relatively strongly to the total ozone perturbation by 60%–80% throughout the year. Methane lifetime changes against OH are affected strongest by ship emissions up to 0.21 (± 0.05)%, followed by road (0.08 (±0.01)%) and air traffic (0.05 (± 0.02)%). Based on the full scale ozone and methane perturbations positive radiative forcings were calculated for road emissions (7.3±6.2 mWm−2) and for aviation (2.9±2.3 mWm−2). Ship induced methane lifetime changes dominate over the ozone forcing and therefore lead to a net negative forcing (−25.5±13.2 mWm−2).

We evaluate black carbon (BC) model predictions from the AeroCom model intercomparison project by considering the diversity among year 2000 model simulations and comparing model predictions with available measurements. These model-measurement intercomparisons include BC surface and aircraft concentrations, aerosol absorption optical depth (AAOD) from AERONET and Ozone Monitoring Instrument (OMI) retrievals and BC column estimations based on AERONET. In regions other than Asia, most models are biased high compared to surface concentration measurements. However compared with (column) AAOD or BC burden retreivals, the models are generally biased low. The average ratio of model to retrieved AAOD is less than 0.7 in South American and 0.6 in African biomass burning regions; both of these regions lack surface concentration measurements. In Asia the average model to observed ratio is 0.6 for AAOD and 0.5 for BC surface concentrations. Compared with aircraft measurements over the Americas at latitudes between 0 and 50 N, the average model is a factor of 10 larger than observed, and most models exceed the measured BC standard deviation in the mid to upper troposphere. At higher latitudes the average model to aircraft BC is 0.6 and underestimates the observed BC loading in the lower and middle troposphere associated with springtime Arctic haze. Low model bias for AAOD but overestimation of surface and upper atmospheric BC concentrations at lower latitudes suggests that most models are underestimating BC absorption and should improve estimates for refractive index, particle size, and optical effects of BC coating. Retrieval uncertainties and/or differences with model diagnostic treatment may also contribute to the model-measurement disparity. Largest AeroCom model diversity occurred in northern Eurasia and the remote Arctic, regions influenced by anthropogenic sources. Changing emissions, aging, removal, or optical properties within a single model generated a smaller change in model predictions than the range represented by the full set of AeroCom models. Upper tropospheric concentrations of BC mass from the aircraft measurements are suggested to provide a unique new benchmark to test scavenging and vertical dispersion of BC in global models.

International audience; The global chemical transport model Oslo CTM2 has been extended to include the formation, transport and deposition of secondary organic aerosol (SOA). Precursor hydrocarbons which are oxidised to form condensible species include both biogenic species such as terpenes and isoprene, as well as species emitted predominantly by anthropogenic activities (toluene, m-xylene, methylbenzene and other aromatics). A model simulation for 2004 gives an annual global SOA production of approximately 55 Tg. Of this total, 2.5 Tg is found to consist of the oxidation products of anthropogenically emitted hydrocarbons, and about 15 Tg is formed by the oxidation products of isoprene. The global production of SOA is increased to about 69 Tg yr?1 by allowing semi-volatile species to partition to ammonium sulphate aerosol. This brings modelled organic aerosol values closer to those observed, however observations in Europe remain significantly underestimated. Allowing SOA to partition into ammonium sulphate aerosol increases the contribution of anthropogenic SOA from about 4.5% to 9.4% of the total production. Total modelled organic aerosol (OA) values are found to represent a lower fraction of the measured values in winter (when primary organic aerosol (POA) is the dominant OA component) than in summer, which may be an indication that estimates of POA emissions are too low. Additionally, for measurement stations where the summer OA values are higher than in winter, the model generally underestimates the increase in summertime OA. In order to correctly model the observed increase in OA in summer, additional SOA sources or formation mechanisms may be necessary. The importance of NO3 as an oxidant of SOA precursors is found to vary regionally, causing up to 50%?60% of the total amount of SOA near the surface in polluted regions and less than 25% in more remote areas, if the yield of condensible oxidation products for ?-pinene is used for NO3 oxidation of all terpenes. Reducing the yield for ?-pinene and limonene oxidation in line with recent measurements reduces the global fraction of SOA formed from NO3 oxidation products from 27% to about 21%. This study underscores the need for SOA to be represented in a more realistic way in global aerosol models in order to better reproduce observations of organic aerosol burdens in industrialised and biomass burning regions.

