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Clouds and Aerosols in the Climate System

Remote sensing of cloud and aerosol properties from space is reviewed for present and planned international satellite sensors. Techniques that are being used to enhance our ability to characterize the global distribution of cloud and aerosol properties include well-calibrated multispectral radiometers that rely on visible, near-infrared, and thermal infrared channels, sometimes including polarization as well. The availability of thermal channels to aid in cloud screening for aerosol properties is an important additional piece of information that has not always been incorporated into sensor designs. In this paper, we describe the radiative properties of clouds as currently determined from satellites (cloud fraction, optical thickness, cloud top pressure, and cloud effective radius), and highlight the global and regional cloud microphysical properties currently available for assessing climate variability and forcing. In addition, we will frustrate the radiative and microphysical properties of aerosol particles that are currently available from space-based observations, as well as enhancements to aerosol remote sensing over bright-reflecting surfaces that is anticipated in the next couple of years. Finally, we will describe the aerosol optical and radiative properties available from the globally distributed AERONET network of ground-based sun-sky radiometers.

King, Michael D.↗

Comparison of predicted and observed solar radiation in an urban area

Measurements of the downward solar radiant flux in the St. Louis area are compared with predictions from an approximate solution to the radiative transfer equation. The atmospheric aerosols were assumed to have a power size distribution and the refractive indices suggested by Fischer (1973) for an urban area. On a relatively clean day, the predictions compared well with observations. On a hazy day, the comparison was poor with the a priori choice of aerosol properties. The particles on the hazy day apparently had more submicron particles than those found in the assumed size distribution, and the particles were considerably less absorbing than those observed by Fischer. These changes could represent the effects of relative humidity and different air mass characteristics.

Bergstrom, R. W.↗

The Cabauw Intercomparison Campaign for Nitrogen Dioxide Measuring Instruments (CINDI): Design, Execution, and Early Results

From June to July 2009 more than thirty different in-situ and remote sensing instruments from all over the world participated in the Cabauw Intercomparison campaign for Nitrogen Dioxide measuring Instruments (CINDI). The campaign took place at KNMI's Cabauw Experimental Site for Atmospheric Research (CESAR) in the Netherlands. Its main objectives were to determine the accuracy of state-ofthe- art ground-based measurement techniques for the detection of atmospheric nitrogen dioxide (both in-situ and remote sensing), and to investigate their usability in satellite data validation. The expected outcomes are recommendations regarding the operation and calibration of such instruments, retrieval settings, and observation strategies for the use in ground-based networks for air quality monitoring and satellite data validation. Twenty-four optical spectrometers participated in the campaign, of which twenty-one had the capability to scan different elevation angles consecutively, the so-called Multi-axis DOAS systems, thereby collecting vertical profile information, in particular for nitrogen dioxide and aerosol. Various in-situ samplers and lidar instruments simultaneously characterized the variability of atmospheric trace gases and the physical properties of aerosol particles. A large data set of continuous measurements of these atmospheric constituents has been collected under various meteorological conditions and air pollution levels. Together with the permanent measurement capability at the CESAR site characterizing the meteorological state of the atmosphere, the CINDI campaign provided a comprehensive observational data set of atmospheric constituents in a highly polluted region of the world during summertime. First detailed comparisons performed with the CINDI data show that slant column measurements of NO2, O4 and HCHO with MAX-DOAS agree within 5 to 15%, vertical profiles of NO2 derived from several independent instruments agree within 25% of one another, and MAX-DOAS aerosol optical thickness agrees within 20-30% with AERONET data. For the in-situ NO2 instrument using a molybdenum converter, a bias was found as large as 5 ppbv during day time, when compared to the other in-situ instruments using photolytic converters.

