Aerosol Direct Radiative Forcing Research Articles

Spatial variability of the direct radiative forcing of biomass burning aerosols and the effects of land use change in Amazonia

Abstract. This paper addresses the Amazonian shortwave radiative budget over cloud-free conditions after considering three aspects of deforestation: (i) the emission of aerosols from biomass burning due to forest fires; (ii) changes in surface albedo after deforestation; and (iii) modifications in the column water vapour amount over deforested areas. Simultaneous Clouds and the Earth's Radiant Energy System (CERES) shortwave fluxes and aerosol optical depth (AOD) retrievals from the Moderate Resolution Imaging SpectroRadiometer (MODIS) were analysed during the peak of the biomass burning seasons (August and September) from 2000 to 2009. A discrete-ordinate radiative transfer (DISORT) code was used to extend instantaneous remote sensing radiative forcing assessments into 24-h averages. The mean direct radiative forcing of aerosols at the top of the atmosphere (TOA) during the biomass burning season for the 10-yr studied period was −5.6 ± 1.7 W m−2. Furthermore, the spatial distribution of the direct radiative forcing of aerosols over Amazonia was obtained for the biomass burning season of each year. It was observed that for high AOD (larger than 1 at 550 nm) the maximum daily direct aerosol radiative forcing at the TOA may be as high as −20 W m−2 locally. The surface reflectance plays a major role in the aerosol direct radiative effect. The study of the effects of biomass burning aerosols over different surface types shows that the direct radiative forcing is systematically more negative over forest than over savannah-like covered areas. Values of −15.7 ± 2.4 W m−2τ550 nm and −9.3 ± 1.7 W m−2τ550 nm were calculated for the mean daily aerosol forcing efficiencies over forest and savannah-like vegetation respectively. The overall mean annual land use change radiative forcing due to deforestation over the state of Rondônia, Brazil, was determined as −7.3 ± 0.9 W m−2. Biomass burning aerosols impact the radiative budget for approximately two months per year, whereas the surface albedo impact is observed throughout the year. Because of this difference, the estimated impact in the Amazonian annual radiative budget due to surface albedo-change is approximately 6 times higher than the impact due to aerosol emissions. The influence of atmospheric water vapour content in the radiative budget was also studied using AERONET column water vapour. It was observed that column water vapour is on average smaller by about 0.35 cm (around 10% of the total column water vapour) over deforested areas compared to forested areas. Our results indicate that this drying contributes to an increase in the shortwave radiative forcing, which varies from 0.4 W m−2 to 1.2 W m−2 depending on the column water vapour content before deforestation. The large radiative forcing values presented in this study point out that deforestation could have strong implications in convection, cloud development and the ratio of direct to diffuse radiation, which impacts carbon uptake by the forest.

A multimodel assessment of the influence of regional anthropogenic emission reductions on aerosol direct radiative forcing and the role of intercontinental transport

In this study, we assess changes of aerosol optical depth (AOD) and direct radiative forcing (DRF) in response to the reduction of anthropogenic emissions in four major pollution regions in the Northern Hemisphere by using results from nine global models in the framework of the Hemispheric Transport of Air Pollution (HTAP). DRF at top of atmosphere (TOA) and surface is estimated based on AOD results from the HTAP models and AOD‐normalized DRF (NDRF) from a chemical transport model. The multimodel results show that, on average, a 20% reduction of anthropogenic emissions in North America, Europe, East Asia, and South Asia lowers the global mean AOD (all‐sky TOA DRF) by 9.2% (9.0%), 3.5% (3.0%), and 9.4% (10.0%) for sulfate, particulate organic matter (POM), and black carbon (BC), respectively. Global annual average TOA all‐sky forcing efficiency relative to particle or gaseous precursor emissions from the four regions (expressed as multimodel mean ± one standard deviation) is −3.5 ± 0.8, −4.0 ± 1.7, and 29.5 ± 18.1 mW m−2 per Tg for sulfate (relative to SO2), POM, and BC, respectively. The impacts of the regional emission reductions on AOD and DRF extend well beyond the source regions because of intercontinental transport (ICT). On an annual basis, ICT accounts for 11 ± 5% to 31 ± 9% of AOD and DRF in a receptor region at continental or subcontinental scale, with domestic emissions accounting for the remainder, depending on regions and species. For sulfate AOD, the largest ICT contribution of 31 ± 9% occurs in South Asia, which is dominated by the emissions from Europe. For BC AOD, the largest ICT contribution of 28 ± 18% occurs in North America, which is dominated by the emissions from East Asia. The large spreads among models highlight the need to improve aerosol processes in models, and evaluate and constrain models with observations.