International audience; The global chemical transport model Oslo CTM2 has been extended to include the formation, transport and deposition of secondary organic aerosol (SOA). Precursor hydrocarbons which are oxidised to form condensible species include both biogenic species such as terpenes and isoprene, as well as species emitted predominantly by anthropogenic activities (toluene, m-xylene, methylbenzene and other aromatics). A model simulation for 2004 gives an annual global SOA production of approximately 55 Tg. Of this total, 2.5 Tg is found to consist of the oxidation products of anthropogenically emitted hydrocarbons, and about 15 Tg is formed by the oxidation products of isoprene. The global production of SOA is increased to about 76 Tg yr?1 by allowing semi-volatile species to condense on ammonium sulphate aerosol. This brings modelled organic aerosol values closer to those observed, however observations in Europe remain significantly underestimated, raising the possibility of an unaccounted for SOA source. Allowing SOA to form on ammonium sulphate aerosol increases the contribution of anthropogenic SOA from about 4.5% to almost 9% of the total production. The importance of NO3 as an oxidant of SOA precursors is found to vary regionally, causing up to 50%?60% of the total amount of SOA near the surface in polluted regions and less than 25% in more remote areas. This study underscores the need for SOA to be represented in a more realistic way in global aerosol models in order to better reproduce observations of organic aerosol burdens in industrialised and biomass burning regions.

The indirect effect of aerosols via liquid clouds is investigated by comparing aerosol and cloud characteristics from the Global Climate Model CAM-Oslo to those observed by the MODIS instrument onboard the TERRA and AQUA satellites (http://modis.gsfc.nasa.gov). The comparison is carried out for 15 selected regions ranging from remote and clean to densely populated and polluted. For each region, the regression coefficient and correlation coefficient for the following parameters are calculated: Aerosol Optical Depth vs. Liquid Cloud Optical Thickness, Aerosol Optical Depth vs. Liquid Cloud Droplet Effective Radius and Aerosol Optical Depth vs. Cloud Liquid Water Path. Modeled and observed correlation coefficients and regression coefficients are then compared for a 3-year period starting in January 2001. Additionally, global maps for a number of aerosol and cloud parameters crucial for the understanding of the aerosol indirect effect are compared for the same period of time. Significant differences are found between MODIS and CAM-Oslo both in the regional and global comparison. However, both the model and the observations show a positive correlation between Aerosol Optical Depth and Cloud Optical Depth in practically all regions and for all seasons, in agreement with the current understanding of aerosol-cloud interactions. The correlation between Aerosol Optical Depth and Liquid Cloud Droplet Effective Radius is variable both in the model and the observations. However, the model reports the expected negative correlation more often than the MODIS data. Aerosol Optical Depth is overall positively correlated to Cloud Liquid Water Path both in the model and the observations, with a few regional exceptions.

The AeroCom exercise diagnoses multi-component aerosol modules in global modeling. In an initial assessment simulated global distributions for mass and mid-visible aerosol optical thickness (aot) were compared among 20 different modules. Model diversity was also explored in the context of previous comparisons. For the component combined aot general agreement has improved for the annual global mean. At 0.11 to 0.14, simulated aot values are at the lower end of global averages suggested by remote sensing from ground (AERONET ca. 0.135) and space (satellite composite ca. 0.15). More detailed comparisons, however, reveal that larger differences in regional distribution and significant differences in compositional mixture remain. Of particular concern are large model diversities for contributions by dust and carbonaceous aerosol, because they lead to significant uncertainty in aerosol absorption (aab). Since aot and aab, both, influence the aerosol impact on the radiative energy-balance, the aerosol (direct) forcing uncertainty in modeling is larger than differences in aot might suggest. New diagnostic approaches are proposed to trace model differences in terms of aerosol processing and transport: These include the prescription of common input (e.g. amount, size and injection of aerosol component emissions) and the use of observational capabilities from ground (e.g. measurements networks) or space (e.g. correlations between aerosol and clouds).

Global atmospheric dust is simulated using the Dust Entrainment and Deposition (DEAD) model in combination with the global-scale Oslo chemical transport model CTM2 using meteorological data for 1996. Dust sources are calculated using both mean wind speeds with model resolution T63 and subgrid wind speeds. Different data sets are used to describe soil erodibility. We explain how the different assumptions about dust production affect atmospheric dust burden and deposition. Some aspects of the annual dust cycle, such as the east Asian dust emissions, are largely dependent on the data used to determine soil erodibility. Other aspects, such as the timing of the maximum in the African plume at Northern Hemisphere summer, are well modeled with all data sets applied here. We show that the daily variation in optical depth at Cape Verde on the west coast of Africa is well simulated when we assume that erodibility is correlated with surface reflectivity from Moderate-Resolution Imaging Spetroradiometer (MODIS) satellite data. Using a subgrid probability density function of wind speed to drive the dust sources facilitates dust emissions in areas with low wind speeds. Dust concentrations in remote areas are sensitive to the parameterization of wet deposition. Our results point out the need for a detailed soil erodibility data set for global dust modeling, and they suggest that surface reflectivity is potentially valuable for producing or evaluating such data sets.