Atmospheric composition↗

Radiative Importance of Aerosol-Cloud Interaction

Aerosol particles are input into the troposphere by biomass burning, among other sources. These aerosol palls cover large expanses of the earth's surface. Aerosols may directly scatter solar radiation back to space, thus increasing the earth's albedo and act to cool the earth's surface and atmosphere. Aerosols also contribute to the earth's energy balance indirectly. Hygroscopic aerosol act as cloud condensation nuclei (CCN) and thus affects cloud properties. In 1977, Twomey theorized that additional available CCN would create smaller but more numerous cloud droplets in a cloud with a given amount of liquid water. This in turn would increase the cloud albedo which would scatter additional radiation back to space and create a similar cooling pattern as the direct aerosol effect. Estimates of the magnitude of the aerosol indirect effect on a global scale range from 0.0 to -4.8 W/sq m. Thus the indirect effect can be of comparable magnitude and opposite in sign to the estimates of global greenhouse gas forcing Aerosol-cloud interaction is not a one-way process. Just as aerosols have an influence on clouds through the cloud microphysics, clouds have an influence on aerosols. Cloud droplets are solutions of liquid water and CCN, now dissolved. When the cloud droplet evaporates it leaves behind an aerosol particle. This new particle does not have to have the same properties as the original CCN. In fact, studies show that aerosol particles that result from cloud processing are larger in size than the original CCN. Optical properties of aerosol particles are dependent on the size of the particles. Larger particles have a smaller backscattering fraction, and thus less incoming solar radiation will be backscattered to space if the aerosol particles are larger. Therefore, we see that aerosols and clouds modify each other to influence the radiative balance of the earth. Understanding and quantifying the spatial and seasonal patterns of the aerosol indirect forcing may have even greater consequences. Presently we know that through the use of fossil fuel and land-use changes we have increased the concentration of greenhouse gases in the atmosphere. In parallel, we have seen a modest increase of global temperature in the last century. These two observations have been linked as cause and effect by climate models, but this connection is still experimentally not verified. The spatial and seasonal distribution of aerosol forcing is different from that of greenhouse gases, thus generating a different spatial fingerprint of climate change. This fingerprint was suggested as a method to identify the response of the climate system to anthropogenic forcing of greenhouse gases and aerosol. The aerosol fingerprint may be the only way to firmly establish the presence (or absence) of human impact on climate. Aerosol-cloud interaction through the indirect effect will be an important component of establishing this fingerprint.

Tsay, Si-Chee↗

Global CALIPSO Observations of Aerosol Changes Near Clouds

Several recent studies have found that clouds are surrounded by a transition zone of rapidly changing aerosol optical properties and particle size. Characterizing this transition zone is important for better understanding aerosol-cloud interactions and aerosol radiative effects, and also for improving satellite retrievals of aerosol properties. This letter presents a statistical analysis of a monthlong global data set of Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) lidar observations over oceans. The results show that the transition zone is ubiquitous over all oceans and extends up to 15 km away from clouds. They also show that near-cloud enhancements in backscatter and particle size are strongest at low altitudes, slightly below the top of the nearest clouds. Also, the enhancements are similar near illuminated and shadowy cloud sides, which confirms that the asymmetry of Moderate Resolution Imaging Spectroradiometer reflectances found in an earlier study comes from 3-D radiative processes and not from differences in aerosol properties. Finally, the effects of CALIPSO aerosol detection and cloud identification uncertainties are discussed. The findings underline the importance of accounting for the transition zone to avoid potential biases in studies of satellite aerosol products, aerosol-cloud interactions, and aerosol direct radiative effects.

Varnai, Tamas↗

Systematic Relationships Between Lidar Observables and Sizes And Mineral Composition Of Dust Aerosols

The physical and chemical properties of soil dust aerosol particles fundamentally affect their interaction with climate, including shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, heterogeneous formation of sulfates and nitrates on the surface of dust particles, and atmospheric processing of iron into bioavailable forms that increase the productivity of marine phytoplankton. Lidar measurements, such as extinction-to-backscatter, color and depolarization ratios, are frequently used to distinguish between aerosol types with different physical and chemical properties. The chemical composition of aerosol particles determines their complex refractive index, hence affecting their backscattering properties. Here we present a study on how dust aerosol backscattering and depolarization properties at wavelengths of 355, 532 and 1064 nm are related to size and complex refractive index, which varies with the mineral composition of the dust. Dust aerosols are represented by collections of spheroids with a range of prolate and oblate aspect ratios and their optical properties are obtained using T-matrix calculations. We find simple, systematic relationships between lidar observables and the dust size and complex refractive index that may aid the use of space-based or airborne lidars for direct retrieval of dust properties or for the evaluation of chemical transport models using forward simulated lidar variables. In addition, we present first results on the spatial variation of forward-simulated lidar variables based on a dust model that accounts for the atmospheric cycle of eight different mineral types plus internal mixtures of seven mineral types with iron oxides, which was recently implemented in the NASA GISS Earth System ModelE2.