Global all‐sky shortwave direct radiative forcing of anthropogenic aerosols from combined satellite observations and GOCART simulations

Estimation of aerosol direct radiative forcing (DRF) from satellite measurements is challenging because current satellite sensors do not have the capability of discriminating between anthropogenic and natural aerosols. We combine 3‐hourly cloud properties from satellite retrievals with two aerosol data sets to calculate the all‐sky aerosol direct radiative effect (DRE), which is the mean radiative perturbation due to the presence of both natural and anthropogenic aerosols. The first aerosol data set is based upon Moderate Resolution Imaging Spectroradiometer (MODIS) and Model for Atmospheric Transport and Chemistry (MATCH) assimilation model and is largely constrained by MODIS aerosol optical depth, but it does not distinguish between anthropogenic and natural aerosols. The other aerosol data set is based upon the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model, which does not assimilate aerosol observations but predicts the anthropogenic and natural components of aerosols. Thus, we can calculate the aerosol DRF using GOCART classifications of anthropogenic and natural aerosols and the ratio of DRF to DRE. We then apply this ratio to DRE calculated using MODIS/MATCH aerosols to partition it into DRF (MODIS/MATCH DRF) by assuming that the anthropogenic fractions from GOCART are representative. The global (60°N~60°S) mean all‐sky MODIS/MATCH DRF is −0.51 Wm−2 at the top of the atmosphere (TOA), 2.51 Wm−2 within the atmosphere, and −3.02 Wm−2 at the surface. The GOCART all‐sky DRF is −0.17 Wm−2 at the TOA, 2.02 Wm−2 within the atmosphere, and −2.19 Wm−2 at the surface. The differences between MODIS/MATCH DRF and GOCART DRF are solely due to the differences in aerosol properties, since both computations use the same cloud properties and surface albedo and the same proportion of anthropogenic contributions to aerosol DRE. Aerosol optical depths simulated by the GOCART model are smaller than those in MODIS/MATCH, and aerosols in the GOCART model are more absorbing than those in MODIS/MATCH. Large difference in all‐sky TOA DRF from these two aerosol data sets highlights the complexity in determining the all‐sky DRF, since the presence of clouds amplifies the sensitivities of DRF to aerosol single‐scattering albedo and aerosol vertical distribution.

Regional and monthly and clear-sky aerosol direct radiative effect (and forcing) derived from the GlobAEROSOL-AATSR satellite aerosol product

Abstract. Using the GlobAEROSOL-AATSR dataset, estimates of the instantaneous, clear-sky, direct aerosol radiative effect and radiative forcing have been produced for the year 2006. Aerosol Robotic Network sun-photometer measurements have been used to characterise the random and systematic error in the GlobAEROSOL product for 22 regions covering the globe. Representative aerosol properties for each region were derived from the results of a wide range of literature sources and, along with the de-biased GlobAEROSOL AODs, were used to drive an offline version of the Met Office unified model radiation scheme. In addition to the mean AOD, best-estimate run of the radiation scheme, a range of additional calculations were done to propagate uncertainty estimates in the AOD, optical properties, surface albedo and errors due to the temporal and spatial averaging of the AOD fields. This analysis produced monthly, regional estimates of the clear-sky aerosol radiative effect and its uncertainty, which were combined to produce annual, global mean values of (−6.7 ± 3.9) W m−2 at the top of atmosphere (TOA) and (−12 ± 6) W m−2 at the surface. These results were then used to give estimates of regional, clear-sky aerosol direct radiative forcing, using modelled pre-industrial AOD fields for the year 1750 calculated for the AEROCOM PRE experiment. However, as it was not possible to quantify the uncertainty in the pre-industrial aerosol loading, these figures can only be taken as indicative and their uncertainties as lower bounds on the likely errors. Although the uncertainty on aerosol radiative effect presented here is considerably larger than most previous estimates, the explicit inclusion of the major sources of error in the calculations suggest that they are closer to the true constraint on this figure from similar methodologies, and point to the need for more, improved estimates of both global aerosol loading and aerosol optical properties.

