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David J. Delene and John A. Ogren

Abstract

Aerosol optical properties measured over several years at surface monitoring stations located at Bondville, Illinois (BND); Lamont, Oklahoma (SGP); Sable Island, Nova Scotia (WSA); and Barrow, Alaska (BRW), have been analyzed to determine the importance of the variability in aerosol optical properties to direct aerosol radiative forcing calculations. The amount of aerosol present is of primary importance and the aerosol optical properties are of secondary importance to direct aerosol radiative forcing calculations. The mean aerosol light absorption coefficient (σ ap) is 10 times larger and the mean aerosol scattering coefficient (σ sp) is 5 times larger at the anthropogenically influenced site at BND than at BRW. The aerosol optical properties of single scattering albedo (ω o) and hemispheric backscatter fraction (b) have variability of approximately ± 3% and ± 8%, respectively, in mean values among the four stations. To assess the importance of the variability in ω o and b on top of the atmosphere aerosol radiative forcing calculations, the aerosol radiative forcing efficiency (ΔF/δ) is calculated. The ΔF/δ is defined as the aerosol forcing (ΔF) per unit optical depth (δ) and does not depend explicitly on the amount of aerosol present. Based on measurements at four North American stations, radiative transfer calculations that assume fixed aerosol properties can have errors of 1%–6% in the annual average forcing at the top of the atmosphere due to variations in average single scattering albedo and backscatter fraction among the sites studied. The errors increase when shorter-term variations in aerosol properties are considered; for monthly and hourly timescales, errors are expected to be greater than 8% and 15%, respectively, approximately one-third of the time. Systematic relationships exist between various aerosol optical properties [σ ap, ω o, b, ΔF/δ, and Ångström exponent (å)] and the amount of aerosol present (measured by σ sp) that are qualitatively similar but quantitatively different among the four stations. These types of systematic relationships and the regional and temporal variations in aerosol optical properties should be considered when using “climatological” averages.

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K. B. Noone, K. J. Noone, J. Heintzenberg, J. Ström, and J. A. Ogren

Abstract

This study presents a new technique for making in situ measurements of cirrus cloud microphysical properties. Sampling of cirrus clouds was performed using a counterflow virtual impactor (CVI). The CVI was used to sample cloud elements larger than 4 µm in aerodynamic diameter. In conjunction with a Lyman-α hygrometer, this gave a direct measurement of the condensed water content. Sampling the cloud elements with the CVI also allowed the authors to examine the size distribution of the residual particles produced by evaporation of the cloud elements. This study discusses and evaluates the CVI technique for use in sampling cirrus clouds, especially for sampling small cloud elements. Measurements of condensed water content and cloud-element (crystal and droplet) concentrations for cirrus uncinus, floccus, and cirrostratus clouds made using the CVI during the International Cirrus Experiment experiment are presented. Examples of size distributions of the residual aerosol particles from cirrus cloud elements are also presented.

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Stephen E. Schwartz, Robert J. Charlson, Ralph A. Kahn, John A. Ogren, and Henning Rodhe
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Stephen E. Schwartz, Robert J. Charlson, Ralph A. Kahn, John A. Ogren, and Henning Rodhe

Abstract

The observed increase in global mean surface temperature (GMST) over the industrial era is less than 40% of that expected from observed increases in long-lived greenhouse gases together with the best-estimate equilibrium climate sensitivity given by the 2007 Assessment Report of the Intergovernmental Panel on Climate Change (IPCC). Possible reasons for this warming discrepancy are systematically examined here. The warming discrepancy is found to be due mainly to some combination of two factors: the IPCC best estimate of climate sensitivity being too high and/or the greenhouse gas forcing being partially offset by forcing by increased concentrations of atmospheric aerosols; the increase in global heat content due to thermal disequilibrium accounts for less than 25% of the discrepancy, and cooling by natural temperature variation can account for only about 15%. Current uncertainty in climate sensitivity is shown to preclude determining the amount of future fossil fuel CO2 emissions that would be compatible with any chosen maximum allowable increase in GMST; even the sign of such allowable future emissions is unconstrained. Resolving this situation, by empirical determination of the earth’s climate sensitivity from the historical record over the industrial period or through use of climate models whose accuracy is evaluated by their performance over this period, is shown to require substantial reduction in the uncertainty of aerosol forcing over this period.

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Theodore L. Anderson, Robert J. Charlson, David M. Winker, John A. Ogren, and Kim Holmén

Abstract

Tropospheric aerosols are calculated to cause global-scale changes in the earth's heat balance, but these forcings are space/time integrals over highly variable quantities. Accurate quantification of these forcings will require an unprecedented synergy among satellite, airborne, and surface-based observations, as well as models. This study considers one aspect of achieving this synergy—the need to treat aerosol variability in a consistent and realistic way. This need creates a requirement to rationalize the differences in spatiotemporal resolution and coverage among the various observational and modeling approaches. It is shown, based on aerosol optical data from diverse regions, that mesoscale variability (specifically, for horizontal scales of 40–400 km and temporal scales of 2–48 h) is a common and perhaps universal feature of lower-tropospheric aerosol light extinction. Such variation is below the traditional synoptic or “airmass” scale (where the aerosol is often assumed to be essentially homogeneous except for plumes from point sources) and below the scales that are readily resolved by chemical transport models. The present study focuses on documenting this variability. Possible physical causes and practical implications for coordinated observational strategies are also discussed.

