How Aerosols Affect the Global Climate and the Relation to Climate Sensitivity Gunnar Myhre, Cathrine E. Lund Myhre, Bjørn H. Samset, Trude Storelvmo Article Preview/”Teaser” (max 165 words) Atmospheric aerosols are part of the human influence on climate, and limited understanding of their effects is a major source of uncertainty in our knowledge about climate change. Aerosols enter the atmosphere from both anthropogenic and natural sources and affect the global radiation balance depending on their sizes and chemical composition. We describe the complexity associated with aerosols, from emissions to climatic effects, and illustrate their importance for the global climate sensitivity. We also show how the aerosol size distribution and chemical composition vary globally due to the multitude of available sources. Finally we describe recent progress in the understanding of aerosol climatic effects and insights into the prevailing uncertainties. What is the source of the aerosols? Atmospheric aerosols are suspensions of liquid, solid, or mixed particles with highly variable chemical composition and size. The variability is due to the numerous sources and varying formation mechanisms (Figure 1). Aerosols are mainly emitted directly to the atmosphere ( primary aerosols) or produced in the atmosphere from precursor gases (secondary aerosols), but may also be influenced by evaporation of clouds (cloud processing). Primary aerosols have both inorganic and organic sources. Inorganic primary aerosols are relatively large (often larger than 1 m) and result from sea spray, mineral dust, and volcanoes. These coarse aerosols have short atmospheric life times, typically less than a few days. Primary aerosols with carbonaceous constituents stem from plant/microbial materials, combustion processes, and biomass burning. The carbonaceous primary aerosols include both organic carbon (OC) in aqueous phase and solid black carbon (BC). BC is the light-absorbing carbonaceous fraction present in aerosols. This compound is of particular importance for climate. The main sources are combustion processes of organic material and fires, but domestic sources (cooking) are also very important in certain regions. Primary BC and OC containing aerosols are generally smaller than 1 m. Secondary aerosols are produced in the atmosphere from precursor gases by condensation of vapours from the gas phase on pre-existing particles or by nucleation of new particles. Secondary aerosols are small; they range in size from a few nanometres up to 1 m and have lifetimes of days to weeks. Secondary aerosols consist of mixtures of compounds; the main components are sulphate, nitrates, and OC. The main precursor gases are anthropogenic emissions from fossil fuel combustion, but fires and biogenic emissions of volatile organic compounds (VOCs) are also important. Occasionally volcanic eruptions result in huge amounts of aerosols both at the ground and in the stratosphere: the volcanic eruption of Mt Pinatubo in 1991 resulted in high concentrations of secondary sulphate aerosols in the stratosphere during the following years. The size and chemical composition of the aerosols evolve with time through coagulation and condensation. Mixing of different aerosol types is of importance for their climate effect. The aerosols may grow by uptake of water, a process which depends on chemical composition, aerosol size, and ambient relative humidity. Figure 1: Atmospheric aerosols: their dominating sources, typical structure, and appearance in the atmosphere. A mixture of aerosol pollution is shown at the top: the picture to the left shows urban aerosol pollution and the picture to the right shows aerosol pollution from the India and Bangladesh region. The main natural and anthropogenic sources are, from the top left corner and counterclockwise: The volcanic eruption of Grimsvotn, 21 May 2011, emitting primary volcanic ash and SO2 resulting in sulphate aerosols. Sea spray, illustrating sea salt aerosols and secondary sulphate aerosols from dimethyl sulphide. Desert storm in Iraq, 26 April 2005 showing mineral dust aerosols. Savannah biomass burning, illustrating both anthropogenic and natural fires as sources of OC and BC containing aerosols. Coal power plants, illustrating secondary sulphate aerosols and other industrial and fossil aerosol sources. Ship in a Norwegian fjord resulting in aerosols containing OC, BC, sulphates, and nitrates. Cooking, representing a large domestic source of BC and OC. A truck, representing the transport sector and emissions of BC and VOCs yielding OC in aerosols. The core of the figure shows examples of aerosol structures illustrated by an electron microscope image of black carbon attached to sulphate particles. The spherical structures in image A are sulphates; the arrows point to smaller chains of black carbon. Black carbon is shown in detail in image B. Image C shows fly ash, a product of