The evolution of the global aerosol system in a transient climate simulation from 1860 to 2100

The evolution of the global aerosol system from 1860 to 2100 is investigated through a transient atmosphere-ocean General Circulation Model climate simulation with interactively coupled atmospheric aerosol and oceanic biogeochemistry modules. The microphysical aerosol module HAM incorporates the major global aerosol cycles with prognostic treatment of their composition, size distribution, and mixing state. Based on an SRES A1B emission scenario, the global mean sulfate burden is projected to peak in 2020 while black carbon and particulate organic matter show a lagged peak around 2070. From present day to future conditions the anthropogenic aerosol burden shifts generally from the northern high-latitudes to the developing low-latitude source regions with impacts on regional climate. Atmospheric residence- and aging-times show significant alterations under varying climatic and pollution conditions. Concurrently, the aerosol mixing state changes with an increasing aerosol mass fraction residing in the internally mixed accumulation mode. The associated increase in black carbon causes a more than threefold increase of its co-single scattering albedo from 1860 to 2100. Mid-visible aerosol optical depth increases from pre-industrial times, predominantly from the aerosol fine fraction, peaks at 0.26 around the sulfate peak in 2020 and maintains a high level thereafter, due to the continuing increase in carbonaceous aerosols. The global mean anthropogenic top of the atmosphere clear-sky short-wave direct aerosol radiative perturbation intensifies to −1.1 W m^−2 around 2020 and weakens after 2050 to −0.6 W m^−2, owing to an increase in atmospheric absorption. The demonstrated modifications in the aerosol residence- and aging-times, the microphysical state, and radiative properties challenge simplistic approaches to estimate the aerosol radiative effects from emission projections

Sources of uncertainties in modelling black carbon at the global scale

Our understanding of the global black carbon (BC) cycle is essentially qualitative due to uncertainties in our knowledge of its properties. This work investigates two source of uncertainties in modelling black carbon: those due to the use of different schemes for BC ageing and its removal rate in the global Transport-Chemistry model TM5 and those due to the uncertainties in the definition and quantification of the observations, which propagate through to both the emission inventories, and the measurements used for the model evaluation. The schemes for the atmospheric processing of black carbon that have been tested with the model are (i) a simple approach considering BC as bulk aerosol and a simple treatment of the removal with fixed 70% of in-cloud black carbon concentrations scavenged by clouds and removed when rain is present and (ii) a more complete description of microphysical ageing within an aerosol dynamics model, where removal is coupled to the microphysical properties of the aerosol, which results in a global average of 40% in-cloud black carbon that is scavenged in clouds and subsequently removed by rain, thus resulting in a longer atmospheric lifetime. This difference is reflected in comparisons between both sets of modelled results and the measurements. Close to the sources, both anthropogenic and vegetation fire source regions, the model results do not differ significantly, indicating that the emissions are the prevailing mechanism determining the concentrations and the choice of the aerosol scheme does not influence the levels. In more remote areas such as oceanic and polar regions the differences can be orders of magnitude, due to the differences between the two schemes. The more complete description reproduces the seasonal trend of the black carbon observations in those areas, although not always the magnitude of the signal, while the more simplified approach underestimates black carbon concentrations by orders of magnitude. The sensitivity to wet scavenging has been tested by varying in-cloud and below-cloud removal. BC lifetime increases by 10% when large scale and convective scale precipitation removal efficiency are reduced by 30%, while the variation is very small when below-cloud scavenging is zero. Since the emission inventories are representative of elemental carbon-like substance, the model output should be compared to elemental carbon measurements and if known, the ratio of black carbon to elemental carbon mass should be taken into account when the model is compared with black carbon observation

The aerosol-climate model ECHAM5-HAM

The aerosol-climate modelling system ECHAM5-HAM is introduced. It is based on a flexible microphysical approach and, as the number of externally imposed parameters is minimised, allows the application in a wide range of climate regimes. ECHAM5-HAM predicts the evolution of an ensemble of microphysically interacting internally- and externally-mixed aerosol populations as well as their size-distribution and composition. The size-distribution is represented by a superposition of log-normal modes. In the current setup, the major global aerosol compounds sulfate (SU), black carbon (BC), particulate organic matter (POM), sea salt (SS), and mineral dust (DU) are included. The simulated global annual mean aerosol burdens (lifetimes) for the year 2000 are for SU: 0.80 Tg(S) (3.9 days), for BC: 0.11 Tg (5.4 days), for POM: 0.99 Tg (5.4 days), for SS: 10.5 Tg (0.8 days), and for DU: 8.28 Tg (4.6 days). An extensive evaluation with in-situ and remote sensing measurements underscores that the model results are generally in good agreement with observations of the global aerosol system. The simulated global annual mean aerosol optical depth (AOD) is with 0.14 in excellent agreement with an estimate derived from AERONET measurements (0.14) and a composite derived from MODIS-MISR satellite retrievals (0.16). Regionally, the deviations are not negligible. However, the main patterns of AOD attributable to anthropogenic activity are reproduced

