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Laboratory experiments in the study of the chemistry of the outer planets

It is shown that much information about planetary chemistry and physics can be gained through laboratory work. The types of experiments relevant to planetary research concern fundamental properties, spectral/optical properties, 'Miller-Urey' syntheses, and detailed syntheses. Specific examples of studies of the chemistry in the atmosphere of Titan are described with attention given to gas phase chemistry in the troposphere and the composition of model Titan aerosols. A list of work that still needs to be done is provided.

Scattergood, Thomas W.↗

Use of aerosol microphysical measurements to model IR backscatter in support of GLOBE

Data on the concentration and composition of free tropospheric aerosol over the Pacific Ocean, collected during the GAMETAG program in 1977-1978 (Davis, 1980 and Patterson et al., 1980) are used to model values of aerosol optical extinction coefficients (sigma) at two wavelengths (0.55 and 1 micron) and values of volume backscatter coefficients (beta) at four wavelengths (1 micron, 9.11 microns, 9.25 microns, and 10.6 microns) and to investigate the relationship between these parameters. The mass concentrations inferred from the GAMETAG measurements with optical particle spectrometers agreed with the results of simultaneous chemical measurements. The study of the relationships among the optical parameters indicates that visible and near-visible values of beta and sigma may be useful in predicting 9.11- and 10.6-micron backscatter.

Patterson, Edward M.↗

The Arctic Boundary Layer Expedition (ABLE 3A) - July-August 1988

The Arctic Boundary Layer Expedition (ABLE 3A), conducted in Arctic and sub-Arctic regions of North America and Greenland during July and August 1988, was the first comprehensive investigation of the sources, sinks, and distribution of trace gas and aerosol chemical species in a northern high-latitude region during summer months. The experimental design emphasized the role of biosphere-atmosphere interactions in determining the chemical composition of the troposphere and in processes which influence the tropospheric O3 budget. This paper reports the overall experimental design of ABLE 3A and includes a brief overview of results.

Harriss, R. C.↗

Ice Nucleation in Deep Convection

The processes controlling production of ice crystals in deep, rapidly ascending convective columns are poorly understood due to the difficulties involved with either modeling or in situ sampling of these violent clouds. A large number of ice crystals are no doubt generated when droplets freeze at about -40 C. However, at higher levels, these crystals are likely depleted due to precipitation and detrainment. As the ice surface area decreases, the relative humidity can increase well above ice saturation, resulting in bursts of ice nucleation. We will present simulations of these processes using a large-eddy simulation model with detailed microphysics. Size bins are included for aerosols, liquid droplets, ice crystals, and mixed-phase (ice/liquid) hydrometers. Microphysical processes simulated include droplet activation, freezing, melting, homogeneous freezing of sulfate aerosols, and heterogeneous ice nucleation. We are focusing on the importance of ice nucleation events in the upper part of the cloud at temperatures below -40 C. We will show that the ultimate evolution of the cloud in this region (and the anvil produced by the convection) is sensitive to these ice nucleation events, and hence to the composition of upper tropospheric aerosols that get entrained into the convective column.