Atmospheric aerosols in Amazonia and land use change: from natural biogenic to biomass burning conditions

In the wet season, a large portion of the Amazon region constitutes one of the most pristine continental areas, with very low concentrations of atmospheric trace gases and aerosol particles. However, land use change modifies the biosphere-atmosphere interactions in such a way that key processes that maintain the functioning of Amazonia are substantially altered. This study presents a comparison between aerosol properties observed at a preserved forest site in Central Amazonia (TT34 North of Manaus) and at a heavily biomass burning impacted site in south-western Amazonia (PVH, close to Porto Velho). Amazonian aerosols were characterized in detail, including aerosol size distributions, aerosol light absorption and scattering, optical depth and aerosol inorganic and organic composition, among other properties. The central Amazonia site (TT34) showed low aerosol concentrations (PM2.5 of 1.3 +/- 0.7 microg m(-3) and 3.4 +/- 2.0 microg m(-3) in the wet and dry seasons, respectively), with a median particle number concentration of 220 cm(-3) in the wet season and 2200 cm(-3) in the dry season. At the impacted site (PVH), aerosol loadings were one order of magnitude higher (PM2.5 of 10.2 +/- 9.0 microg m(-3) and 33.0 +/- 36.0 microg m(-3) in the wet and dry seasons, respectively). The aerosol number concentration at the impacted site ranged from 680 cm(-3) in the wet season up to 20 000 cm(-3) in the dry season. An aerosol chemical speciation monitor (ACSM) was deployed in 2013 at both sites, and it shows that organic aerosol account to 81% to the non-refractory PM1 aerosol loading at TT34, while biomass burning aerosols at PVH shows a 93% content of organic particles. Three years of filter-based elemental composition measurements shows that sulphate at the impacted site decreases, on average, from 12% of PM2.5 mass during the wet season to 5% in the dry season. This result corroborates the ACSM finding that the biomass burning contributed overwhelmingly to the organic fine mode aerosol during the dry season in this region. Aerosol light scattering and absorption coefficients at the TT34 site were low during the wet season, increasing by a factor of 5, approximately, in the dry season due to long range transport of biomass burning aerosols reaching the forest site in the dry season. Aerosol single scattering albedo (SSA) ranged from 0.84 in the wet season up to 0.91 in the dry. At the PVH site, aerosol scattering coefficients were 3-5 times higher in comparison to the TT34 site, an indication of strong regional background pollution, even in the wet season. Aerosol absorption coefficients at PVH were about 1.4 times higher than at the forest site. Ground-based SSA at PVH was around 0.92 year round, showing the dominance of scattering aerosol particles over absorption, even for biomass burning aerosols. Remote sensing observations from six AERONET sites and from MODIS since 1999, provide a regional and temporal overview. Aerosol Optical Depth (AOD) at 550 nm of less than 0.1 is characteristic of natural conditions over Amazonia. At the perturbed PVH site, AOD550 values greater than 4 were frequently observed in the dry season. Combined analysis of MODIS and CERES showed that the mean direct radiative forcing of aerosols at the top of the atmosphere (TOA) during the biomass burning season was -5.6 +/- 1.7 W m(-2), averaged over whole Amazon Basin. For high AOD (larger than 1) the maximum daily direct aerosol radiative forcing at the TOA was as high as -20 W m(-2) locally. This change in the radiation balance caused increases in the diffuse radiation flux, with an increase of Net Ecosystem Exchange (NEE) of 18-29% for high AOD. From this analysis, it is clear that land use change in Amazonia shows alterations of many atmospheric properties, and these changes are affecting the functioning of the Amazonian ecosystem in significant ways.