Dust↗

Multi-Angle Imager for Aerosols (MAIA) spectral and radiometric calibration

The Multi-angle Imaging SpectroRadiometer (MISR) was launched as part of NASA’s Terra satellite suite of instruments. Still operational, it makes use of observations from multiple view angles to retrieve aerosol abundance and particle properties. The Multi-Angle Imager for Aerosols (MAIA) instrument improves on this heritage by incorporating polarimetry and an expanded spectral range. Combining these data with surface measurements, the relationship between pollution and human health will be explored. MAIA has just completed camera testing, building on the experience from MISR. Spectral calibration now makes use of a double subtractive monochromator, built with the intent to allow the exit slit output to be uniform in spectral content. For radiometric testing, hardware upgrades have included adding UV lamps to the 1.65 cm (65") integrating sphere, use of a NIST-traceable sphere to establish absolute radiances, and the addition of a UV transfer spectrometer to support characterization of the sphere output from 300 to 2500 nm. During camera build, Newton’s rings were observed in the detector Quantum Efficiency (QE) measurements. This is due to etaloning within the detector itself. Etaloning was also evident in the spectral and radiometric characterizations performed on the completed camera. Spectral metrics, including center wavelength and width, are presented here using a moment’s analysis. This better represents the band properties, particularly in bands where fringing is observed, as compared to a full-width at half-maximum determination. It is believed that the MAIA camera has been carefully characterized, and meet its spectral and radiometric requirements.

Harten, Gerard Van↗

Characterization of Individual Aerosol Particles Associated with Clouds (CRYSTAL-FACE)

The aim of our research was to obtain data on the chemical and physical properties of individual aerosol particles from near the bottoms and tops of the deep convective systems that lead to the generation of tropical cirrus clouds and to provide insights into the particles that serve as CCN or IN. We used analytical transmission electron microscopy (ATEM), including energy-dispersive X-ray spectrometry (EDS) and electron energy-loss spectroscopy (EELS), and field-emission electron microscopy (FESEM) to compare the compositions, concentrations, size distributions, shapes, surface coatings, and degrees of aggregation of individual particles from cloud bases and the anvils near the tropopause. Aggregates of sea salt and mineral dust, ammonium sulfate, and soot particles are abundant in in-cloud samples. Cirrus samples contain many H2SO4 droplets, but acidic sulfate particles are rare at the cloud bases. H2SO4 probably formed at higher altitudes through oxidation of SO2 in cloud droplets. The relatively high extent of ammoniation in the upper troposphere in-cloud samples appears to have resulted from vertical transport by strong convection. The morphology of H2SO4 droplets indicates that they had been at least yartiy ammoniated at the time of collection. They are internally mixed with organic materials, metal sulfates, and solid particles of various compositions. Ammoniation and internal mixing of result in freezing at higher temperature than in pure H2SO4 aerosols. K- and S-bearing organic particles and Si-Al-rich particles are common throughout. Sea salt and mineral dust were incorporated into the convective systems from the cloud bases and worked as ice nuclei while being vertically transported. The nonsulfate particles originated from the lower troposphere and were transported to the upper troposphere and lower stratosphere.

Buseck, Peter R.↗

Satellite Contributions to the Quantitative Characterization of Biomass Burning for Climate Modeling

