Published by Copernicus Publications on behalf of the European Geosciences Union. 8698 J. Quaas et al.: Aerosol indirect effects -general circulation model intercomparisonbetween τ a and f cld . The short-wave total aerosol radiative forcing as simulated by the GCMs is strongly influenced by the simulated anthropogenic fraction of τ a , and parameterisation assumptions such as a lower bound on N d . Nevertheless, the strengths of the statistical relationships are good predictors for the aerosol forcings in the models. An estimate of the total short-wave aerosol forcing inferred from the combination of these predictors for the modelled forcings with the satellite-derived statistical relationships yields a global annual mean value of −1.5±0.5 Wm −2 . In an alternative approach, the radiative flux perturbation due to anthropogenic aerosols can be broken down into a component over the cloud-free portion of the globe (approximately the aerosol direct effect) and a component over the cloudy portion of the globe (approximately the aerosol indirect effect). An estimate obtained by scaling these simulated clearand cloudy-sky forcings with estimates of anthropogenic τ a and satellite-retrieved N d -τ a regression slopes, respectively, yields a global, annual-mean aerosol direct effect estimate of −0.4±0.2 Wm −2 and a cloudy-sky (aerosol indirect effect) estimate of −0.7±0.5 Wm −2 , with a total estimate of −1.2±0.4 Wm −2 .

We present an overview of the background, scientific goals, and execution of the Aerosol, Radiation, and Cloud Processes affecting Arctic Climate (ARCPAC) project of April 2008. We then summarize airborne measurements, made in the troposphere of the Alaskan Arctic, of aerosol particle size distributions, composition, and optical properties and discuss the sources and transport of the aerosols. The aerosol data were grouped into four categories based on gas-phase composition. First, the background troposphere contained a relatively diffuse, sulfate-rich aerosol extending from the top of the sea-ice inversion layer to 7.4 km altitude. Second, a region of depleted (relative to the background) aerosol was present within the surface inversion layer over sea-ice. Third, layers of dense, organic-rich smoke from open biomass fires in southern Russia and southeastern Siberia were frequently encountered at all altitudes from the top of the inversion layer to 7.1 km. Finally, some aerosol layers were dominated by components originating from fossil fuel combustion. <br></br> Of these four categories measured during ARCPAC, the diffuse background aerosol was most similar to the average springtime aerosol properties observed at a long-term monitoring site at Barrow, Alaska. The biomass burning (BB) and fossil fuel layers were present above the sea-ice inversion layer and did not reach the sea-ice surface during the course of the ARCPAC measurements. The BB aerosol layers were highly scattering and were moderately hygroscopic. On average, the layers produced a noontime net heating of ~0.1 K day^&minus;1 between 3 and 7 km and a slight cooling at the surface. The ratios of particle mass to carbon monoxide (CO) in the BB plumes, which had been transported over distances >5000 km, were comparable to the high end of literature values derived from previous measurements in wildfire smoke. These ratios suggest minimal precipitation scavenging and removal of the BB particles between the time they were emitted and the time they were observed in dense layers above the sea-ice inversion layer

[1] Values for Mie-equivalent aerosol asymmetry parameter (g) were derived using a variety of methods from the large suite of measurements (in situ and remote from surface and aircraft) made in Oklahoma during the 2003 aerosol Intensive Operations Period (IOP). Median values derived for dry asymmetry parameter at 550 nm ranged between 0.55 and 0.63 over all instruments and for all derivation methods, with the exception of one instrument which did not measure over the full size range of optically important aerosol. Median values for the ''wet'' asymmetry parameter (i.e., asymmetry parameter at humidity conditions closer to ambient) were between 0.59 and 0.72. Values for g derived for surface and airborne in situ measurements were highly correlated, but in situ and remote sensing measurements both at the surface and aloft did not agree as well because of vertical inhomogeneity of the aerosol. Radiative forcing calculations suggest that a 10% decrease in g would result in a 19% reduction in top of atmosphere radiative forcing for the conditions observed during the IOP. Comparison of the different methods for deriving g suggests that in computing the asymmetry parameter, aerosol size is the most important parameter to measure; composition is less important except for how it influences the hygroscopic growth (i.e., size) of particles.

[1] An assessment of aerosol-cloud interactions (ACI) from ground-based remote sensing under coastal stratiform clouds is presented. The assessment utilizes a long-term, high temporal resolution data set from the Atmospheric Radiation Measurement (ARM) Program deployment at Pt. Reyes, California, United States, in 2005 to provide statistically robust measures of ACI and to characterize the variability of the measures based on variability in environmental conditions and observational approaches. The average ACI N (= dlnN d /dlna, the change in cloud drop number concentration with aerosol concentration) is 0.48, within a physically plausible range of 0-1.0. Values vary between 0.18 and 0.69 with dependence on (1) the assumption of constant cloud liquid water path (LWP), (2) the relative value of cloud LWP, (3) methods for retrieving N d , (4) aerosol size distribution, (5) updraft velocity, and (6) the scale and resolution of observations. The sensitivity of the local, diurnally averaged radiative forcing to this variability in ACI N values, assuming an aerosol perturbation of 500 cm À3 relative to a background concentration of 100 cm À3 , ranges between À4 and À9 W m À2 . Further characterization of ACI and its variability is required to reduce uncertainties in global radiative forcing estimates.

