Biomass smoke from southern Africa can significantly enhance the brightness of stratocumulus over the southeastern Atlantic Ocean.

Marine stratocumulus clouds cover nearly one-quarter of the ocean surface and thus play an extremely important role in determining the global radiative balance. The semipermanent marine stratocumulus deck over the southeastern Atlantic Ocean is of particular interest, because of its interactions with seasonal biomass burning aerosols that are emitted in southern Africa. Understanding the impacts of biomass burning aerosols on stratocumulus clouds and the implications for regional and global radiative balance is still very limited. Previous studies have focused on assessing the magnitude of the warming caused by solar scattering and absorption by biomass burning aerosols over stratocumulus (the direct radiative effect) or cloud adjustments to the direct radiative effect (the semidirect effect). Here, using a nested modeling approach in conjunction with observations from multiple satellites, we demonstrate that cloud condensation nuclei activated from biomass burning aerosols entrained into the stratocumulus (the microphysical effect) can play a dominant role in determining the total radiative forcing at the top of the atmosphere, compared with their direct and semidirect radiative effects. Biomass burning aerosols over the region and period with heavy loadings can cause a substantial cooling (daily mean -8.05 W m-2), primarily as a result of clouds brightening by reducing the cloud droplet size (the Twomey effect) and secondarily through modulating the diurnal cycle of cloud liquid water path and coverage (the cloud lifetime effect). Our results highlight the importance of realistically representing the interactions of stratocumulus with biomass burning aerosols in global climate models in this region.

Mechanism of SOA formation determines magnitude of radiative effects.

Secondary organic aerosol (SOA) nearly always exists as an internal mixture, and the distribution of this mixture depends on the formation mechanism of SOA. A model is developed to examine the influence of using an internal mixing state based on the mechanism of formation and to estimate the radiative forcing of SOA in the future. For the present day, 66% of SOA is internally mixed with sulfate, while 34% is internally mixed with primary soot. Compared with using an external mixture, the direct effect of SOA is decreased due to the decrease in total aerosol surface area and the increase of absorption efficiency. Aerosol number concentrations are sharply reduced, and this is responsible for a large decrease in the cloud albedo effect. Internal mixing decreases the radiative effect of SOA by a factor of >4 compared with treating SOA as an external mixture. The future SOA burden increases by 24% due to CO2 increases and climate change, leading to a total (direct plus cloud albedo) radiative forcing of -0.05 W m-2 When the combined effects of changes in climate, anthropogenic emissions, and land use are included, the SOA forcing is -0.07 W m-2, even though the SOA burden only increases by 6.8%. This is caused by the substantial increase of SOA associated with sulfate in the Aitken mode. The Aitken mode increase contributes to the enhancement of first indirect radiative forcing, which dominates the total radiative forcing.

Improving our fundamental understanding of the role of aerosol-cloud interactions in the climate system.

The effect of an increase in atmospheric aerosol concentrations on the distribution and radiative properties of Earth's clouds is the most uncertain component of the overall global radiative forcing from preindustrial time. General circulation models (GCMs) are the tool for predicting future climate, but the treatment of aerosols, clouds, and aerosol-cloud radiative effects carries large uncertainties that directly affect GCM predictions, such as climate sensitivity. Predictions are hampered by the large range of scales of interaction between various components that need to be captured. Observation systems (remote sensing, in situ) are increasingly being used to constrain predictions, but significant challenges exist, to some extent because of the large range of scales and the fact that the various measuring systems tend to address different scales. Fine-scale models represent clouds, aerosols, and aerosol-cloud interactions with high fidelity but do not include interactions with the larger scale and are therefore limited from a climatic point of view. We suggest strategies for improving estimates of aerosol-cloud relationships in climate models, for new remote sensing and in situ measurements, and for quantifying and reducing model uncertainty.

Radiative forcing associated with particulate carbon emissions resulting from the use of mercury control technology.