coal-combustion,. Credit for microscope picture: Peter Buseck, Arizona State University. How are aerosols distributed globally? Figure 2 shows the aerosol optical depth (AOD) determined by remote sensing from space by the MODIS instrument. The AOD pattern is highly inhomogeneous, with the largest values in the tropical regions in Africa and Asia. The pie charts show the contributions from different aerosol types in selected regions. In general there is large variability in the global aerosol composition. The different aerosol species have varying impacts in the atmosphere, and the wide spread of both sources and sizes further complicates a quantification of their effects. Remote sensing from both space and the ground has substantially advanced the understanding of the total aerosol distribution, but there are still large uncertainties in the chemical composition and the anthropogenic contribution to the observed AOD. Figure 2: MODIS aerosol optical depth (AOD) averaged over the 10 year period 2001–2010 (Remer et al., 2008). AOD is the column integrated aerosol extinction, where extinction is the attenuation of solar light given in terms of length (m-1).The contribution to the total AOD from different aerosol types in selected regions, as indicated on the figure (pie charts), is estimated by use of a global aerosol model based on a simulation for one year (Myhre et al., 2009). The aerosol types are Sul (sulphate), BC and OC from use of fossil fuel, Bio (OC and BC from biomass burning), Nitrate, Sea (sea salt), and Min (mineral dust). Water uptake of the aerosols is taken into account and enhances the radiative properties of some of the aerosol types substantially, e.g. sulphate aerosols, which increase in size due to hygroscopic growth. In the grey areas there is no data available from MODIS. How do aerosols affect the climate? All atmospheric aerosols scatter incoming solar radiation, and a few aerosol types can also absorb solar radiation. BC is the most important of the latter, but mineral dust and some OC types are also solar absorbers. Aerosols which mainly scatter solar radiation have a cooling effect, by enhancing the total reflected solar radiation from the Earth. Strongly absorbing aerosols have a warming effect. In the atmosphere there is a mixture of scattering and absorbing aerosols, and the degree of scattering is quite variable. It is quantified through the single scattering albedo = s/, where s is scattering AOD and is total AOD. The net effect of the scattering and absorbing aerosols is dependent on surface and cloud characteristics. Scattering aerosols above a dark surface and absorbing aerosols above a bright surface are most efficient (see Figure 3a). Scattering aerosol above a bright surface is less efficient since the solar radiation is reflected anyway; similarly for absorbing aerosol and a dark surface, the solar radiation will be to a large extent absorbed. Since clouds are the main contributors to the total reflection of solar radiation, absorbing aerosols are particularly efficient when positioned above clouds. Aerosols are vital for cloud formation, acting as sources of cloud condensation nuclei (CCN) and ice nuclei (IN). An increased amount of aerosols may increase the CCN number concentration and lead to more, but smaller, cloud droplets. This increases the albedo of the cloud, resulting in enhanced reflection and a cooling effect, termed the cloud albedo or first indirect effect (Twomey, 1977); see Figure 3b). Smaller and more numerous cloud droplets may also inhibit the precipitation process, since many similarly sized cloud droplets reduce the growth to cloud droplets necessary for initiation of precipitation. This effect, called the cloud lifetime or second indirect effect, may enhance the cloud cover and also has a cooling effect (Albrecht, 1989). Absorbing aerosols also have the potential to modify clouds properties, without directly acting as CCN and IN, by: i) reducing the solar radiation reaching the ground, which diminishes the convection and thus the potential for cloud formation, ii) changing the temperature profile, which will in most cases lead to reduced instability and weakened cloud formation, iii) increasing the temperature, which reduces the relative humidity, inhibits cloud formation, and enhances evaporation of existing clouds. This is termed the semi-direct aerosol effect (Hansen et al., 1997). The net effect is uncertain and depends highly on the vertical profile of BC (Koch and Del Genio, 2010). In addition BC (and other absorbing aerosols) deposited on snow or ice surfaces may reduce the albedo, leading to reduced reflectance of solar radiation, and hence a heating effect (Hansen and Nazarenko, 2004). Figure 3: a) An illustration of the direct aerosol effect for low surface albedo (in this example zero surface albedo) and high surface albedo (in this example all solar radiation is reflected and surface albedo equals one) for