A Hemispheric Transport of Air Pollution multimodel assessment of the influence of regional anthropogenic emission reductions on aerosol direct radiative forcing and the role of intercontinental transport

A Hemispheric Transport of Air Pollution multimodel assessment of the influence of regional anthropogenic emission reductions on aerosol direct radiative forcing and the role of intercontinental transport

A multimodel assessment of the influence of regional anthropogenic emission reductions on aerosol direct radiative forcing and the role of intercontinental transport: AEROSOL INTERCONTINENTAL TRANSPORT

A multimodel assessment of the influence of regional anthropogenic emission reductions on aerosol direct radiative forcing and the role of intercontinental transport: AEROSOL INTERCONTINENTAL TRANSPORT

Comments on “direct radiative forcing of anthropogenic aerosols over oceans from satellite observation”

Previous observational studies have estimated anthropogenic aerosol direct radiative forcing over oceans without due consideration of cloudy-sky aerosols. However, when interaction between clouds and aerosols located below or above the cloud level is taken into account, the aerosol direct radiative forcing is larger by as much as 5 W m−2 in most mid-latitude regions in the Northern Hemisphere.

Effect of spectrally varying albedo of vegetation surfaces on shortwave radiation fluxes and aerosol direct radiative forcing

Abstract. This study develops an algorithm for representing detailed spectral features of vegetation albedo based on Moderate Resolution Imaging Spectrometer (MODIS) observations at 7 discrete channels, referred to as the MODIS Enhanced Vegetation Albedo (MEVA) algorithm. The MEVA algorithm empirically fills spectral gaps around the vegetation red edge near 0.7 μm and vegetation water absorption features at 1.48 and 1.92 μm which cannot be adequately captured by the MODIS 7 channels. We then assess the effects of applying MEVA in comparison to four other traditional approaches to calculate solar fluxes and aerosol direct radiative forcing (DRF) at the top of atmosphere (TOA) based on the MODIS discrete reflectance bands. By comparing the DRF results obtained through the MEVA method with the results obtained through the other four traditional approaches, we show that filling the spectral gap of the MODIS measurements around 0.7 μm based on the general spectral behavior of healthy green vegetation leads to significant improvement in the instantaneous aerosol DRF at TOA (up to 3.02 W m−2 difference or 48% fraction of the aerosol DRF, −6.28 W m−2, calculated for high spectral resolution surface reflectance from 0.3 to 2.5 μm for deciduous vegetation surface). The corrections of the spectral gaps in the vegetation spectrum in the near infrared, again missed by the MODIS reflectances, also contributes to improving TOA DRF calculations but to a much lower extent (less than 0.27 W m−2, or about 4% of the instantaneous DRF). Compared to traditional approaches, MEVA also improves the accuracy of the outgoing solar flux between 0.3 to 2.5 μm at TOA by over 60 W m−2 (for aspen 3 surface) and aerosol DRF by over 10 W m−2 (for dry grass). Specifically, for Amazon vegetation types, MEVA can improve the accuracy of daily averaged aerosol radiative forcing in the spectral range of 0.3 to 2.5 μm at equator at the equinox by 3.7 W m−2. These improvements indicate that MEVA can contribute to regional climate studies over vegetated areas and can help to improve remote sensing-based studies of climate processes and climate change.

Development of a new data-processing method for SKYNET sky radiometer observations