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John H. Seinfeld, Ralph A. Kahn, Theodore L. Anderson, Robert J. Charlson, Roger Davies, David J. Diner, John A. Ogren, Stephen E. Schwartz, and Bruce A. Wielicki

Aerosols are involved in a complex set of processes that operate across many spatial and temporal scales. Understanding these processes, and ensuring their accurate representation in models of transport, radiation transfer, and climate, requires knowledge of aerosol physical, chemical, and optical properties and the distributions of these properties in space and time. To derive aerosol climate forcing, aerosol optical and microphysical properties and their spatial and temporal distributions, and aerosol interactions with clouds, need to be understood. Such data are also required in conjunction with size-resolved chemical composition in order to evaluate chemical transport models and to distinguish natural and anthropogenic forcing. Other basic parameters needed for modeling the radiative influences of aerosols are surface reflectivity and three-dimensional cloud fields. This large suite of parameters mandates an integrated observing and modeling system of commensurate scope. The Progressive Aerosol Retrieval and Assimilation Global Observing Network (PARAGON) concept, designed to meet this requirement, is motivated by the need to understand climate system sensitivity to changes in atmospheric constituents, to reduce climate model uncertainties, and to analyze diverse collections of data pertaining to aerosols. This paper highlights several challenges resulting from the complexity of the problem. Approaches for dealing with them are offered in the set of companion papers.

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T.L. Anderson, D.S. Covert, S.F. Marshall, M.L. Laucks, R.J. Charlson, A.P. Waggoner, J.A. Ogren, R. Caldow, R.L. Holm, F.R. Quant, G.J. Sem, A. Wiedensohler, N.A. Ahlquist, and T.S. Bates

Abstract

As designed in the 1940s by Beuttell and Brewer, the integrating nephelometer offers a direct method of measuring light scattering by airborne particles without assumptions about particle composition, shape, or physical state. A large number of such instruments have been deployed; however, only a limited number of validation experiments have been attempted. This paper reports a set of closure experiments in which a gas-calibrated nephelometer is used to measure the scattering coefficient of laboratory-generated particles of known size and refractive index.

Specifically, it evaluates the performance of a high-sensitivity, three-wavelength, total scatter/backscatter integrating nephelometer (TSI, Inc., model 3563). Sources of uncertainty associated with the gas-calibration procedure, with photon-counting statistics, and with nonidealities in wavelength and angular sensitivity are investigated. Tests with particle-free gases indicate that noise levels are well predicted by photon-counting statistics and that the nephelometer response is linear over a wide range of scattering coefficients. Tests with particles show average discrepancies between measured and predicted scattering of 4%–7%. Error analysis indicates that these discrepancies are within experimental uncertainty, which was dominated by particle generation uncertainty. The simulation of nephelometer response, which is validated by these tests, is used to show that errors arising from nephelometer nonidealities are less than 10% for accumulation-mode or smaller particles (i.e., size distributions for which the volume mean diameter is 0.4µm or less) and that significant differences exist between the total scatter and backscatter uncertainties. Based on these findings, appropriate applications of the model 3563 nephelometer am discussed.

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Ralph A. Kahn, John A. Ogren, Thomas P. Ackerman, Jens Bösenberg, Robert J. Charlson, David J. Diner, Brent N. Holben, Robert T. Menzies, Mark A. Miller, and John H. Seinfeld

We briefly but systematically review major sources of aerosol data, emphasizing suites of measurements that seem most likely to contribute to assessments of global aerosol climate forcing. The strengths and limitations of existing satellite, surface, and aircraft remote sensing systems are described, along with those of direct sampling networks and ship-based stations. It is evident that an enormous number of aerosol-related observations have been made, on a wide range of spatial and temporal sampling scales, and that many of the key gaps in this collection of data could be filled by technologies that either exist or are expected to be available in the near future. Emphasis must be given to combining remote sensing and in situ active and passive observations and integrating them with aerosol chemical transport models, in order to create a more complete environmental picture, having sufficient detail to address current climate forcing questions. The Progressive Aerosol Retrieval and Assimilation Global Observing Network (PARAGON) initiative would provide an organizational framework to meet this goal.

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J. Heintzenberg, A. Wiedensohler, T. M. Tuch, D. S. Covert, P. Sheridan, J. A. Ogren, J. Gras, R. Nessler, C. Kleefeld, N. Kalivitis, V. Aaltonen, R-T. Wilhelm, and M. Havlicek

Abstract

This study determined measured and Mie-calculated angular signal truncations for total and backscatter TSI, Inc., nephelometers, as a function of wavelength and for particles of known size and composition. Except for the total scattering channels, similar agreements as in a previous study of measured and calculated truncations were derived for submicrometer test aerosols. For the first time, instrument responses were also determined for supermicrometer test aerosols up to 1.9 μm in geometric mean diameter. These supermicrometer data confirm the theoretical predictions of strong angular truncations of the total scatter signals in integrating nephelometers due to the limited range of measured forward scattering angles. Truncations up to 60% were determined for the largest measured particles. Rough empirical truncation corrections have been derived from the calibration data for Radiance Research and Ecotech nephelometers for which no detailed response characteristics exist. Intercomparisons of the nephelometers measuring urban atmospheric aerosols yield average deviations of the slope from a 1:1 relation with a TSI reference nephelometer of less than 7%. Average intercepts range between +0.53 and −0.19 Mm−1. For the Radiance Research and Ecotech nephelometers ambient regressions of the Radiance Research and Ecotech instruments with the TSI nephelometer show larger negative intercepts, which are attributed to their less well characterized optics.

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