Abstract

The uncertainties of integral aerosol properties calculated using aerosol size distributions retrieved from multiwavelength observations of aerosol optical depth have been determined for a variety of typical atmospheric aerosol size distributions and refractive indices. The results suggest that more information about the aerosol composition, as well as more information about the sizes that are less efficient, in the optical sense, is needed to improve the shape of the retrieved size distributions. All the calculations in this paper assume spherical homogeneous particles. The sensitivity results refer to these conditions. The moments of the retrieved size distributions are systematically underestimated and errors can be as large as −82%, −30%, and −35% for the total number of particles, the total surface, and the total volume, respectively. The errors in the mass scattering efficiency, the effective radius, and the total volume depend very much on whether the actual volume size distribution is monomodal or bimodal. For a known refractive index, the total scattering coefficient, the hemispherical backscattering coefficient, and the extinction coefficient, as well as the hemispheric backscattering to total scattering ratio and the asymmetry factor, are obtained with absolute values for the average errors less than 4%. Similar behavior was expected for cases with uncertainty in the refractive index, especially for parameters defined by the ratio of two integral properties. However, it turns out that the hemispheric backscattering coefficient and the hemispheric backscattering to total scattering ratio were poorly retrieved, reaching errors of 29% in several cases, while the asymmetry factor was very well recovered with absolute values of the average errors always under 7%. When the wavelength dependence of the refractive index is included, the retrieved size distribution is very unrealistic, with average errors in the hemispheric backscattering coefficients and the hemispheric backscattering to total scattering ratio around 30% at some wavelengths. However, even in this case the errors in the retrieved asymmetry factor stay under 8%. Thus, for spherical and homogeneous particles, the spectral optical depth data can be used to determine the asymmetry factor with little sensitivity to the assumptions in the calculations. Furthermore, the retrieved size distribution can be used as an intermediate step to extrapolate one set of optical properties from another set of optical properties.

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.

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.

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.

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.

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.

The primary goal of the Cumulus Humilis Aerosol Processing Study (CHAPS) was to characterize and contrast freshly emitted aerosols below, within, and above fields of cumuli, and to study changes to the cloud microphysical structure within these same cloud fields in the vicinity of Oklahoma City during June 2007. CHAPS is one of few studies that have had an aerosol mass spectrometer (AMS) sampling downstream of a counterflow virtual impactor (CVI) inlet on an aircraft, allowing the examination of the chemical composition of activated aerosols within the cumuli. The results from CHAPS provide insights into changes in the aerosol chemical and optical properties as aerosols move through shallow cumuli downwind of a moderately sized city. Three instrument platforms were employed during CHAPS, including the U.S. Department of Energy Gulfstream-1 aircraft, which was equipped for in situ sampling of aerosol optical and chemical properties; the NASA Langley King Air B200, which carried the downward-looking NASA Langley High Spectral Resolution Lidar (HSRL) to measure profiles of aerosol backscatter, extinction, and depolarization between the King Air and the surface; and a surface site equipped for continuous in situ measurements of aerosol optical properties, profiles of aerosol backscatter, and meteorological conditions, including total sky cover and thermodynamic profiles of the atmosphere. In spite of record precipitation over central Oklahoma, a total of 8 research flights were made by the G-l and 18 by the B200, including special satellite verification flights timed to coincide with NASA satellite A-Train overpasses.