Characterization of biomass burning from space has been the subject of an extensive body of literature published over the last few decades. Given the importance of this topic, we review how satellite observations contribute toward improving the representation of biomass burning quantitatively in climate and air-quality modeling and assessment. Satellite observations related to biomass burning may be classified into five broad categories: (i) active fire location and energy release, (ii) burned areas and burn severity, (iii) smoke plume physical disposition, (iv) aerosol distribution and particle properties, and (v) trace gas concentrations. Each of these categories involves multiple parameters used in characterizing specific aspects of the biomass-burning phenomenon. Some of the parameters are merely qualitative, whereas others are quantitative, although all are essential for improving the scientific understanding of the overall distribution (both spatial and temporal) and impacts of biomass burning. Some of the qualitative satellite datasets, such as fire locations, aerosol index, and gas estimates have fairly long-term records. They date back as far as the 1970s, following the launches of the DMSP, Landsat, NOAA, and Nimbus series of earth observation satellites. Although there were additional satellite launches in the 1980s and 1990s, space-based retrieval of quantitative biomass burning data products began in earnest following the launch of Terra in December 1999. Starting in 2000, fire radiative power, aerosol optical thickness and particle properties over land, smoke plume injection height and profile, and essential trace gas concentrations at improved resolutions became available. The 2000s also saw a large list of other new satellite launches, including Aqua, Aura, Envisat, Parasol, and CALIPSO, carrying a host of sophisticated instruments providing high quality measurements of parameters related to biomass burning and other phenomena. These improved data products have enabled significant progress in the study of biomass burning from space. However, appreciable uncertainty remains in many of the measurements that still needs to be addressed. Nevertheless, climate and other atmospheric models are

Ichoku, Charles↗

Atmospheric Condensational Properties of Ultrafine Chain and Fractal Aerosol Particles

The purpose for the research sponsored by this grant was to lay the foundations for qualitative understanding and quantitative description of the equilibrium vapor pressure of water vapor over the irregularly shaped, carbonaceous particles that are present in the atmosphere. This work apparently was the first systematic treatment of the subject. Research was conducted in two complementary components: 1. Calculations were performed of the equilibrium vapor pressure of water over particles comprised of aggregates of spheres in the 50-200 nm radius range. The purposes of this work were two-fold. First, since no systematic treatment of this subject had previously been conducted, its availability would be directly useful for quantitative treatment for a limited range of atmospheric aerosols. Second, it would provide qualitative indications of the effects of highly irregular particle shape on equilibrium vapor pressure of aggregates comprised of smaller spheres.

Marlow, William H.↗

The Evolution of Lidar Networks: A US Perspective

Atmospheric aerosols and clouds play an important role in climate by directly scattering and absorbing sunlight. Aerosol-cloud interactions modify the particle properties causing indirect effects, alter aerosol deposition and rainfall, and contribute substantially to the uncertainties in predicting climate effects. Aerosols also affect air quality and both constituents modulate boundary layer dynamics to a certain extent, in turn impacting aerosol transport and aerosol-cloud interactions. The spatiotemporal distribution of aerosol and cloud layers is thus important, and lidar remains the primary instrument for determining the vertical distribution of aerosols and thin clouds. Lidar still provides important information for opaque cloud layers by determining base heights. Combined lidar and radar data provide a comprehensive coverage of aerosol and cloud vertical distributions, and thus locations where and when they interact. Lidar data provide a means of constraining column aerosol loading observations (e.g. AOD) to vertical extents. In addition, lidar has proven effective at determining a proxy for boundary layer height by examining aerosol gradients and/or cloud base heights in lidar profiles. Polarized lidars provide additional information on particle shape, allowing estimates of cloud phase and separation of dust or smoke from sulfate and sea salt aerosols. Given the importance of lidar observations and a critical maturation in technology and retrieval techniques, several organizations began to build operational lidar networks around 2000. The European Aerosol Research Lidar Network (EARLINET) was started as a research focused network of advanced lidars across Europe. The Asian Dust Lidar Network (ADNET) was also developed as a regional network providing lidar profiles of dust and pollution across Eastern Asia. In the US, the NASA Micro Pulse Lidar Network (MPLNET) was created to provide global lidar profiling at key sites in the NASA Aerosol Robotic Network (AERONET). The Network for the Detection of Atmospheric Composition Change (NDACC) pre-dates these networks and many sites have lidar, but it is not strictly a lidar network and at the time focused less on the lower troposphere. Finally, there were already existing ceilometer networks operated by various meteorological agencies, but in particular here in the US the profile data has not been available. The ceilometer networks were used to provide only clouds base heights and estimates of PBL height. Thus, the distinguishing feature between lidar and ceilometer networks was historically the ability to actually provide profile information (in addition to differences in wavelength, and advanced retrievals such as the raman technique). As time progressed, each lidar network matured and developed more operational capabilities and data sets, coupled with viable data centers providing DAAC services and access to near-real-time (NRT) data. In 2008 under WMO guidance, the Global Atmospheric Watch (GAW) Aerosol Lidar Observation Network (GALION) was formed as a global network made up of the existing lidar networks. The goal was to share information, best practices, and develop frameworks and techniques for quality data. GALION grew to include several other regional lidar networks and this has led to a vast increase in quality lidar sites worldwide.

