Direct radiative effect of aerosols emitted by transport from road, shipping and aviation

Aerosols and their precursors are emitted abundantly by transport activities. Transportation constitutes one of the fastest growing activities and its growth is predicted to increase significantly in the future. Previous studies have estimated the aerosol direct radiative forcing from one transport sub-sector, but only one study to our knowledge estimated the range of radiative forcing from the main aerosol components (sulphate, black carbon (BC) and organic carbon) for the whole transportation sector. In this study, we compare results from two different chemical transport models and three radiation codes under different hypothesis of mixing: internal and external mixing using emission inventories for the year 2000. The main results from this study consist of a positive direct radiative forcing for aerosols emitted by road traffic of +20±11 mW m−2 for an externally mixed aerosol, and of +32±13 mW m−2 when BC is internally mixed. These direct radiative forcings are much higher than the previously published estimate of +3±11 mW m−2. For transport activities from shipping, the net direct aerosol radiative forcing is negative. This forcing is dominated by the contribution of the sulphate. For both an external and an internal mixture, the radiative forcing from shipping is estimated at −26±4 mW m−2. These estimates are in very good agreement with the range of a previously published one (from −46 to −13 mW m−2) but with a much narrower range. By contrast, the direct aerosol forcing from aviation is estimated to be small, and in the range −0.9 to +0.3 mW m−2.

Enhancement of the aerosol direct radiative effect by semi-volatile aerosol components: airborne measurements in North-Western Europe

A case study of atmospheric aerosol measurements exploring the impact of the vertical distribution of aerosol chemical composition upon the radiative budget in North-Western Europe is presented. Sub-micron aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS) on both an airborne platform and a ground-based site at Cabauw in the Netherlands. The examined period in May 2008 was characterised by enhanced pollution loadings in North-Western Europe and was dominated by ammonium nitrate and Organic Matter (OM). Both ammonium nitrate and OM were observed to increase with altitude in the atmospheric boundary layer. This is primarily attributed to partitioning of semi-volatile gas phase species to the particle phase at reduced temperature and enhanced relative humidity. Increased ammonium nitrate concentrations in particular were found to strongly increase the ambient scattering potential of the aerosol burden, which was a consequence of the large amount of associated water as well as the enhanced mass. During particularly polluted conditions, increases in aerosol optical depth of 50–100% were estimated to occur due to the observed increase in secondary aerosol mass and associated water uptake. Furthermore, the single scattering albedo was also shown to increase with height in the boundary layer. These enhancements combined to increase the negative direct aerosol radiative forcing by close to a factor of two at the median percentile level. Such increases have major ramifications for regional climate predictions as semi-volatile components are often not included in aerosol models. The results presented here provide an ideal opportunity to test regional and global representations of both the aerosol vertical distribution and subsequent impacts in North-Western Europe. North-Western Europe can be viewed as an analogue for the possible future air quality over other polluted regions of the Northern Hemisphere, where substantial reductions in sulphur dioxide emissions have yet to occur. Anticipated reductions in sulphur dioxide in polluted regions will result in an increase in the availability of ammonia to form ammonium nitrate as opposed to ammonium sulphate. This will be most important where intensive agricultural practises occur. Our observations over North-Western Europe, a region where sulphur dioxide emissions have already been reduced, indicate that failure to include the semi-volatile behaviour of ammonium nitrate will result in significant errors in predicted aerosol direct radiative forcing. Such errors will be particularly significant on regional scales.

Comparison of the radiative properties and direct radiative effect of aerosols from a global aerosol model and remote sensing data over ocean

A global aerosol transport model (Oslo CTM2) with main aerosol components included is compared to five satellite retrievals of aerosol optical depth (AOD) and one data set of the satellite-derived radiative effect of aerosols. The model is driven with meteorological data for the period November 1996 to June 1997 which is the time period investigated in this study. The modelled AOD is within the range of the AOD from the various satellite retrievals over oceanic regions. The direct radiative effect of the aerosols as well as the atmospheric absorption by aerosols are in both cases found to be of the order of 20 Wm−2 in certain regions in both the satellite-derived and the modelled estimates as a mean over the period studied. Satellite and model data exhibit similar patterns of aerosol optical depth, radiative effect of aerosols, and atmospheric absorption of the aerosols. Recently published results show that global aerosol models have a tendency to underestimate the magnitude of the clear-sky direct radiative effect of aerosols over ocean compared to satellite-derived estimates. However, this is only to a small extent the case with the Oslo CTM2. The global mean direct radiative effect of aerosols over ocean is modelled with the Oslo CTM2 to be –5.5 Wm−2 and the atmospheric aerosol absorption 1.5 Wm−2.

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

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)Wm−2 at the top of atmosphere (TOA) and (−12±6)Wm−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.