Abstract. In order to reduce uncertainty in the estimation of Direct Aerosol Radiative Forcing (DARF), it is important to improve the estimation of the single scattering albedo (SSA). In this study, we propose a new data processing method to improve SSA retrievals for the SKYNET sky radiometer network, which is one of the growing number of networks of sun-sky photometers, such as NASA AERONET and others. There are several reports that SSA values from SKYNET have a bias compared to those from AERONET, which is regarded to be the most accurate due to its rigorous calibration routines and data quality and cloud screening algorithms. We investigated possible causes of errors in SSA that might explain the known biases through sensitivity experiments using a numerical model, and also using real data at the SKYNET sites at Pune (18.616° N/73.800° E) in India and Beijing (39.586° N/116.229° E) in China. Sensitivity experiments showed that an uncertainty of the order of ±0.03 in the SSA value can be caused by a possible error in the ground surface albedo or solid view angle assumed for each observation site. Another candidate for possible error in the SSA was found in cirrus contamination generated by imperfect cloud screening in the SKYNET data processing. Therefore, we developed a new data quality control method to get rid of low quality or cloud contamination data, and we applied this method to the real observation data at the Pune site in SKYNET. After applying this method to the observation data, we were able to screen out a large amount of cirrus-contaminated data and to reduce the deviation in the SSA value from that of AERONET. We then estimated DARF using data screened by our new method. The result showed that the method significantly reduced the difference of 5 W m−2 that existed between the SKYNET and AERONET values of DARF before screening. The present study also suggests the necessity of preparing suitable a priori information on the distribution of coarse particles ranging in radius between 10 μm and 30 μm for the analysis of heavily dust-laden atmospheric cases.

Initial Assessment of the Spectrometer for Sky-Scanning, Sun-Tracking Atmospheric Research (4STAR)-Based Aerosol Retrieval: Sensitivity Study

The Spectrometer for Sky-Scanning, Sun-Tracking Atmospheric Research (4STAR) being developed for airborne measurements will offer retrievals of aerosol microphysical and optical properties from multi-angular and multi-spectral measurements of sky radiance and direct-beam sun transmittance. In this study, we assess the expected accuracy of the 4STAR-based aerosol retrieval and its sensitivity to major sources of anticipated perturbations in the 4STAR measurements. The major anticipated perturbations are (1) an apparent enhancement of sky radiance at small scattering angles associated with the necessarily compact design of the 4STAR and (2) an offset (i.e., uncertainty) of sky radiance calibration independent of scattering angle. The assessment is performed through application of the operational AERONET aerosol retrieval and constructed synthetic 4STAR-like data. Particular attention is given to the impact of these perturbations on the broadband fluxes and the direct aerosol radiative forcing. The results from this study suggest that limitations in the accuracy of 4STAR-retrieved particle size distributions and scattering phase functions have diminished impact on the accuracy of retrieved bulk microphysical parameters, permitting quite accurate retrievals of properties including the effective radius (up to 10%, or 0.03), and the radiatively important optical properties, such as the asymmetry factor (up to 4%, or ±0.02) and single-scattering albedo (up to 6%, or ±0.04). Also, the obtained results indicate that the uncertainties in the retrieved aerosol optical properties are quite small in the context of the calculated fluxes and direct aerosol radiative forcing (up to 15%, or 3 W∙m−2).

Sensitivity of scattering and absorbing aerosol direct radiative forcing to physical climate factors

The direct radiative forcing of the climate system includes effects due to scattering and absorbing aerosols. This study explores how important physical climate characteristics contribute to the magnitudes of the direct radiative forcings (DRF) from anthropogenic sulfate, black carbon, and organic carbon. For this purpose, we employ the GFDL CM2.1 global climate model, which has reasonable aerosol concentrations and reconstruction of twentieth‐century climate change. Sulfate and carbonaceous aerosols constitute the most important anthropogenic aerosol perturbations to the climate system and provide striking contrasts between primarily scattering (sulfate and organic carbon) and primarily absorbing (black carbon) species. The quantitative roles of cloud coverage, surface albedo, and relative humidity in governing the sign and magnitude of all‐sky top‐of‐atmosphere (TOA) forcings are examined. Clouds reduce the global mean sulfate TOA DRF by almost 50%, reduce the global mean organic carbon TOA DRF by more than 30%, and increase the global mean black carbon TOA DRF by almost 80%. Sulfate forcing is increased by over 50% as a result of hygroscopic growth, while high‐albedo surfaces are found to have only a minor (less than 10%) impact on all global mean forcings. Although the radiative forcing magnitudes are subject to uncertainties in the state of mixing of the aerosol species, it is clear that fundamental physical climate characteristics play a large role in governing aerosol direct radiative forcing magnitudes.