Constraining uncertainty in aerosol direct forcing

The uncertainty in present-day anthropogenic forcing is dominated by uncertainty in the strength of the contribution from aerosol. Much of the uncertainty in the direct aerosol forcing can be attributed to uncertainty in the anthropogenic fraction of aerosol in the present-day atmosphere, due to a lack of historical observations. Here we present a robust relationship between total present-day aerosol optical depth and the anthropogenic contribution across three multi-model ensembles and a large single-model perturbed parameter ensemble. Using observations of aerosol optical depth, we determine a reduced likely range of the anthropogenic component and hence a reduced uncertainty in the direct forcing of aerosol

Brightening of the global cloud field by nitric acid and the associated radiative forcing

Clouds cool Earth's climate by reflecting 20% of the incoming solar energy, while also trapping part of the outgoing radiation. The effect of human activities on clouds is poorly understood, but the present-day anthropogenic cooling via changes of cloud albedo and lifetime could be of the same order as warming from anthropogenic addition in CO<sub>2</sub>. Soluble trace gases can increase water condensation to particles, possibly leading to activation of smaller aerosols and more numerous cloud droplets. We have studied the effect of nitric acid on the aerosol indirect effect with the global aerosol-climate model ECHAM5.5-HAM2. Including the nitric acid effect in the model increases cloud droplet number concentrations globally by 7%. The nitric acid contribution to the present-day cloud albedo effect was found to be −0.32 W m<sup>−2</sup> and to the total indirect effect −0.46 W m<sup>−2</sup>. The contribution to the cloud albedo effect is shown to increase to −0.37 W m<sup>−2</sup> by the year 2100, if considering only the reductions in available cloud condensation nuclei. Overall, the effect of nitric acid can play a large part in aerosol cooling during the following decades with decreasing SO<sub>2</sub> emissions and increasing NO<sub>x</sub> and greenhouse gases

Technical Note: Anthropogenic and natural offline emissions and the online EMissions and dry DEPosition submodel EMDEP of the Modular Earth Submodel system (MESSy)

International audienceWe present the online calculated Earth's surface trace gas and aerosol emissions and dry deposition in the Modular Earth Submodel System (MESSy) submodel EMDEP as well as the currently applied anthropogenic and natural emissions inventories. These inventories, being read-in by the MESSy submodel OFFLEM, include the industrial, fossil fuel, agricultural and biomass burning emissions considering emission height profiles as a function of the source category based on the EDGAR v3.2 fast track 2000 inventory. Terrestrial and marine emissions of a selection of trace gases and aerosols are calculated online in EMDEP using climate model parameters such as wind speed, temperature and land cover and land use parameters. The online dry deposition calculation includes gases and aerosols, where the default selection for the trace gases for the dry deposition scheme can be easily extended using a commonly applied method based on trace gas solubility and reactivity. In general, the simulated global annual emissions agree with previously reported inventories, although differences exist, partly dependent on the applied model resolution. A high sensitivity of the simulated dry deposition to the applied emission height profiles stresses the importance of a realistic and consistent representation of the spatial and temporal variability in surface exchange processes in Earth system models

Answering the Call for Model-Relevant Observations of Aerosols and Clouds

We describe a technique for combining multiple A-Train aerosol data sets, namely MODIS spectral AOD (aerosol optical depth), OMI AAOD (absorption aerosol optical depth) and CALIOP aerosol backscatter retrievals (hereafter referred to as MOC retrievals) to estimate full spectral sets of aerosol radiative properties, and ultimately to calculate the 3-D distribution of direct aerosol radiative effects (DARE). We present MOC results using almost two years of data collected in 2007 and 2008, and show comparisons of the aerosol radiative property estimates to collocated AERONET retrievals. We compare the spatio-temporal distribution of the MOC retrievals and MOC-based calculations of seasonal clear-sky DARE to values derived from four models that participated in the Phase II AeroCom model intercomparison initiative. Comparisons of seasonal aerosol property to AeroCom Phase II results show generally good agreement best agreement with forcing results at TOA is found with GMI-MerraV3.We discuss the challenges in making observations that really address deficiencies in models, with some of the more relevant aspects being representativeness of the observations for climatological states, and whether a given model-measurement difference addresses a sampling or a model error