Welton, Ellsworth J.↗

Atmospheric aerosols: Their Optical Properties and Effects

Measured properties of atmospheric aerosol particles are presented. These include aerosol size frequency distribution and complex retractive index. The optical properties of aerosols are computed based on the presuppositions of thermodynamic equilibrium and of Mie-theory.

Source record↗

Chapter 10 - Remote Sensing Measurements of Aerosol Properties

Satellite instruments have proven especially capable at monitoring the quantity of airborne particles in columns of atmosphere, globally. This chapter describes the principles of satellite measurements and retrieval algorithms, and surveys current instruments and their capabilities. We outline the issues associated with retrieval algorithms, such as surface characterization and aerosol proximity to clouds, and the challenges with interpretation of the results. The relationship between measured aerosol properties and climate-relevant aerosol properties simulated in models is outlined, as well as how measurements are used to evaluate models. Most space-based aerosol instruments are passive sensors that measure reflected sunlight at multiple wavelengths, some at multiple viewing angles. A few are active sensors that send out their own laser light and measure the returned signal. Except when clouds are present, the excess amount of light scattered back to space, beyond that expected from the surface and atmospheric gas, is attributed to aerosol. Satellite measurements are used in many ways in aerosol research. They often provide the only method for monitoring hazardous phenomena such as major wildfire and volcanic eruption plumes, especially in remote areas. Stable, long-term, near-global-scale satellite data records make it possible to identify regional and global aerosol trends. Aerosol radiative effects on climate can be quantified on a near-global scale and used to estimate the strength of aerosol–radiation and aerosol–cloud interactions as well as to evaluate climate model simulations of these interactions. Aerosol-type mapping from satellite imagery is helpful for source attribution, model validation, and to constrain particle light-absorption properties that are essential for radiative forcing calculations. The range of aerosol properties retrieved from satellite observations has grown considerably since the first global estimates of aerosol optical depth (τ a) over ocean were made in the late 1970s. Methods for retrieving particle size and light-absorption properties were explored in the 1990s using multispectral, multi-angle observations, and polarization in visible and near-infrared wavelengths. Sensitivity to particle light absorption, primarily from black or brown carbon content, improved with the inclusion of UV channels, and sensitivity to very thin aerosol layers in the upper troposphere and lower stratosphere was advanced with the use of limb-sounding instruments and active sensors. There are limitations to every measurement technique, including satellite aerosol remote sensing. For wide-swath, passive instruments, aerosol retrievals near clouds can present substantial challenges as far as 15 km away due to cloud-scattered light contaminating the signal. In nearly all cases, retrievals over bright snow and ice surfaces are precluded because surface reflectance uncertainties can overwhelm the aerosol signal. Similarly, meteorological cloud is identified and masked out where possible. Data from passive sensors also lack vertical resolution except those that view toward the limb or where multi-angle imagery is acquired over plumes from wildfires, erupting volcanoes, and wind-blown dust. Yet, passive sensors provide vastly more coverage than the active instruments that mitigate these issues. Particle microphysical information is qualitative from all remote sensing techniques, relying on proxies to infer particle composition, hygroscopicity, and the amount of light-absorbing material. Further, particles smaller than about 200 nm diameter cannot be distinguished from atmospheric gas molecules with remote sensing, which hinders studies of cloud condensation nuclei and their effects on clouds. Most satellite instruments dedicated to aerosol observations are in low-Earth, near-polar, sun-synchronous orbits, which means they cross the equator at the same local time each day. Most are set on cycles that repeat approximately every 16 days, which makes it difficult to monitor aerosol evolution locally. Geostationary satellites make it possible to observe changes occurring from minutes to hours over regions up to 8000 km in size, but lack coverage of high latitudes, and often provide more limited constraints on aerosol properties. Ground-truth data are vital for satellite aerosol-retrieval validation. The AErosol RObotic NETwork (AERONET) of sun photometers was created in 1993 and has become an established global network of over 350 instruments for validating satellite measurements. The network, as well as global networks of ground-based lidars, solar flux radiometers and other sun photometers, are widely used for evaluating global satellite retrievals and model simulations. NASA's Earth Observing System (EOS) program beginning in 1999 led to improvements in reliability, spatial resolution, and spectral resolution (and hence, to improved particle size discrimination and light absorption properties). Satellite payloads include advanced broad-swath and multi-angle imagers, along with the first space-based active sensor focused largely on long-term aerosol monitoring. Since about 2002, Europe's SENTINEL and operational meteorological satellite fleets are also providing sustained aerosol observations, with planned continuation until at least 2030. Satellite remote sensing instruments offer valuable data for evaluating aerosol representations in global climate models. They have been used to assess aerosol optical and physical properties, trends and distributions, and are applied increasingly as direct model constraints in data assimilation to create global aerosol reanalysis products. Aerosol optical depth is the most common quantity adopted for routine model evaluation, including multiwavelength data to loosely constrain particle-size distributions. These evaluations of multiple models have revealed general biases in their regional aerosol amounts and seasonal patterns of transport and removal. Although satellite measurements have near-global coverage, substantial errors can be introduced into the model observation comparison unless attention is paid to spatial and temporal collocation, cloud screening, subgrid-scale variability, and measurement uncertainties that vary with retrieval conditions.

