Bounding Global Aerosol Radiative Forcing of Climate Change.

Aerosols interact with radiation and clouds. Substantial progress made over the past 40 years in observing, understanding, and modeling these processes helped quantify the imbalance in the Earth's radiation budget caused by anthropogenic aerosols, called aerosol radiative forcing, but uncertainties remain large. This review provides a new range of aerosol radiative forcing over the industrial era based on multiple, traceable, and arguable lines of evidence, including modeling approaches, theoretical considerations, and observations. Improved understanding of aerosol absorption and the causes of trends in surface radiative fluxes constrain the forcing from aerosol-radiation interactions. A robust theoretical foundation and convincing evidence constrain the forcing caused by aerosol-driven increases in liquid cloud droplet number concentration. However, the influence of anthropogenic aerosols on cloud liquid water content and cloud fraction is less clear, and the influence on mixed-phase and ice clouds remains poorly constrained. Observed changes in surface temperature and radiative fluxes provide additional constraints. These multiple lines of evidence lead to a 68% confidence interval for the total aerosol effective radiative forcing of -1.6 to -0.6 W m-2, or -2.0 to -0.4 W m-2 with a 90% likelihood. Those intervals are of similar width to the last Intergovernmental Panel on Climate Change assessment but shifted toward more negative values. The uncertainty will narrow in the future by continuing to critically combine multiple lines of evidence, especially those addressing industrial-era changes in aerosol sources and aerosol effects on liquid cloud amount and on ice clouds.

Large contribution of natural aerosols to uncertainty in indirect forcing.

The effect of anthropogenic aerosols on cloud droplet concentrations and radiative properties is the source of one of the largest uncertainties in the radiative forcing of climate over the industrial period. This uncertainty affects our ability to estimate how sensitive the climate is to greenhouse gas emissions. Here we perform a sensitivity analysis on a global model to quantify the uncertainty in cloud radiative forcing over the industrial period caused by uncertainties in aerosol emissions and processes. Our results show that 45 per cent of the variance of aerosol forcing since about 1750 arises from uncertainties in natural emissions of volcanic sulphur dioxide, marine dimethylsulphide, biogenic volatile organic carbon, biomass burning and sea spray. Only 34 per cent of the variance is associated with anthropogenic emissions. The results point to the importance of understanding pristine pre-industrial-like environments, with natural aerosols only, and suggest that improved measurements and evaluation of simulated aerosols in polluted present-day conditions will not necessarily result in commensurate reductions in the uncertainty of forcing estimates.

Impact on short-lived climate forcers (SLCFs) from a realistic land-use change scenario via changes in biogenic emissions.

More than one quarter of natural forests have been cleared by humans to make way for other land-uses, with changes to forest cover projected to continue. The climate impact of land-use change (LUC) is dependent upon the relative strength of several biogeophysical and biogeochemical effects. In addition to affecting the surface albedo and exchanging carbon dioxide (CO2) and moisture with the atmosphere, vegetation emits biogenic volatile organic compounds (BVOCs), altering the formation of short-lived climate forcers (SLCFs) including aerosol, ozone (O3) and methane (CH4). Once emitted, BVOCs are rapidly oxidised by O3, and the hydroxyl (OH) and nitrate (NO3) radicals. These oxidation reactions yield secondary organic products which are implicated in the formation and growth of aerosol particles and are estimated to have a negative radiative effect on the climate (i.e. a cooling). These reactions also deplete OH, increasing the atmospheric lifetime of CH4, and directly affect concentrations of O3; the latter two being greenhouse gases which impose a positive radiative effect (i.e. a warming) on the climate. Our previous work assessing idealised deforestation scenarios found a positive radiative effect due to changes in SLCFs; however, since the radiative effects associated with changes to SLCFs result from a combination of non-linear processes it may not be appropriate to scale radiative effects from complete deforestation scenarios according to the deforestation extent. Here we combine a land-surface model, a chemical transport model, a global aerosol model, and a radiative transfer model to assess the net radiative effect of changes in SLCFs due to historical LUC between the years 1850 and 2000.

Iceland is an episodic source of atmospheric ice-nucleating particles relevant for mixed-phase clouds.