Abstract

A modest operational program of systematic aircraft measurements can resolve key satellite aerosol data record limitations. Satellite observations provide frequent global aerosol amount maps but offer only loose aerosol property constraints needed for climate and air quality applications. We define and illustrate the feasibility of flying an aircraft payload to measure key aerosol optical, microphysical, and chemical properties in situ. The flight program could characterize major aerosol airmass types statistically, at a level of detail unobtainable from space. It would 1) enhance satellite aerosol retrieval products with better climatology assumptions and 2) improve translation between satellite-retrieved optical properties and species-specific aerosol mass and size simulated in climate models to assess aerosol forcing, its anthropogenic components, and other environmental impacts. As such, Systematic Aircraft Measurements to Characterize Aerosol Air Masses (SAM-CAAM) could add value to data records representing several decades of aerosol observations from space; improve aerosol constraints on climate modeling; help interrelate remote sensing, in situ, and modeling aerosol-type definitions; and contribute to future satellite aerosol missions. Fifteen required variables are identified and four payload options of increasing ambition are defined to constrain these quantities. “Option C” could meet all the SAM-CAAM objectives with about 20 instruments, most of which have flown before, but never routinely several times per week, and never as a group. Aircraft integration and approaches to data handling, payload support, and logistical considerations for a long-term, operational mission are discussed. SAM-CAAM is feasible because, for most aerosol sources and specified seasons, particle properties tend to be repeatable, even if aerosol loading varies.

A comprehensive and cohesive aerosol measurement record with consistent, well-understood uncertainties is a prerequisite to understanding aerosol impacts on long-term climate and environmental variability. Objectives to attaining such an understanding include improving upon the current state-of-the-art sensor calibration and developing systematic validation methods for remotely sensed microphysical properties. While advances in active and passive remote sensors will lead to needed improvements in retrieval accuracies and capabilities, ongoing validation is essential so that the changing sensor characteristics do not mask atmospheric trends. Surface-based radiometer, chemical, and lidar networks have critical roles within an integrated observing system, yet they currently undersample key geographic regions, have limitations in certain measurement capabilities, and lack stable funding. In situ aircraft observations of size-resolved aerosol chemical composition are necessary to provide important linkages between active and passive remote sensing. A planned, systematic approach toward a global aerosol observing network, involving multiple sponsoring agencies and surface-based, suborbital, and spaceborne sensors, is required to prioritize trade-offs regarding capabilities and costs. This strategy is a key ingredient of the Progressive Aerosol Retrieval and Assimilation Global Observing Network (PARAGON) framework. A set of recommendations is presented.

This document outlines a practical strategy for achieving an observationally based quantification of direct climate forcing by anthropogenic aerosols. The strategy involves a four-step program for shifting the current assumption-laden estimates to an increasingly empirical basis using satellite observations coordinated with suborbital remote and in situ measurements and with chemical transport models. Conceptually, the problem is framed as a need for complete global mapping of four parameters: clear-sky aerosol optical depth f _f, radiative efficiency per unit optical depth δ, fine-mode fraction of optical depth f _f, and the anthropogenic fraction of the fine mode f _af . The first three parameters can be retrieved from satellites, but correlative, suborbital measurements are required for quantifying the aerosol properties that control E, for validating the retrieval of f _f, and for partitioning fine-mode δ between natural and anthropogenic components. The satellite focus is on the “A-Train,” a constellation of six spacecraft that will fly in formation from about 2005 to 2008. Key satellite instruments for this report are the Moderate Resolution Imaging Spectroradiometer (MODIS) and Clouds and the Earth's Radiant Energy System (CERES) radiometers on Aqua, the Ozone Monitoring Instrument (OMI) radiometer on Aura, the Polarization and Directionality of Earth's Reflectances (POLDER) polarimeter on the Polarization and Anistropy of Reflectances for Atmospheric Sciences Coupled with Observations from a Lidar (PARASOL), and the Cloud and Aerosol Lider with Orthogonal Polarization (CALIOP) lidar on the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO). This strategy is offered as an initial framework—subject to improvement over time—for scientists around the world to participate in the A-Train opportunity. It is a specific implementation of the Progressive Aerosol Retrieval and Assimilation Global Observing Network (PARAGON) program, presented earlier in this journal, which identified the integration of diverse data as the central challenge to progress in quantifying global-scale aerosol effects. By designing a strategy around this need for integration, we develop recommendations for both satellite data interpretation and correlative suborbital activities that represent, in many respects, departures from current practice.