Aerosols in central California: Unexpectedly large contribution of coarse mode to aerosol radiative forcing

The majority of previous studies dealing with effect of coarse mode aerosols (supermicron) on the radiation budget have focused primarily on regions where total aerosol loadings are substantial. We reexamine this effect for a relatively clean area using a unique 1‐month dataset collected during the recent Carbonaceous Aerosol and Radiative Effects Study (CARES, June 2010) in the central California region near Sacramento. Here we define “clean” as aerosol optical depths less than 0.1 at 0.5μm. We demonstrate that coarse mode particles contributed substantially (more than 50%) and frequently (up to 85% of time) to the total aerosol volume during this study. In contrast to conventional expectations that the radiative impact of coarse mode aerosols should be small for clean regions, we find that neglecting large particles may lead to significant overestimation, up to 45%, of direct aerosol radiative forcing despite very small aerosol optical depths. Our findings highlight the potential for substantial impacts of coarse mode aerosols on radiative properties over clean areas and the need for more explicit inclusion of coarse mode aerosols in climate‐related observational studies.

Impacts of future air pollution mitigation strategies on the aerosol direct radiative forcing over Europe

Projections of aerosol emissions for 2030 have been recently generated and implemented in a comprehensive chemistry-transport model to analyse the future evolution of the aerosol radiative forcing over Europe. In this study, numerical developments based on an off-line coupling between the regional chemistry-transport model CHIMERE (extended by an aerosol optical module) and the radiative transfer code GAME have been implemented in order to simulate the interaction of physico-chemically resolved aerosols with radiation at regional scale. This novel approach is used to examine the shortwave aerosol direct radiative forcing response to two air pollution reduction scenarios for 2030 over Europe. Our study suggests that measures introduced to improve future air quality could have large implication on the aerosol climate forcing over Europe. Results of simulations indicate that abatement of aerosols in the near future could lead to a decrease of the aerosol cooling effect at the surface and at the top of the atmosphere over the main anthropogenic emission regions. Especially over the Moscow region, different strategies of reduction for scattering sulphate and absorbing black carbon aerosols between the two scenarios could result, however, in either a reduction or an enhancement in atmospheric radiative forcing.

Spatially Refined Aerosol Direct Radiative Forcing Efficiencies

Global aerosol direct radiative forcing (DRF) is an important metric for assessing potential climate impacts of future emissions changes. However, the radiative consequences of emissions perturbations are not readily quantified nor well understood at the level of detail necessary to assess realistic policy options. To address this challenge, here we show how adjoint model sensitivities can be used to provide highly spatially resolved estimates of the DRF from emissions of black carbon (BC), primary organic carbon (OC), sulfur dioxide (SO(2)), and ammonia (NH(3)), using the example of emissions from each sector and country following multiple Representative Concentration Pathway (RCPs). The radiative forcing efficiencies of many individual emissions are found to differ considerably from regional or sectoral averages for NH(3), SO(2) from the power sector, and BC from domestic, industrial, transportation and biomass burning sources. Consequently, the amount of emissions controls required to attain a specific DRF varies at intracontinental scales by up to a factor of 4. These results thus demonstrate both a need and means for incorporating spatially refined aerosol DRF into analysis of future emissions scenario and design of air quality and climate change mitigation policies.

Monsoon sensitivity to aerosol direct radiative forcing in the community atmosphere model