International audience; Trends in cirrus cloud cover have been estimated based on 16 years of data from ISCCP (International Satellite Cloud Climatology Project). The results have been spatially correlated with aircraft density data to determine the changes in cirrus cloud cover due to aircraft traffic. The correlations are only moderate, as many other factors have also contributed to changes in cirrus. Still we regard the results to be indicative of an impact of aircraft on cirrus amount. The main emphasis of our study is on the area covered by the METEOSAT satellite to avoid trends in the ISCCP data resulting from changing satellite viewing geometry. In Europe, which is within the METEOSAT region, we find indications of a trend of about 1-2% cloud cover per decade due to aircraft, in reasonable agreement with previous studies. The positive trend in cirrus in areas of high aircraft traffic contrasts with a general negative trend in cirrus. Extrapolation in time to cover the entire period of aircraft operations and in space to cover the global scale yields a mean estimate of 0.03 Wm-2 (lower limit 0.01, upper limit 0.08 Wm-2) for the radiative forcing due to aircraft induced cirrus. The mean is close to the value given by IPCC (1999) as an upper limit.

New estimates of the various contributions to the radiative forcing (RF) from aviation are presented, mainly based on results from the TRADEOFF project that update those of the Intergovernmental Panel on Climate Change (IPCC, 1999). The new estimate of the total RF from aviation for 2000 is approximately the same as that of the IPCC's estimate for 1992. This is mainly a consequence of the strongly reduced RF from contrails, which compensates the increase due to increased traffic from 1992 to 2000. The RF from other aviation-induced cirrus clouds might be as large as the present estimate of the total RF (without cirrus). However, our present knowledge on these aircraft-induced cirrus clouds is too poor to provide a reliable estimate of the associated RF. © Gebrüder Borntraeger, Berlin, Stuttgart 2005.

International audience; HFC-134a (CF3CH2F) is the most rapidly growing hydrofluorocarbon in terms of atmospheric abundance. It is currently used in a large number of household refrigerators and air-conditioning systems and its concentration in the atmosphere is forecast to increase substantially over the next 50–100 years. Previous estimates of its radiative forcing per unit concentration have differed significantly 25%. This paper uses a two-step approach to resolve this discrepancy. In the first step six independent absorption cross section datasets are analysed. We find that, for the integrated cross section in the spectral bands that contribute most to the radiative forcing, the differences between the various datasets are typically smaller than 5% and that the dependence on pressure and temperature is not significant. A “recommended'' HFC-134a infrared absorption spectrum was obtained based on the average band intensities of the strongest bands. In the second step, the “recommended'' HFC-134a spectrum was used in six different radiative transfer models to calculate the HFC-134a radiative forcing efficiency. The clear-sky instantaneous radiative forcing, using a single global and annual mean profile, differed by 8%, between the 6 models, and the latitudinally-resolved adjusted cloudy sky radiative forcing estimates differed by a similar amount. We calculate that the radiative forcing efficiency of HFC-134a is

International audience; Monthly mean aerosol optical depth (AOD) over ocean is compared from a total of 9 aerosol retrievals during a 40 months period. Comparisons of AOD have been made both for the entire period and sub periods. We identify regions where there is large disagreement and good agreement between the aerosol satellite retrievals. Significant differences in AOD have been identified in most of the oceanic regions. Several analyses are performed including spatial correlation between the retrievals as well as comparison with AERONET data. During the 40 months period studied there have been several major aerosol field campaigns as well as events of high aerosol content. It is studied how the aerosol retrievals compare during such circumstances. The differences found in this study are larger than found in a previous study where 5 aerosol retrievals over an 8 months period were compared. Part of the differences can be explained by limitations and deficiencies in some of the aerosol retrievals. In particular, results in coastal regions are promising especially for aerosol retrievals from satellite instruments particularly suited for aerosol research. In depth analyses explaining the differences between AOD obtained in different retrievals are clearly needed. We limit this study to identifying differences and similarities and indicating possible sources that affect the quality of the retrievals. This is a necessary first step towards understanding the differences and improving the retrievals.

Radiative forcing due to changes in ozone is expected for the 21st century. An assessment on changes in the tropospheric oxidative state through a model intercomparison ("OxComp'') was conducted for the IPCC Third Assessment Report (IPCC-TAR). OxComp estimated tropospheric changes in ozone and other oxidants during the 21st century based on the "SRES'' A2p emission scenario. In this study we analyze the results of 11 chemical transport models (CTMs) that participated in OxComp and use them as input for detailed radiative forcing calculations. We also address future ozone recovery in the lower stratosphere and its impact on radiative forcing by applying two models that calculate both tropospheric and stratospheric changes. The results of OxComp suggest an increase in global-mean tropospheric ozone between 11.4 and 20.5 DU for the 21st century, representing the model uncertainty range for the A2p scenario. As the A2p scenario constitutes the worst case proposed in IPCC-TAR we consider these results as an upper estimate. The radiative transfer model yields a positive radiative forcing ranging from 0.40 to 0.78 W m(-2) on a global and annual average. The lower stratosphere contributes an additional 7.5-9.3 DU to the calculated increase in the ozone column, increasing radiative forcing by 0.15-0.17 W m(-2). The modeled radiative forcing depends on the height distribution and geographical pattern of predicted ozone changes and shows a distinct seasonal variation. Despite the large variations between the 11 participating models, the calculated range for normalized radiative forcing is within 25%, indicating the ability to scale radiative forcing to global-mean ozone column change.