scattering and absorbing aerosols. A dark surface (i.e. low surface albedo) will absorb a large portion of the solar radiation, and absorbing aerosols will thus have a small effect since solar radiation is absorbed anyway. On the other hand, scattering aerosols may substantially amplify the total reflectance of solar radiation since the solar radiation will otherwise be absorbed at the surface. Similarly over a bright surface (high surface albedo), scattering aerosols have a small effect since the solar radiation is scattered anyway. Absorbing aerosol may however substantially reduce the outgoing radiation under such conditions and has a warming effect. b) Illustration of the first indirect aerosol effect (cloud albedo effect), second indirect aerosol effect (cloud lifetime effect), and semi-direct effect. Different sizes of cloud droplets, cloud fraction, and initiation of the precipitation process are shown. Why is the uncertainty in the aerosols important for predictions of the climate sensitivity? The change in temperature (T) as a result of radiative forcing (RF, a change in the Earth’s radiation balance due to a perturbation of anthropogenic or natural origin) can be expressed by the following simple heat balance equation: c d(T)/dt = RF -T (1) Here c is the heat capacity and is the climate sensitivity. At radiative equilibrium (d(T)/dt = 0), Equation 1 reduces to T = RF/. However the Earth is not in radiative equilibrium, since less thermal radiation is currently emitted to space compared to what is absorbed of solar radiation (Hansen et al., 2005). This radiative imbalance causes the Earth to gradually warm, with global warming as a result (Trenberth and Fasullo, 2010). The simple equation above has two key uncertainties. The observed surface temperature change is rather well determined, but the climate sensitivity and the total RF are both highly uncertain. Quantifying the climate sensitivity , an essential parameter for prediction of future climate change, has long been attempted by using global climate models or temperature records, but it still has a wide range of reported values (IPCC, 2007; Knutti and Hegerl, 2008). The total RF through the industrial era is also uncertain, mainly due to lack of quantification of the aerosol effects discussed above. The implication of this uncertainty in the aerosol RF for the quantification of the climate sensitivity can be illustrated as follows: Figure 4a shows the climate sensitivity as a function of the total aerosol RF (shown for both the most certain aerosol effects and a more comprehensive set of aerosol effects), where uncertainties in the radiative imbalance are included. A similar figure has previously been presented in Andreae et al. (2005). The figure shows that using the known industrial age warming of around 0.8K and the present best knowledge on RF from non-aerosol components, radiative imbalance and the 90% confidence interval of the total aerosol RF for the most certain effect, we can get a climate sensitivity range from about 2 to 8 K for a doubling of CO2. Figure 4b breaks down the total aerosol forcing probability density function (PDF) into individual components, indicating both the magnitudes and uncertainties of the effects. Figure 4: a) Climate sensitivity for a doubling of CO2 as a function of the total aerosol RF. The curve is shown for a best estimate of the radiative imbalance of 0.85 Wm-2 (Hansen et al., 2005) with grey shading for imbalances between 0.7 and 1.0 Wm-2 representing the uncertainty. A thin dotted line for radiative imbalance of zero (radiative equilibrium) is added. The observed temperature change is taken as 0.8 K and radiative forcing of non-aerosol components is 2.9 Wm-2 over the industrial era. The red line shows the probability density function (PDF) for the total of the direct aerosol, cloud albedo effect, and the BC on snow and ice, whereas the dotted red line shows the total of all aerosol effects. b) PDFs of various aerosol effects taken from Isaksen et al. (2009), except a small update for the cloud albedo effect; the range for the cloud lifetime effect is here estimated to be somewhat weaker, and for the mixed phase and ice clouds recent studies are taken into account to narrow the range somewhat. Monte Carlo simulations are performed to derive total aerosol RF, shown as the red curves (Boucher and Haywood, 2001). Has there been any progress in the understanding of the climate effect of aerosol? There has been a tremendous improvement in the understanding of atmospheric aerosols and their climate effect over the last decades, with some important observational and modelling breakthroughs. Long term measurements of aerosols (e.g.Putaud et al., 2004), observational campaigns (e.g.Quinn and Bates, 2005), and remote sensing from space and ground (Holben et al., 1998; Remer et al., 2008) have remarkably increased the knowledge about the atmospheric aerosol composition