Mechanisms of the negative shortwave cloud feedback in mid to high latitudes

Increases in cloud optical depth and liquid water path (LWP) are robust features of global warming model simulations in high latitudes, yielding a negative shortwave cloud feedback, but the mechanisms are still uncertain. We assess the importance of microphysical processes for the negative optical depth feedback by perturbing temperature in the microphysics schemes of two aquaplanet models, both of which have separate prognostic equations for liquid water and ice. We find that most of the LWP increase with warming is caused by a suppression of ice microphysical processes in mixed-phase clouds, resulting in reduced conversion efficiencies of liquid water to ice and precipitation. Perturbing the temperature-dependent phase partitioning of convective condensate also yields a small LWP increase. Together, the perturbations in large-scale microphysics and convective condensate partitioning explain more than two-thirds of the LWP response relative to a reference case with increased SSTs, and capture all of the vertical structure of the liquid water response. In support of these findings, we show the existence of a very robust positive relationship between monthly-mean LWP and temperature in CMIP5 models and observations in mixed-phase cloud regions only. In models, the historical LWP sensitivity to temperature is a good predictor of the forced global warming response poleward of about 45°, although models appear to overestimate the LWP response to warming compared to observations. We conclude that in climate models, the suppression of ice-phase microphysical processes that deplete cloud liquid water is a key driver of the LWP increase with warming and of the associated negative shortwave cloud feedback.

Connections between clouds, radiation, and midlatitude dynamics: a review

We review the effects of dynamical variability on clouds and radiation in observations and models and discuss their implications for cloud feedbacks. Jet shifts produce robust meridional dipoles in upper-level clouds and longwave cloud-radiative effect (CRE), but low-level clouds, which do not simply shift with the jet, dominate the shortwave CRE. Because the effect of jet variability on CRE is relatively small, future poleward jet shifts with global warming are only a second-order contribution to the total CRE changes around the midlatitudes, suggesting a dominant role for thermodynamic effects. This implies that constraining the dynamical response is unlikely to reduce the uncertainty in extratropical cloud feedback. However, we argue that uncertainty in the cloud-radiative response does affect the atmospheric circulation response to global warming, by modulating patterns of diabatic forcing. How cloud feedbacks can affect the dynamical response to global warming is an important topic of future research.

Trends in the CERES dataset, 2000–13: the effects of sea ice and jet shifts and comparison to climate models

We review the effects of dynamical variability on clouds and radiation in observations and models and discuss their implications for cloud feedbacks. Jet shifts produce robust meridional dipoles in upper-level clouds and longwave cloud-radiative effect (CRE), but low-level clouds, which do not simply shift with the jet, dominate the shortwave CRE. Because the effect of jet variability on CRE is relatively small, future poleward jet shifts with global warming are only a second-order contribution to the total CRE changes around the midlatitudes, suggesting a dominant role for thermodynamic effects. This implies that constraining the dynamical response is unlikely to reduce the uncertainty in extratropical cloud feedback. However, we argue that uncertainty in the cloud-radiative response does affect the atmospheric circulation response to global warming, by modulating patterns of diabatic forcing. How cloud feedbacks can affect the dynamical response to global warming is an important topic of future research.

Observational evidence for a negative shortwave cloud feedback in middle to high latitudes

Exploiting the observed robust relationships between temperature and optical depth in extratropical clouds, we calculate the shortwave cloud feedback from historical data, by regressing observed and modeled cloud property histograms onto local temperature in middle to high southern latitudes. In this region, all CMIP5 models and observational data sets predict a negative cloud feedback, mainly driven by optical thickening. Between 45° and 60°S, the mean observed shortwave feedback (−0.91 ± 0.82 W m−2 K−1, relative to local rather than global mean warming) is very close to the multimodel mean feedback in RCP8.5 (−0.98 W m−2 K−1), despite differences in the meridional structure. In models, historical temperature-cloud property relationships reliably predict the forced RCP8.5 response. Because simple theory predicts this optical thickening with warming, and cloud amount changes are relatively small, we conclude that the shortwave cloud feedback is very likely negative in the real world at middle to high latitudes.

A case study of the direct radiative effect of biomass burning aerosols on precipitation in the Eastern Amazon

Numerical experiments with the Brazilian additions to the Regional Atmospheric Modeling System were performed with two nested grids (50 and 10 km horizontal resolution, respectively) with and without the effect of biomass burning for 8 different situations for 96 h integrations. Only the direct radiative effect of aerosols is considered. The results were analyzed in large areas encompassing the BR163 road (one of the main areas of deforestation in the Amazon). mainly where most of the burning takes place. The precipitation change due to the direct radiative impact of biomass burning is generally negative (i.e., there is a decrease of precipitation). However, there are a few cases with a positive impact. Two opposite forcing mechanisms were explored: (a) the thermodynamic forcing that is generally negative in the sense that the aerosol tends to stabilize the lower atmosphere and (b) the dynamic impact associated with the low level horizontal pressure gradients produced by the aerosol plumes. In order to understand the non-linear relationship between the two effects, experiments were performed with 4-fold emissions. In these cases, the dynamic effect overcomes the stabilization produced by the radiative forcing and precipitation increase is observed in comparison with the control experiment. This study suggests that. in general, the biomass burning radiative forcing decreases the precipitation. However, very large concentrations of aerosols may lead to an increase of precipitation due to the dynamical forcing associated with the horizontal pressure gradients. (C) 2009 Elsevier B.V. All rights reserved.