aerosol properties↗

Validation of the aerosol optical property products derived by the GRASP/Component approach from multi-angular polarimetric observations

The multi-angle polarimetric satellite observations are helpful for improving the retrievals of aerosol parameters. However, practical applications of polarization technology are still limited because of complexity of measurement and interpretation of polarimetric observations. In this study, we analyze the performance of a new component approach developed in the frame of the Generalized Retrieval of Atmosphere and Surface Properties (GRASP) algorithm. In addition to aerosol optical properties including particle size distribution, non-sphericity and index of refraction that are commonly derived from multi-angle radiance and polarization measurements, the GRASP/Component approach also provides some information about aerosol composition. Specifically, in this approach aerosol is modeled as an internal mixture of several components with distinctly different chemical compositions and known refractive indices. The approach is intended not only to provide additional insight on aerosol composition but also to improve retrieval of basic aerosol optical properties. This study presents comprehensive validation and evaluation of Aerosol Optical Depth (AOD), Ångstrom exponent (AE), fine mode AOD (AODF), coarse mode AOD (AODC), and single scattering albedo (SSA) as retrieved by the GRASP/Component approach. The GRASP/Component products include aerosol retrievals using two different aerosol component mixing rules, i.e., Maxwell-Garnett (MG) effective medium approximation and a simple Volume- Weighted averaging (VW). The differences between the results obtained using these two assumptions are also discussed. The obtained results show that the aerosol optical property products of GRASP/Component approach have good agreement with the ground-based AERONET measurements, which is comparable to other PARASOL/ GRASP approaches. Specifically, the AOD retrieved by GRASP/Component approach show high correlation and nearly no bias both over land and ocean, as compared with AERONET. The more detailed aerosol properties such as AE, AODF, AODC and SSA also show one of the best comparisons with AERONET. These improvements can probably be attributed to the use of the additional physical constraints on spectral dependence of the complex refractive index and the reduction of total number of aerosol parameters directly retrieved in the GRASP/Component approach. In addition, the choice of mixing rules had no significant effect on optical retrievals. With the exception of SSA, the results obtained based on the MG mixing rule were found to be slightly better over those obtained using VW mixing rule, especially for bias.