Injection of powdered activated carbon (PAC) adsorbents into the flue gas of coal fired power plants with electrostatic precipitators (ESPs) is the most mature technology to control mercury emissions for coal combustion. However, the PAC itself can penetrate ESPs to emit into the atmosphere. These emitted PACs have similar size and optical properties to submicron black carbon (BC) and thus could increase BC radiative forcing unintentionally. The present paper estimates, for the first time, the potential emission of PAC together with their climate forcing. The global average maximum potential emissions of PAC is 98.4 Gg/yr for the year 2030, arising from the assumed adoption of the maximum potential PAC injection technology, the minimum collection efficiency, and the maximum PAC injection rate. These emissions cause a global warming of 2.10 mW m(-2) at the top of atmosphere and a cooling of -2.96 mW m(-2) at the surface. This warming represents about 2% of the warming that is caused by BC from direct fossil fuel burning and 0.86% of the warming associated with CO2 emissions from coal burning in power plants. Its warming is 8 times more efficient than the emitted CO2 as measured by the 20-year-integrated radiative forcing per unit of carbon input (the 20-year Global Warming Potential).

Satellite methods underestimate indirect climate forcing by aerosols.

Satellite-based estimates of the aerosol indirect effect (AIE) are consistently smaller than the estimates from global aerosol models, and, partly as a result of these differences, the assessment of this climate forcing includes large uncertainties. Satellite estimates typically use the present-day (PD) relationship between observed cloud drop number concentrations (N(c)) and aerosol optical depths (AODs) to determine the preindustrial (PI) values of N(c). These values are then used to determine the PD and PI cloud albedos and, thus, the effect of anthropogenic aerosols on top of the atmosphere radiative fluxes. Here, we use a model with realistic aerosol and cloud processes to show that empirical relationships for ln(N(c)) versus ln(AOD) derived from PD results do not represent the atmospheric perturbation caused by the addition of anthropogenic aerosols to the preindustrial atmosphere. As a result, the model estimates based on satellite methods of the AIE are between a factor of 3 to more than a factor of 6 smaller than model estimates based on actual PD and PI values for N(c). Using ln(N(c)) versus ln(AI) (Aerosol Index, or the optical depth times angstrom exponent) to estimate preindustrial values for N(c) provides estimates for N(c) and forcing that are closer to the values predicted by the model. Nevertheless, the AIE using ln(N(c)) versus ln(AI) may be substantially incorrect on a regional basis and may underestimate or overestimate the global average forcing by 25 to 35%.

Observational evidence of a change in radiative forcing due to the indirect aerosol effect.

Anthropogenic aerosols enhance cloud reflectivity by increasing the number concentration of cloud droplets, leading to a cooling effect on climate known as the indirect aerosol effect. Observational support for this effect is based mainly on evidence that aerosol number concentrations are connected with droplet concentrations, but it has been difficult to determine the impact of these indirect effects on radiative forcing. Here we provide observational evidence for a substantial alteration of radiative fluxes due to the indirect aerosol effect. We examine the effect of aerosols on cloud optical properties using measurements of aerosol and cloud properties at two North American sites that span polluted and clean conditions-a continental site in Oklahoma with high aerosol concentrations, and an Arctic site in Alaska with low aerosol concentrations. We determine the cloud optical depth required to fit the observed shortwave downward surface radiation. We then use a cloud parcel model to simulate the cloud optical depth from observed aerosol properties due to the indirect aerosol effect. From the good agreement between the simulated indirect aerosol effect and observed surface radiation, we conclude that the indirect aerosol effect has a significant influence on radiative fluxes.

Decrease in radiative forcing by organic aerosol nucleation, climate, and land use change.

Organic nucleation is an important source of atmospheric aerosol number concentration, especially in pristine continental regions and during the preindustrial period. Here, we improve on previous simulations that overestimate boundary layer nucleation in the tropics and add changes to climate and land use to evaluate climate forcing. Our model includes both pure organic nucleation and heteromolecular nucleation of sulfuric acid and organics and reproduces the profile of aerosol number concentration measured in the Amazon. Organic nucleation decreases the sum of the total aerosol direct and indirect radiative forcing by 12.5%. The addition of climate and land use change decreases the direct radiative forcing (-0.38 W m-2) by 6.3% and the indirect radiative forcing (-1.68 W m-2) by 3.5% due to the size distribution and number concentration change of secondary organic aerosol and sulfate. Overall, the total radiative forcing associated with anthropogenic aerosols is decreased by 16%.