Aerosol-cloud interactions studied with a chemistry-climate model

This study aims at a comprehensive understanding of the effects of aerosol-cloud interactions and their effects on cloud properties and climate using the chemistry-climate model EMAC. In this study, CCN activation is regarded as the dominant driver in aerosol-cloud feedback loops in warm clouds. The CCN activation is calculated prognostically using two different cloud droplet nucleation parameterizations, the STN and HYB CDN schemes. Both CDN schemes account for size and chemistry effects on the droplet formation based on the same aerosol properties. The calculation of the solute effect (hygroscopicity) is the main difference between the CDN schemes. The kappa-method is for the first time incorporated into Abdul-Razzak and Ghan activation scheme (ARG) to calculate hygroscopicity and critical supersaturation of aerosols (HYB), and the performance of the modied scheme is compared with the osmotic coefficient model (STN), which is the standard in the ARG scheme. Reference simulations (REF) with the prescribed cloud droplet number concentration have also been carried out in order to understand the effects of aerosol-cloud feedbacks. In addition, since the calculated cloud coverage is an important determinant of cloud radiative effects and is influencing the nucleation process two cloud cover parameterizations (i.e., a relative humidity threshold; RH-CLC and a statistical cloud cover scheme; ST-CLC) have been examined together with the CDN schemes, and their effects on the simulated cloud properties and relevant climate parameters have been investigated. The distinct cloud droplet spectra show strong sensitivity to aerosol composition effects on cloud droplet formation in all particle sizes, especially for the Aitken mode. As Aitken particles are the major component of the total aerosol number concentration and CCN, and are most sensitive to aerosol chemical composition effect (solute effect) on droplet formation, the activation of Aitken particles strongly contribute to total cloud droplet formation and thereby providing different cloud droplet spectra. These different spectra influence cloud structure, cloud properties, and climate, and show regionally varying sensitivity to meteorological and geographical condition as well as the spatiotemporal aerosol properties (i.e., particle size, number, and composition). The changes responding to different CDN schemes are more pronounced at lower altitudes than higher altitudes. Among regions, the subarctic regions show the strongest changes, as the lower surface temperature amplifies the effects of the activated aerosols; in contrast, the Sahara desert, where is an extremely dry area, is less influenced by changes in CCN number concentration. The aerosol-cloud coupling effects have been examined by comparing the prognostic CDN simulations (STN, HYB) with the reference simulation (REF). Most pronounced effects are found in the cloud droplet number concentration, cloud water distribution, and cloud radiative effect. The aerosol-cloud coupling generally increases cloud droplet number concentration; this decreases the efficiency of the formation of weak stratiform precipitation, and increases the cloud water loading. These large-scale changes lead to larger cloud cover and longer cloud lifetime, and contribute to high optical thickness and strong cloud cooling effects. This cools the Earth's surface, increases atmospheric stability, and reduces convective activity. These changes corresponding to aerosol-cloud feedbacks are also differently simulated depending on the cloud cover scheme. The ST-CLC scheme is more sensitive to aerosol-cloud coupling, since this scheme uses a tighter linkage of local dynamics and cloud water distributions in cloud formation process than the RH-CLC scheme. For the calculated total cloud cover, the RH-CLC scheme simulates relatively similar pattern to observations than the ST-CLC scheme does, but the overall properties (e.g., total cloud cover, cloud water content) in the RH simulations are overestimated, particularly over ocean. This is mainly originated from the difference in simulated skewness in each scheme: the RH simulations calculate negatively skewed distributions of cloud cover and relevant cloud water, which is similar to that of the observations, while the ST simulations yield positively skewed distributions resulting in lower mean values than the RH-CLC scheme does. The underestimation of total cloud cover over ocean, particularly over the intertropical convergence zone (ITCZ) relates to systematic defficiency of the prognostic calculation of skewness in the current set-ups of the ST-CLC scheme.rnOverall, the current EMAC model set-ups perform better over continents for all combinations of the cloud droplet nucleation and cloud cover schemes. To consider aerosol-cloud feedbacks, the HYB scheme is a better method for predicting cloud and climate parameters for both cloud cover schemes than the STN scheme. The RH-CLC scheme offers a better simulation of total cloud cover and the relevant parameters with the HYB scheme and single-moment microphysics (REF) than the ST-CLC does, but is not very sensitive to aerosol-cloud interactions.