[1] Understanding sources of uncertainty in aerosol direct radiative forcing (DRF), the difference in a given radiative flux component with and without aerosol, is essential to quantifying changes in Earth's radiation budget. We examine the uncertainty in DRF owing to measurement uncertainty in the quantities on which it depends: aerosol optical depth, single scattering albedo, asymmetry parameter, solar geometry, and surface albedo. Direct radiative forcing at the top of the atmosphere and at the surface is calculated at three locations representing distinct aerosol types and radiative environments. Sensitivities, the changes in DRF in response to unit changes in individual aerosol or surface properties, are also calculated for these conditions. The uncertainty in DRF associated with a given property is computed as the product of the sensitivity and typical measurement uncertainty in the respective property. Sensitivity and uncertainty values permit estimation of total uncertainty in calculated DRF and identification of properties that most limit accuracy in estimating forcing. Absolute total uncertainties in modeled local diurnally averaged forcing range from 0.2 to 3.1 W m À2 for the ranges of properties examined here. Relative total uncertainties range from $20 to 80% with larger values at higher latitudes, where fluxes are low. The largest contributor to total uncertainty in DRF is single scattering albedo; however, decreasing measurement uncertainties for any property would increase accuracy in DRF. Comparison of two radiative transfer models suggests the contribution of modeling error is small compared to the total uncertainty although comparable to uncertainty arising from some individual properties.

Abstract.A wide range of estimates exists for the radiative forcing of the aerosol effect on cloud albedo. We argue that a component of this uncertainty derives from the use of a wide range of observational scales and platforms. Aerosol influences cloud properties at the microphysical scale, or the "process scale", but observations are most often made of bulk properties over a wide range of resolutions, or "analysis scales". We show that differences between process and analysis scales incur biases in quantification of the albedo effect through the impact that data aggregation and computational approach have on statistical properties of the aerosol or cloud variable, and their covariance. Measures made within this range of scales are erroneously treated as equivalent, leading to a large uncertainty in associated radiative forcing estimates. Issues associated with the coarsening of observational resolution particular to quantifying the albedo effect are discussed. Specifically, the omission of the constraint on cloud liquid water path and the separation in space of cloud and aerosol properties from passive, space-based remote sensors dampen the measured strength of the albedo effect. We argue that, because of this lack of constraints, many of these values are in fact more representative of the full range of aerosol-cloud interactions and their associated feedbacks. Based on our understanding of these biases we propose a new observationally-based and process-model-constrained, method for estimating aerosol-cloud interactions that can be used for radiative forcing estimates as well as a better characterization of the uncertainties associated with those estimates.

[1] Surface, airborne, and satellite measurements over the eastern Pacific Ocean off the coast of California during the period between 2005 and 2007 are used to explore the relationship between ocean chlorophyll a, aerosol, and marine clouds. Periods of enhanced chlorophyll a and wind speed are coincident with increases in particulate diethylamine and methanesulfonate concentrations. The measurements indicate that amines are a source of secondary organic aerosol in the marine atmosphere. Subsaturated aerosol hygroscopic growth measurements indicate that the organic component during periods of high chlorophyll a and wind speed exhibit considerable water uptake ability. Increased average cloud condensation nucleus (CCN) activity during periods of increased chlorophyll a levels likely results from both size distribution and aerosol composition changes. The available data over the period of measurements indicate that the cloud microphysical response, as represented by either cloud droplet number concentration or cloud droplet effective radius, is likely influenced by a combination of atmospheric dynamics and aerosol perturbations during periods of high chlorophyll a concentrations.Citation: Sorooshian, A., et al. (2009), On the link between ocean biota emissions, aerosol, and maritime clouds: Airborne, ground, and satellite measurements off the coast of California, Global Biogeochem. Cycles, 23, GB4007,

Emissions of SO 2 in the United States have declined since the early 1990s, resulting in a decrease in aerosol sulfate mass in the Southeastern U.S. of À4.5(±0.9)% yr À1 between 1992 and 2013. Organic aerosol mass, the other major aerosol component in the Southeastern U.S., has decreased more slowly despite concurrent emission reductions in anthropogenic precursors. Summertime measurements in rural Alabama quantify the change in aerosol light extinction as a function of aerosol composition and relative humidity. Application of this relationship to composition data from 2001 to 2013 shows that a À1.1(±0.7)% yr À1 decrease in extinction can be attributed to decreasing aerosol water mass caused by the change in aerosol sulfate/organic ratio. Calculated reductions in extinction agree with regional trends in ground-based and satellite-derived aerosol optical depth. The diurnally averaged summertime surface radiative effect has changed by 8.0 W m À2 , with 19% attributed to the decrease in aerosol water.