Radiative forcing by light-absorbing aerosols of pyrogenetic iron oxides.

Iron (Fe) oxides in aerosols are known to absorb sun light and heat the atmosphere. However, the radiative forcing (RF) of light-absorbing aerosols of pyrogenetic Fe oxides is ignored in climate models. For the first time, we use a global chemical transport model and a radiative transfer model to estimate the RF by light-absorbing aerosols of pyrogenetic Fe oxides. The model results suggest that strongly absorbing Fe oxides (magnetite) contribute a RF that is about 10% of the RF due to black carbon (BC) over East Asia. The seasonal average of the RF due to dark Fe-rich mineral particles over East Asia (0.4-1.0 W m-2) is comparable to that over major biomass burning regions. This additional warming effect is amplified over polluted regions where the iron and steel industries have been recently developed. These findings may have important implications for the projection of the climate change, due to the rapid growth in energy consumption of the heavy industry in newly developing countries.

Anthropogenic Aerosol Indirect Effects in Cirrus Clouds.

We have implemented a parameterization for forming ice in large-scale cirrus clouds that accounts for the changes in updrafts associated with a spectrum of waves acting within each time step in the model. This allows us to account for the frequency of homogeneous and heterogeneous freezing events that occur within each time step of the model and helps to determine more realistic ice number concentrations as well as changes to ice number concentrations. The model is able to fit observations of ice number at the lowest temperatures in the tropical tropopause but is still somewhat high in tropical latitudes with temperatures between 195°K and 215°K. The climate forcings associated with different representations of heterogeneous ice nuclei (IN or INPs) are primarily negative unless large additions of IN are made, such as when we assumed that all aircraft soot acts as an IN. However, they can be close to zero if it is assumed that all background dust can act as an INP irrespective of how much sulfate is deposited on these particles. Our best estimate for the forcing of anthropogenic aircraft soot in this model is -0.2 ± 0.06 W/m2, while that from anthropogenic fossil/biofuel soot is -0.093 ± 0.033 W/m2. Natural and anthropogenic open biomass burning leads to a net forcing of -0.057 ± 0.05 W/m2.

SAM-CAAM: A Concept for Acquiring Systematic Aircraft Measurements to Characterize Aerosol Air Masses.

A modest operational program of systematic aircraft measurements can resolve key satellite-aerosol-data-record limitations. Satellite observations provide frequent, global aerosol-amount maps, but offer only loose aerosol property constraints needed for climate and air quality applications. We define and illustrate the feasibility of flying an aircraft payload to measure key aerosol optical, microphysical, and chemical properties in situ. The flight program could characterize major aerosol air-mass types statistically, at a level-of-detail unobtainable from space. It would: (1) enhance satellite aerosol retrieval products with better climatology assumptions, and (2) improve translation between satellite-retrieved optical properties and species-specific aerosol mass and size simulated in climate models to assess aerosol forcing, its anthropogenic components, and other environmental impacts. As such, Systematic Aircraft Measurements to Characterize Aerosol Air Masses (SAM-CAAM) could add value to data records representing several decades of aerosol observations from space, improve aerosol constraints on climate modeling, help interrelate remote-sensing, in situ, and modeling aerosol-type definitions, and contribute to future satellite aerosol missions. Fifteen Required Variables are identified, and four Payload Options of increasing ambition are defined, to constrain these quantities. "Option C" could meet all the SAM-CAAM objectives with about 20 instruments, most of which have flown before, but never routinely several times per week, and never as a group. Aircraft integration, and approaches to data handling, payload support, and logistical considerations for a long-term, operational mission are discussed. SAM-CAAM is feasible because, for most aerosol sources and specified seasons, particle properties tend to be repeatable, even if aerosol loading varies.