Brent N Holben↗

Direct Aerosol Radiative Forcing: Calculations and Measurements from the Tropospheric

Radiative forcing is defined as the change in the net (downwelling minus upwelling) radiative flux at a given level in the atmosphere. This net flux is the radiative power density available to drive climatic processes in the earth-atmosphere system below that level. Recent research shows that radiative forcing by aerosol particles is a major source of uncertainty in climate predictions. To reduce those uncertainties, TARFOX was designed to determine direct (cloud-free) radiative forcing by the aerosols in one of the world's major industrial pollution plumes--that flowing from the east coast of the US over the Atlantic Ocean. TARFOX measured a variety of aerosol radiative effects (including direct forcing) while simultaneously measuring the chemical, physical, and optical properties of the aerosol particles causing those effects. The resulting data sets permit a wide variety of tests of the consistency, or closure, among the measurements and the models that link them. Because climate predictions use the same or similar model components, closure tests help to assess and reduce prediction uncertainties. In this work we use the TARFOX-determined aerosol, gas, and surface properties to compute radiative forcing for a variety of aerosol episodes, with inadvisable optical depths ranging from 0.07 to 0.6. We calculate forcing by several techniques with varying degrees of sophistication, in part to test the range of applicability of simplified techniques--which are often the only ones feasible in climate predictions by general circulation models (GCMs). We then compare computed forcing to that determined from: (1) Upwelling and downwelling fluxes (0.3-0.7 mm and 0.7-3.0 mm) measured by radiometers on the UK MRF C-130. and (2) Daily average cloud-free absorbed solar and emitted thermal radiative flux at the top of the atmosphere derived from the AVHRR radiometer on the NOAA- 14 satellite. The calculations and measurements all yield aerosol direct radiative forcing in the range -50 to -190 W sq m per unit inadvisable optical depth. The magnitudes are about 15 to 100 times larger than the global-average direct forcing expected for the global-average sulfate aerosol optical depth of 0.04. The reasons for the larger forcing in TARFOX include the relatively large optical depths and the focus on cloud-free, daytime conditions over the dark ocean surface. These are the conditions that produce the actual major radiative forcing events that contribute to any global-average climate effect. Detailed comparisons of calculated and measured forcings for specific events are used for more refined tests of closure.

Russell, P. B.↗

Scattering and absorption from poly-dispersed aerosols

Results from numerical computations of the diffuse sky radiances and degree of polarization are given. These results were obtained by solving the equation of radiative transfer in the formulation of Eschelbach. In these computations, multiple scattering and absorption by aerosol particles were considered. In addition, results from experimental measurements of the complex refractive index of aerosol samples at different relative humidities are presented. From the radiation flux divergences which were computed based on the determined properties of atmospheric aerosol particles, atmospheric heating rates were derived which were found to be comparable to the heating rates by water vapor.

Bullrich, K.↗

Aerosol-Induced Radiative Flux Changes Off the United States Mid-Atlantic Coast: Comparison of Values Calculated from Sunphotometer and In Situ Data with Those Measured by Airborne Pyranometer

The Tropospheric Aerosol Radiative Forcing Observational Experiment (TARFOX) measured a variety of aerosol radiative effects (including flux changes) while simultaneously measuring the chemical, physical, and optical properties of the responsible aerosol particles. Here we use TARFOX-determined aerosol and surface properties to compute shortwave radiative flux changes for a variety of aerosol situations, with midvisible optical depths ranging from 0.06 to 0.55. We calculate flux changes by several techniques with varying degrees of sophistication, in part to investigate the sensitivity of results to computational approach. We then compare computed flux changes to those determined from aircraft measurements. Calculations using several approaches yield downward and upward flux changes that agree with measurements. The agreement demonstrates closure (i.e. consistency) among the TARFOX-derived aerosol properties, modeling techniques, and radiative flux measurements. Agreement between calculated and measured downward flux changes is best when the aerosols are modeled as moderately absorbing (midvisible single-scattering albedos between about 0.89 and 0.93), in accord with independent measurements of the TARPOX aerosol. The calculated values for instantaneous daytime upwelling flux changes are in the range +14 to +48 W/sq m for midvisible optical depths between 0.2 and 0.55. These values are about 30 to 100 times the global-average direct forcing expected for the global-average sulfate aerosol optical depth of 0.04. The reasons for the larger flux changes in TARFOX include the relatively large optical depths and the focus on cloud-free, daytime conditions over the dark ocean surface. These are the conditions that produce major aerosol radiative forcing events and contribute to any global-average climate effect.

Russell, P. B.↗