[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.

The nucleation of atmospheric vapours is an important source of new aerosol particles that can subsequently grow to form cloud condensation nuclei in the atmosphere. Most field studies of atmospheric aerosols over continents are influenced by atmospheric vapours of anthropogenic origin (for example, ref. 2) and, in consequence, aerosol processes in pristine, terrestrial environments remain poorly understood. The Amazon rainforest is one of the few continental regions where aerosol particles and their precursors can be studied under near-natural conditions, but the origin of small aerosol particles that grow into cloud condensation nuclei in the Amazon boundary layer remains unclear. Here we present aircraft- and ground-based measurements under clean conditions during the wet season in the central Amazon basin. We find that high concentrations of small aerosol particles (with diameters of less than 50 nanometres) in the lower free troposphere are transported from the free troposphere into the boundary layer during precipitation events by strong convective downdrafts and weaker downward motions in the trailing stratiform region. This rapid vertical transport can help to maintain the population of particles in the pristine Amazon boundary layer, and may therefore influence cloud properties and climate under natural conditions.

The Impact of Arctic Aerosols on Clouds During one flight leg over the water on 4 April, large chunks of ice were seen floating in the Arctic Ocean after breaking up from the ice sheet along the coastline near Barrow, Alaska. Photo by Alexei Korolev.

Estimating the aerosol contribution to the global or regional radiative forcing can take advantage of the relationship between the spectral aerosol optical properties and the size and chemical composition of aerosol. Long term global optical measurements from observational networks or satellites can be used in such studies. Using in-situ chemical mixing state measurements can help us to constrain the limitations of such estimates.

In this study, the Absorption Ångström Exponent (AAE) and the Scattering Ångström Exponent (SAE) derived from 10 operational AERONET sites in California are combined for deducing chemical speciation based on wavelength dependence of the optical properties. In addition, in-situ optical properties and single particle chemical composition measured during three aircraft field campaigns in California between 2010 and 2011 are combined in order to validate the methodology used for the estimates of aerosol chemistry using spectral optical properties.

Results from this study indicate a dominance of mixed types in the classification leading to an underestimation of the primary sources, however secondary sources are better classified. The distinction between carbonaceous aerosols from fossil fuel and biomass burning origins is not clear, since their optical properties are similar. On the other hand, knowledge of the aerosol sources in California from chemical studies help to identify other misclassification such as the dust contribution

[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.

The Reno Aerosol Optics Study (RAOS) was designed and conducted to compare the performance of many existing and new instruments for the in situ measurement of aerosol optical properties with a focus on the determination of aerosol light absorption. For this study, simple test aerosols of black and white particles were generated and combined in external mixtures under low relative humidity conditions and delivered to each measurement system. The aerosol mixing and delivery system was constantly monitored using particle counters and nephelometers to ensure that the same aerosol number concentration and amount reached the different instruments. The aerosol light-scattering measurements of four different nephelometers were compared, while the measurements of seven light-absorption instruments (5 filter based, 2 photoacoustic) were evaluated. Four methods for determining the aerosol lightextinction coefficient (3 cavity ring-down instruments and 1 foldedpath optical extinction cell) were also included in the comparisons. An emphasis was placed on determining the representativeness of the filter-based light absorption methods, since these are used Address correspondence to Patrick J. Sheridan, Climate Monitoring and Diagnostics Laboratory, National Oceanic and Atmospheric Administration, 325 Broadway, Boulder, CO 80305, USA. E-mail: patrick.sheridan@noaa.gov widely and because major corrections to the raw attenuation measurements are known to be required. The extinction measurement from the optical extinction cell was compared with the scattering measurement from a high-sensitivity integrating nephelometer on fine, nonabsorbing ammonium sulfate aerosols, and the two were found to agree closely (within 1% for blue and green wavelengths and 2% for red). The wavelength dependence of light absorption for small kerosene and diesel soot particles was found to be very near λ −1 , the theoretical small-particle limit. Larger, irregularly shaped graphite particles showed widely variable wavelength dependencies over several graphite runs. The light-absorption efficiency at a wavelength of 530 nm for pure kerosene soot with a number size distribution peak near 0.3 µm diameter was found to be 7.5 ± 1.2 m 2 g −1 . The two most fundamental independent absorption methods used in this study were photoacoustic absorption and the difference between suspended-state light extinction and scattering, and these showed excellent agreement (typically within a few percent) on mixed black/white aerosols, with the photoacoustic measurement generally slightly lower. Excellent agreement was also observed between some filter-based light-absorption measurements and the RAOS reference absorption method. For atmospherically relevant levels of the aerosol light-absorption coefficient (<25 Mm −1 ), the particle soot absorption photometer (PSAP) absorption measurement at mid-visible wavelengths agreed with the reference absorption measurement to within ∼11% for experiment tests on externally mixed kerosene soot and ammonium sulfate. At higher absorption ...

The new Cloud Physics Lidar (CPL) has been built for use on the NASA ER-2 high altitude aircraft.The purpose of the CPL is to provide multi-wavelength measurements of cirrus, subvisual cirrus, and aerosols with high temporal and spatial resolution. The CPL utilizes state-of-the-art technology with a high repetition rate, low pulse energy laser and photon-counting detection. The first deployment for the CPL was the SAFARI-2000 field campaign during AugustSeptember 2000. We provide here an overview of the instrument and initial data results to illustrate the measurement capability of the CPL.

[1] We present a new approach to retrieve the aerosol properties over land that uses accurate polarization measurements over a broad spectral (410-2250 nm) and angular (±60°from nadir) ranges. The approach uses longer wavelength observations to accurately estimate the surface effects, and it is incorporated into an optimal estimation framework for retrieving the particle number density and a detailed aerosol microphysical model: effective radius, variance, and complex refractive index. A sensitivity analysis shows that the uncertainties in aerosol optical thickness (AOT) increase with AOT while the uncertainties in the microphysical model decrease. The uncertainty in the single scattering albedo (SSA) is notably less than 0.05 by the time the AOT is greater than 0.2. We find that calibration is the major source of uncertainty and that perfect angular and spectral correlation of calibration errors reduces the uncertainties in retrieved quantities. Finally, we observe that shorter wavelength (<500 nm) observations are crucial for determining the aerosols vertical extent and imaginary refractive index from polarization measurements. The retrieval approach is tested under pristine and polluted conditions using observations made by the Research Scanning Polarimeter during the Aerosol Lidar Validation experiment and over California Southern wild fires. In both cases we find that the retrievals are within the combined uncertainties of the retrieval and the Aerosol Robotic Network Cimel products and Total Ozone Mapping Spectrometer Aerosol Index. This demonstrates the unique capability of polarization measurements to accurately retrieve AOTs under pristine conditions and provide estimation of the SSA at higher AOTs.