Seth Nemesure

Direct shortwave forcing of climate by the anthropogenic sulfate aerosol: Sensitivity to particle size, composition, and relative humidity

Recent estimates of global or hemispheric average forcing of climate by anthropogenic sulfate aerosol caused by scattering of shortwave radiation (“direct” effect) are uncertain by somewhat more than a factor of 2. The principal sources of this uncertainty are atmospheric chemistry properties (yield, residence time), and microphysical properties (scattering efficiency, upscatter fraction, and the dependence of these properties on particle size, composition, and relative humidity, (RH)). This paper examines the sensitivity of forcing to these microphysical properties to identify and improve understanding of the properties required to reduce the uncertainty in the forcing. The relations between aerosol loading and forcing developed here are suitable for comparing modeled and measured aerosol forcing at specific locations and for use in climate models, provided aerosol composition and microphysical properties are known, calculated, or assumed. Results are presented showing the dependence of scattering efficiency, upscatter fraction, and normalized forcing (W m−2/g(SO24−) m−2 or W g(SO24−)−1) on dry particle size (expressed as mole(sulfate) per particle), composition ((NH4)2SO4, NH4HSO4, H2SO4), solar zenith angle, latitude, and season. Forcing is strongly dependent on dry particle size and RH but is relatively insensitive to composition. The normalized forcing can be integrated over a known or assumed size distribution to evaluate the sulfate aerosol forcing. Global and annual average values of the normalized forcing are evaluated as a function of particle size and RH. Depending on values of these variables, normalized forcing may be less than, intermediate to, or greater than the range of previous estimates of sulfate aerosol forcing.

Intercomparison of models representing direct shortwave radiative forcing by sulfate aerosols

The importance of aerosols as agents of climate change has recently been highlighted. However, the magnitude of aerosol forcing by scattering of shortwave radiation (direct forcing) is still very uncertain even for the relatively well characterized sulfate aerosol. A potential source of uncertainty is in the model representation of aerosol optical properties and aerosol influences on radiative transfer in the atmosphere. Although radiative transfer methods and codes have been compared in the past, these comparisons have not focused on aerosol forcing (change in net radiative flux at the top of the atmosphere). Here we report results of a project involving 12 groups using 15 models to examine radiative forcing by sulfate aerosol for a wide range of values of particle radius, aerosol optical depth, surface albedo, and solar zenith angle. Among the models that were employed were high and low spectral resolution models incorporating a variety of radiative transfer approximations as well as a line-by-line model. The normalized forcings (forcing per sulfate column burden) obtained with the several radiative transfer models were examined, and the discrepancies were characterized. All models simulate forcings of comparable amplitude and exhibit a similar dependence on input parameters. As expected for a non-light-absorbing aerosol, forcings were negative (cooling influence) except at high surface albedo combined with small solar zenith angle. The relative standard deviation of the zenith-angle-averaged normalized broadband forcing for 15 models was 8% for particle radius near the maximum in this forcing (∼0.2 μm) and at low surface albedo. Somewhat greater model-to-model discrepancies were exhibited at specific solar zenith angles. Still greater discrepancies were exhibited at small particle radii, and much greater discrepancies were exhibited at high surface albedos, at which the forcing changes sign; in these situations, however, the normalized forcing is quite small. Discrepancies among the models arise from inaccuracies in Mie calculations, differing treatment of the angular scattering phase function, differing wavelength and angular resolution, and differing treatment of multiple scattering. These results imply the need for standardized radiative transfer methods tailored to the direct aerosol forcing problem. However, the relatively small spread in these results suggests that the uncertainty in forcing arising from the treatment of radiative forcing of a well-characterized aerosol at well-specified surface albedo is smaller than some of the other sources of uncertainty in estimates of direct forcing by anthropogenic sulfate aerosols and anthropogenic aerosols generally.

MODELS OVERESTIMATE DIFFUSE CLEAR-SKY SURFACE IRRADIANCE: A CASE FOR EXCESS ATMOSPHERIC ABSORPTION

Radiative transfer models consistently overestimate surface diffuse downward irradiance in cloud-free atmospheres by 9 to 40% at two low altitude sites while correctly calculating direct-normal Solar irradiance. For known systematic and random measurement errors and for realistic aerosol optical properties, the discrepancy can be resolved by a reduction in the vertical aerosol optical thickness (AOT) inferred from sunphotometric measurements by an average 0.02 ± 0.01 for 32 cases examined, together with a compensating increase in a continuum-like atmospheric absorptance over the solar spectrum of ∼5.0% ± 3.0%. This phenomenon is absent at two high altitude sites, where models and measurements agree to within their mutual uncertainties. Examination of apparent AOT at several locations around the globe also indicates presence of such excess atmospheric absorption. The proposed absorption and corresponding reduction in AOT would have important consequences for climate prediction and remote sensing.

Properties and evolution of aerosols with size distributions having identical moments

It has been proposed that the properties and evolution of an aerosol can be represented by lower-order moments of its size distribution without requiring additional knowledge of the distribution itself. However, certain distributions, including the log-normal and modified gamma distributions widely used to represent aerosol size distributions, belong to classes of multiple distributions having identical sets of moments, a situation that brings into question the utility of moment-based representations of aerosol properties and dynamics. We compare aerosol properties and evolution for explicit dissimilar test distributions having identical moments. It is found that despite their dissimilarity (e.g. multimode vs single mode) these distributions exhibit virtually identical physical and optical properties and dynamics. This analysis allays the concern regarding applicability of moment-based representations of aerosol properties that arises out of the existence of sets of distributions exhibiting identical moments.

Aerosol Optical Depth over Oceans: High Space- and Time-Resolution Retrieval and Error Budget from Satellite Radiometry

A method to retrieve aerosol vertical optical depth at 0.64 mm from satellite observations of cloud-free scenes over oceans with high spatial resolution (;18) and instantaneous temporal resolution is described and evaluated. The observed radiance is treated as the linear sum of contributions to path radiance by different scattering processes in the atmosphere‐ocean system. This treatment allows examination of errors in the retrieved vertical aerosol optical depth contributed by each process and approximation. Random error in retrieved aerosol optical depth is typically 0.03. The systematic error due to absolute calibration uncertainty in the measured radiance is 0.01. The largest errors and biases are due to radiative transfer approximations (122%) and assumptions regarding aerosol microphysical and optical properties (220%). The latter errors, which are due to the optical properties (e.g., phase function), vary systematically with latitude and season because of the variation of the mean observing geometry. This method is applied to Advanced Very High Resolution Radiometer global area coverage data, and example maps of aerosol optical depth are presented for specific dates in July and October 1986. The aerosol optical depth derived from the satellite data is suitable for examining large aerosol signatures by instantaneous comparison of the amplitude and location of aerosol plumes with model predictions based on meteorological conditions at and preceding the time of observation.

Impact of clouds on the shortwave radiation budget of the surface-atmosphere system for snow-covered surfaces

Abstract Recent data from the Earth Radiation Budget Experiment (ERBE) have raised the question as to whether or not the addition of clouds to the atmospheric column can decrease the top-of-the-atmosphere (TOA) albedo over bright snow-covered surfaces. To address this issue, ERBE shortwave pixel measurements have been collocated with surface insolation measurements made at two snow-covered locations: the South Pole and Saskatoon, Saskatchewan. Both collocated datasets show a negative correlation (with solar zenith angle variability removed) between TOA albedo and surface insulation. Because increased cloudiness acts to reduce surface insulation, these negative correlations demonstrate that clouds increase the TOA albedo at both snow-covered locations.