Ice-nucleating particles (INPs) have the potential to remove much of the liquid water in climatically important mid- to high-latitude shallow supercooled clouds, markedly reducing their albedo. The INP sources at these latitudes are very poorly defined, but it is known that there are substantial dust sources across the high latitudes, such as Iceland. Here, we show that Icelandic dust emissions are sporadically an important source of INPs at mid to high latitudes by combining ice-nucleating active site density measurements of aircraft-collected Icelandic dust samples with a global aerosol model. Because Iceland is only one of many high-latitude dust sources, we anticipate that the combined effect of all these sources may strongly contribute to the INP population in the mid- and high-latitude northern hemisphere. This is important because these emissions are directly relevant for the cloud-phase climate feedback and because high-latitude dust emissions are expected to increase in a warmer climate.

The detection of large HNO3-containing particles in the winter Arctic stratosphere.

Large particles containing nitric acid (HNO3) were observed in the 1999/2000 Arctic winter stratosphere. These in situ observations were made over a large altitude range (16 to 21 kilometers) and horizontal extent (1800 kilometers) on several airborne sampling flights during a period of several weeks. With diameters of 10 to 20 micrometers, these sedimenting particles have significant potential to denitrify the lower stratosphere. A microphysical model of nitric acid trihydrate particles is able to simulate the growth and sedimentation of these large sizes in the lower stratosphere, but the nucleation process is not yet known. Accurate modeling of the formation of these large particles is essential for understanding Arctic denitrification and predicting future Arctic ozone abundances.

Reassessment of pre-industrial fire emissions strongly affects anthropogenic aerosol forcing.

Uncertainty in pre-industrial natural aerosol emissions is a major component of the overall uncertainty in the radiative forcing of climate. Improved characterisation of natural emissions and their radiative effects can therefore increase the accuracy of global climate model projections. Here we show that revised assumptions about pre-industrial fire activity result in significantly increased aerosol concentrations in the pre-industrial atmosphere. Revised global model simulations predict a 35% reduction in the calculated global mean cloud albedo forcing over the Industrial Era (1750-2000 CE) compared to estimates using emissions data from the Sixth Coupled Model Intercomparison Project. An estimated upper limit to pre-industrial fire emissions results in a much greater (91%) reduction in forcing. When compared to 26 other uncertain parameters or inputs in our model, pre-industrial fire emissions are by far the single largest source of uncertainty in pre-industrial aerosol concentrations, and hence in our understanding of the magnitude of the historical radiative forcing due to anthropogenic aerosol emissions.

Impact on short-lived climate forcers increases projected warming due to deforestation.

The climate impact of deforestation depends on the relative strength of several biogeochemical and biogeophysical effects. In addition to affecting the exchange of carbon dioxide (CO2) and moisture with the atmosphere and surface albedo, vegetation emits biogenic volatile organic compounds (BVOCs) that alter the formation of short-lived climate forcers (SLCFs), which include aerosol, ozone and methane. Here we show that a scenario of complete global deforestation results in a net positive radiative forcing (RF; 0.12 W m-2) from SLCFs, with the negative RF from decreases in ozone and methane concentrations partially offsetting the positive aerosol RF. Combining RFs due to CO2, surface albedo and SLCFs suggests that global deforestation could cause 0.8 K warming after 100 years, with SLCFs contributing 8% of the effect. However, deforestation as projected by the RCP8.5 scenario leads to zero net RF from SLCF, primarily due to nonlinearities in the aerosol indirect effect.

Cosmic rays, clouds, and climate.

It has been proposed that Earth's climate could be affected by changes in cloudiness caused by variations in the intensity of galactic cosmic rays in the atmosphere. This proposal stems from an observed correlation between cosmic ray intensity and Earth's average cloud cover over the course of one solar cycle. Some scientists question the reliability of the observations, whereas others, who accept them as reliable, suggest that the correlation may be caused by other physical phenomena with decadal periods or by a response to volcanic activity or El Niño. Nevertheless, the observation has raised the intriguing possibility that a cosmic ray-cloud interaction may help explain how a relatively small change in solar output can produce much larger changes in Earth's climate. Physical mechanisms have been proposed to explain how cosmic rays could affect clouds, but they need to be investigated further if the observation is to become more than just another correlation among geophysical variables.