Aerosol forcing remains a dominant uncertainty in climate studies. The impact of aerosol direct radiative forcing on Indian monsoon is extremely complex and is strongly dependent on the model, aerosol distribution and characteristics specified in the model, modelling strategy employed as well as on spatial and temporal scales. The present study investigates (i) the aerosol direct radiative forcing impact on mean Indian summer monsoon when a combination of quasi-realistic mean annual cycles of scattering and absorbing aerosols derived from an aerosol transport model constrained with satellite observed Aerosol Optical Depth (AOD) is prescribed, (ii) the dominant feedback mechanism behind the simulated impact of all-aerosol direct radiative forcing on monsoon and (iii) the relative impacts of absorbing and scattering aerosols on mean Indian summer monsoon. We have used CAM3, an atmospheric GCM (AGCM) that has a comprehensive treatment of the aerosol–radiation interaction. This AGCM has been used to perform climate simulations with three different representations of aerosol direct radiative forcing due to the total, scattering aerosols and black carbon aerosols. We have also conducted experiments without any aerosol forcing. Aerosol direct impact due to scattering aerosols causes significant reduction in summer monsoon precipitation over India with a tendency for southward shift of Tropical Convergence Zones (TCZs) over the Indian region. Aerosol forcing reduces surface solar absorption over the primary rainbelt region of India and reduces the surface and lower tropospheric temperatures. Concurrent warming of the lower atmosphere over the warm oceanic region in the south reduces the land–ocean temperature contrast and weakens the monsoon overturning circulation and the advection of moisture into the landmass. This increases atmospheric convective stability, and decreases convection, clouds, precipitation and associated latent heat release. Our analysis reveals a defining negative moisture-advection feedback that acts as an internal damping mechanism spinning down the regional hydrological cycle and leading to significant circulation changes in response to external radiative forcing perturbations. When total aerosol loading (both absorbing and scattering aerosols) is prescribed, dust and black carbon aerosols are found to cause significant atmospheric heating over the monsoon region but the aerosol-induced weakening of meridional lower tropospheric temperature gradient (leading to weaker summer monsoon rainfall) more than offsets the increase in summer-time rainfall resulting from the atmospheric heating effect of absorbing aerosols, leading to a net decrease of summer monsoon rainfall. Further, we have carried out climate simulations with globally constant AODs and also with the constant AODs over the extended Indian region replaced by realistic AODs. Regional aerosol radiative forcing perturbations over the Indian region is found to have impact not only over the region of loading but over remote tropical regions as well. This warrants the need to prescribe realistic aerosol properties in strategic regions such as India in order to accurately assess the aerosol impact.

Simulation of mineral dust aerosol with Piecewise Log-normal Approximation (PLA) in CanAM4-PAM

Abstract. A new size-resolved dust scheme based on the numerical method of piecewise log-normal approximation (PLA) was developed and implemented in the fourth generation of the Canadian Atmospheric Global Climate Model with the PLA Aerosol Model (CanAM4-PAM). The total simulated annual global dust emission is 2500 Tg yr−1, and the dust mass load is 19.3 Tg for year 2000. Both are consistent with estimates from other models. Results from simulations are compared with multiple surface measurements near and away from dust source regions, validating the generation, transport and deposition of dust in the model. Most discrepancies between model results and surface measurements are due to unresolved aerosol processes. Biases in long-range transport are also contributing. Radiative properties of dust aerosol are derived from approximated parameters in two size modes using Mie theory. The simulated aerosol optical depth (AOD) is compared with satellite and surface remote sensing measurements and shows general agreement in terms of the dust distribution around sources. The model yields a dust AOD of 0.042 and dust aerosol direct radiative forcing (ADRF) of −1.24 W m−2 respectively, which show good consistency with model estimates from other studies.

Aerosol and ozone changes as forcing for climate evolution between 1850 and 2100

Global aerosol and ozone distributions and their associated radiative forcings were simulated between 1850 and 2100 following a recent historical emission dataset and under the representative concentration pathways (RCP) for the future. These simulations were used in an Earth System Model to account for the changes in both radiatively and chemically active compounds, when simulating the climate evolution. The past negative stratospheric ozone trends result in a negative climate forcing culminating at −0.15 W m−2 in the 1990s. In the meantime, the tropospheric ozone burden increase generates a positive climate forcing peaking at 0.41 W m−2. The future evolution of ozone strongly depends on the RCP scenario considered. In RCP4.5 and RCP6.0, the evolution of both stratospheric and tropospheric ozone generate relatively weak radiative forcing changes until 2060–2070 followed by a relative 30 % decrease in radiative forcing by 2100. In contrast, RCP8.5 and RCP2.6 model projections exhibit strongly different ozone radiative forcing trajectories. In the RCP2.6 scenario, both effects (stratospheric ozone, a negative forcing, and tropospheric ozone, a positive forcing) decline towards 1950s values while they both get stronger in the RCP8.5 scenario. Over the twentieth century, the evolution of the total aerosol burden is characterized by a strong increase after World War II until the middle of the 1980s followed by a stabilization during the last decade due to the strong decrease in sulfates in OECD countries since the 1970s. The cooling effects reach their maximal values in 1980, with −0.34 and −0.28 W m−2 respectively for direct and indirect total radiative forcings. According to the RCP scenarios, the aerosol content, after peaking around 2010, is projected to decline strongly and monotonically during the twenty-first century for the RCP8.5, 4.5 and 2.6 scenarios. While for RCP6.0 the decline occurs later, after peaking around 2050. As a consequence the relative importance of the total cooling effect of aerosols becomes weaker throughout the twenty-first century compared with the positive forcing of greenhouse gases. Nevertheless, both surface ozone and aerosol content show very different regional features depending on the future scenario considered. Hence, in 2050, surface ozone changes vary between −12 and +12 ppbv over Asia depending on the RCP projection, whereas the regional direct aerosol radiative forcing can locally exceed −3 W m−2.