and characteristics. However, the understanding of the greater complexity of atmospheric aerosols has at the same time limited more robust quantification of their climate effect. The first estimate of the direct aerosol effect in the early 1990s was limited to sulphate aerosols (Charlson et al., 1991), with estimates for BC coming a few years later (Haywood and Shine, 1995). Observations have shown that OC is an important aerosol component (Novakov et al., 1997; Ramanathan et al., 2001) and substantial investigations have later explored the complex composition and optical characteristics of this compound (e.g.Graber and Rudich, 2006; Kanakidou et al., 2005). Global aerosol models today provide RF estimates for a large set of aerosol components such as sulphate, BC (from fossil fuel and biomass burning), OC (primary and secondary from fossil fuel and biomass burning), nitrate (Jacobson, 2001; Koch et al., 2009; Liao and Seinfeld, 2005). In addition multi-model studies are performed to understand and reduce uncertainties due to model differences (Schulz et al., 2006). An example of recent progress is reduced uncertainty in the estimate of the total direct aerosol effect given by IPCC AR4 (Forster et al., 2007). This estimate was made possible by the advances that have occurred on both the modelling and the observational side, and was based on a combination of global aerosol models and observation based methods (mostly sensed data). Initially, the two approaches gave conflicting results, the observation based methods yielding a stronger RF than the models. Consistency between these two different approaches has later been reached, and was found to arise from necessary and simplified assumptions of the pre-industrial aerosol composition in the observation based method (Myhre, 2009). Although the uncertainty in the total direct aerosol effect is reduced, the uncertainty for several of the aerosol components such as BC, OC, and nitrate is still large. Similar to the early estimates of the direct aerosol effect, many of the first model estimates of the aerosol indirect effect only accounted for the effect of sulphate particles acting as CCN (Jones et al., 1994; Kaufman and Chou, 1993). Furthermore, they only included the influence of sulphate aerosols on cloud albedo, disregarding any effects on cloud lifetime and extent. With the realization that other aerosol species of anthropogenic origin could also form cloud droplets and that effects on cloud lifetime and extent were also possible, global climate models estimated the aerosol indirect effect to be stronger (e.g.Lohmann and Feichter, 1997; Menon et al., 2002). Some even predicted this cooling effect to be comparable in magnitude to the warming greenhouse effect. Recent publications have later pointed to oversimplifications in the model representation of clouds and how their lifetimes are affected by aerosols (e.g.Stevens and Feingold, 2009). It is now acknowledged that aerosol effects on cloud lifetime will vary with the cloud type in question. For example, a few recent model studies have found that by forming ice in super-cooled liquid clouds, aerosols may in fact shorten cloud lifetime, because of the more efficient precipitation formation when cloud ice is present (e.g.Lohmann and Hoose, 2009; Storelvmo et al., 2011). In summary, whether aerosols are acting as CCN or IN or are simply modifying atmospheric stability by absorbing solar radiation, there is still high uncertainty associated with their effect on cloud lifetime. In contrast, model and satellite estimates of the cloud albedo effect seem to agree on a negative RF that has about half the magnitude of the positive RF attributed to increasing CO2 concentrations. Albrecht, B. A. Aerosols, Cloud Microphysics, And Fractional Cloudiness. Science 245, 1227-1230 (1989). Andreae, M. O., Jones, C. D. and Cox, P. M. Strong present-day aerosol cooling implies a hot future. Nature 435, 1187-1190 (2005). Boucher, O. and Haywood, J. On summing the components of radiative forcing of climate change. Climate Dynamics 18, 297-302 (2001). Charlson, R. J., Langner, J., Rodhe, H. et al. Perturbation of the Northern-Hemisphere Radiative Balance by Backscattering from Anthropogenic Sulfate Aerosols. Tellus Series A-Dynamic Meteorology and Oceanography 43, 152-163 (1991). Forster, P., Ramaswamy, V., Artaxo, P. et al., 2007. Changes in Atmospheric Constituents and in Radiative Forcing, Climate Change 2007: The Physical Science Basis. Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change. Cambridge University Press, Cambridge, United Kingdom and New York, NY, USA. Graber, E. R. and Rudich, Y. Atmospheric HULIS: How humic-like are they? A comprehensive and critical review. Atmospheric Chemistry and Physics 6, 729-753 (2006). Hansen, J. and Nazarenko, L. Soot climate forcing via snow and ice albedos. Proceedings of the National Academy of Sciences of the United States of America 101, 423-428 (2004). Hansen, J., Nazarenko, L., Ruedy, R. et al. Earth's energy imbalance: Confirmation and implications. Science 308, 1431-1435 (2005). Hansen, J., Sato, M. and Ruedy, R. Radiative forcing and climate response. Journal of Geophysical Research-Atmospheres 102, 6831-6864 (1997). Haywood, J. M. and Shine, K. P. The effect of anthropogenic sulfate and soot aerosol on the clear-sky planetary radiation budget. Geophysical Research Letters 22, 603-606 (1995). Holben, B. N., Eck, T. F., Slutsker, I. et al. AERONET - A federated instrument network and data archive for aerosol characterization. Remote Sensing of Environment 66, 1-16 (1998). IPCC, 2007. The Physical Science Basis. Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change Cambridge University Press, Cambridge, United Kingdom and New York, NY, USA. Isaksen, I., Granier, C., Myhre, G. et al. Atmospheric composition change: Climate-Chemistry interactions. Atmospheric Environment, 5138-5192 (2009). Jacobson, M. Z. Global direct radiative forcing due to multicomponent anthropogenic and natural aerosols. Journal of Geophysical Research-Atmospheres 106, 1551-1568 (2001). Jones, A., Roberts, D. L. and Slingo, A. A climate model study of indirect radiative forcing by anthropogenic sulfate aerosols. Nature 370, 450-453 (1994). Kanakidou, M., Seinfeld, J. H., Pandis, S. N. et al. Organic aerosol and global climate modelling: a review. Atmospheric Chemistry and Physics 5, 1053-1123 (2005). Kaufman, Y. J. and Chou, M. D. Model simulations of the competing climatic effects of SO2 and CO2 Journal of Climate 6, 1241-1252 (1993). Knutti, R. and Hegerl, G. C. The equilibrium sensitivity of the Earth's temperature to radiation changes. Nature Geoscience 1, 735-743 (2008). Koch, D. and Del Genio, A. D. Black carbon semi-direct effects on cloud cover: review and synthesis. Atmospheric Chemistry and Physics 10, 7685-7696 (2010). Koch, D., Menon, S., Del Genio, A. et al. Distinguishing Aerosol Impacts on Climate over the Past Century. Journal of Climate 22, 2659-2677 (2009). Liao, H. and Seinfeld, J. H. Global impacts of gas-phase chemistry-aerosol interactions on direct radiative forcing by anthropogenic aerosols and ozone. Journal of Geophysical Research 110, D18208 (2005). Lohmann, U. and Feichter, J. Impact of sulfate aerosols on albedo and lifetime of clouds: A sensitivity study with the ECHAM4 GCM. Journal of Geophysical Research-Atmospheres 102, 1368513700 (1997). Lohmann, U. and Hoose, C. Sensitivity studies of different aerosol indirect effects in mixed-phase clouds. Atmospheric Chemistry and Physics 9, 8917-8934 (2009). Menon, S., Del Genio, A. D., Koch, D. et al. GCM Simulations of the aerosol indirect effect: Sensitivity to cloud parameterization and aerosol burden. Journal of the Atmospheric Sciences 59, 692713 (2002). Myhre, G. Consistency between satellite-derived and modeled estimates of the direct aerosol effect. Science 325, 187-190 (2009). Myhre, G., Berglen, T. F., Johnsrud, M. et al. Modelled radiative forcing of the direct aerosol effect with multi-observation evaluation. Atmospheric Chemistry and Physics 9, 1365-1392 (2009). Novakov, T., Hegg, D. A. and Hobbs, P. V. Airborne measurements of carbonaceous aerosols on the East Coast of the United States. Journal of Geophysical Research-Atmospheres 102, 3002330030 (1997). Putaud, J. P., Raes, F., Van Dingenen, R. et al. European aerosol phenomenology-2: chemical characteristics of particulate matter at kerbside, urban, rural and background sites in Europe. Atmospheric Environment 38, 2579-2595 (2004). Quinn, P. K. and Bates, T. S. Regional aerosol properties: Comparisons of boundary layer measurements from ACE 1, ACE 2, aerosols99, INDOEX, ACE asia, TARFOX, and NEAQS. Journal of Geophysical Research-Atmospheres 110, D14202 (2005). Ramanathan, V., Crutzen, P. J., Lelieveld, J. et al. Indian Ocean Experiment: An integrated analysis of the climate forcing and effects of the great Indo-Asian haze. Journal of Geophysical ResearchAtmospheres 106, 28371-28398 (2001). Remer, L. A., Kleidman, R. G., Levy, R. C. et al. Global aerosol climatology from the MODIS satellite sensors. Journal of Geophysical Research-Atmospheres 113, D14s07 (2008). Schulz, M., Textor, C., Kinne, S. et al. Radiative forcing by aerosols as derived from the AeroCom present-day and pre-industrial simulations. Atmospheric Chemistry and Physics, 5225-5246 (2006). Stevens, B. and Feingold, G. Untangling aerosol effects on clouds and precipitation in a buffered system. Nature 461, 607-613 (2009). Storelvmo, T., Hoose, C. and Eriksson, P. Global modeling of mixed-phase clouds: The albedo and lifetime effects of aerosols. Journal of Geophysical Research-Atmospheres 116, D05207 (2011). Trenberth, K. E. and Fasullo, J. T. Tracking Earth's Energy. Science 328, 316-317 (2010). Twomey, S. Influence of pollution on shortwave albedo of clouds. Journal of the Atmospheric Sciences 34, 1149-1152 (1977).