Estimation of radiative forcing by the dust and non-dust content in mixed East Asian pollution plumes on the basis of depolarization ratios measured with lidar

The contribution of dust and non-dust aerosols to the lidar observed total backscattering was estimated from the linear particle depolarization ratios (δp) under the assumption of externally mixed aerosols. During intensive observation period, the contribution rate of the non-dust aerosol optical depth (AOD, τ) to total AOD increased from 30% on 22 October to 82% on 30 October, which implies that large amount of non-dust particles was transported along with Asian dust storm. Using independent aerosol optics and profiles for dust and non-dust, for the first time, instantaneous aerosol direct radiative forcing (ADRF) of the Asian dust plumes on atmosphere-surface system was quantified. The average ADRF by the dust particles was −31.5 ± 16.1 (−66.3 ± 20.2) W m−2 at the surface, −16.5 ± 8.8 (−11.2 ± 9.2) W m−2 at the TOA, respectively. The forcing efficiency, defined as the aerosol forcing per unit τ (532 nm), for dust (non-dust) particles was −124.6 ± 12.2 (−209.4 ± 59.1) W m−2/τ532 at the surface and −64.9 ± 7.8 (−35.1 ± 28.0) W m−2/τ532 at the TOA, respectively. Though the contribution of non-dust optical depth to total τ was smaller than the contribution of optical depth from dust to total optical depth, the non-dust particles contributed larger to the radiative forcing at the surface than the dust radiative forcing. This result demonstrates that increased Asian dust radiative forcing can be largely attributed to the presence of non-dust particles mixed into Asian dust layers rather than the radiative forcing by pure dust particles. We also found that non-dust particles play a significant role in stabilizing the dust layer by increasing the radiative heating rates within dust layers.

Aerosol direct radiative forcing based on GEOS-Chem-APM and uncertainties

Abstract. Aerosol direct radiative forcing (DRF) plays an important role in global climate change but has a large uncertainty. Here we investigate aerosol DRF with GEOS-Chem-APM, a recently developed global aerosol microphysical model that is designed to capture key particle properties (size, composition, coating of primary particles by volatile species, etc.). The model, with comprehensive chemistry, microphysics and up-to-date emission inventories, is driven by assimilated meteorology, which is presumably more realistic compared to the model-predicted meteorology. For this study, the model is extended by incorporating a radiation transfer model. Optical properties are calculated using Mie theory, where the core-shell configuration could be treated with the refractive indices from the recently updated values available in the literature. The surface albedo is taken from MODIS satellite retrievals for the simulation year, in which the data set for the 8-day mean at 0.05° (5600 m) resolution for 7 wavebands is provided. We derive the total and anthropogenic aerosol DRF, mainly focus on the results of anthropogenic aerosols, and then compare with those values reported in previous studies. In addition, we examine the anthropogenic aerosol DRF's dependence on several key factors, including the particle size of black carbon (BC) and primary organic carbon (POC), the density of BC and the mixing state. Our studies show that the anthropogenic aerosol DRF at top of atmosphere (TOA) for all sky is −0.41 W m−2. However, the sensitivity experiments suggest that the magnitude could vary from −0.08 W m−2 to −0.61 W m−2, depending on assumptions regarding the mixing state, size and density of particles.