Jensen, Eric↗

Titan's Atmospheric Dynamics and Meteorology

Titan, after Venus, is the second example of an atmosphere with a global cyclostrophic circulation in the solar system, but a circulation that has a strong seasonal modulation in the middle atmosphere. Direct measurement of Titan's winds, particularly observations tracking the Huygens probe at 10degS, indicate that the zonal winds are generally in the sense of the satellites rotation. They become cyclostrophic approx. 35 km above the surface and generally increase with altitude, with the exception of a sharp minimum centered near 75 km, where the wind velocity decreases to nearly zero. Zonal winds derived from the temperature field retrieved from Cassini measurements, using the thermal wind equation, indicate a strong winter circumpolar vortex, with maximum winds at mid northern latitudes of 190 ms-' near 300 km. Above this level, the vortex decays. Curiously, the zonal winds and temperatures are symmetric about a pole that is offset from the surface pole by approx.4 degrees. The cause of this is not well understood, but it may reflect the response of a cyclostrophic circulation to the offset between the equator, where the distance to the rotation axis is greatest, and the solar equator. The mean meridional circulation can be inferred from the temperature field and the meridional distribution of organic molecules and condensates and hazes. Both the warm temperatures in the north polar region near 400 km and the enhanced concentration of several organic molecules suggests subsidence there during winter and early spring. Stratospheric condensates are localized at high northern latitudes, with a sharp cut-off near 50degN. Titan's winter polar vortex appears to share many of the same characteristics of winter vortices on Earth-the ozone holes. Global mapping of temperatures, winds, and composition in he troposphere, by contrast, is incomplete. The few suitable discrete clouds that have bee found for tracking indicate smaller velocities than aloft, consistent with the Huygens measurements. At low latitudes the zonal winds near the surface appear not to be westward as on Earth, but eastward. Because the net zonal-mean time-averaged torq exerted by the surface on the atmosphere should vanish, this implies westward flow o part of the surface; the question is where. The latitude contrast in tropospheric temperatures, deduced from radio occultations at low, mid, and high latitudes, is small approx.5 K at the tropopause and approx.3 K at the surface.

Flasar, F. M.↗

OMI Validation from the SAUNA and ARCTAS Campaigns

Initial results are presented on Ozone Monitoring Instrumnet (OMI) validation from the Sodankyla Total Column Ozone Intercomparison (SAUNA) and from the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. SAUNA was held in Sodankyla, Finland in March-April 2006 and February-March 2007 in support of Aura validation. The purpose of SAUNA was to assess the comparative performance of the ground-based instruments and algorithms when measuring total column ozone at large solar zenith angles and high total column ozone amounts. Results showed that the ozone profiles from the satellite instruments (MLS on Aura and SBUV/2 on NOAA 16) generally agreed with profiles from the ground-based instruments (lidar and sondes) within 10%. The ARCTAS spring campaign was flown out of Fairbanks, Alaska, from, April 1 - April 19, 2008. The purpose of ARCTAS was to study arctic haze and pollution sources in the arctic, but also to provide validation of CALIPSO and Aura. The differences between the OMI OMTO3 ozone retrieval and the DOAS ozone are examined.

McPeters, R. D.↗

Enhancements and Evolution of the Real Time Mission Monitor

The Real Time Mission Monitor (RTMM) is a visualization and information system that fuses multiple Earth science data sources, to enable real time decision-making for airborne and ground validation experiments. Developed at the National Aeronautics and Space Administration (NASA) Marshall Space Flight Center, RTMM is a situational awareness, decision-support system that integrates satellite imagery, radar, surface and airborne instrument data sets, model output parameters, lightning location observations, aircraft navigation data, soundings, and other applicable Earth science data sets. The integration and delivery of this information is made possible using data acquisition systems, network communication links, network server resources, and visualizations through the Google Earth virtual globe application. RTMM has proven extremely valuable for optimizing individual Earth science airborne field experiments. Flight planners, mission scientists, instrument scientists and program managers alike appreciate the contributions that RTMM makes to their flight projects. We have received numerous plaudits from a wide variety of scientists who used RTMM during recent field campaigns including the 2006 NASA African Monsoon Multidisciplinary Analyses (NAMMA), 2007 Tropical Composition, Cloud, and Climate Coupling (TC4), 2008 Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) missions, the 2007-2008 NOAA-NASA Aerosonde Hurricane flights and the 2008 Soil Moisture Active-Passive Validation Experiment (SMAP-VEX). Improving and evolving RTMM is a continuous process. RTMM recently integrated the Waypoint Planning Tool, a Java-based application that enables aircraft mission scientists to easily develop a pre-mission flight plan through an interactive point-and-click interface. Individual flight legs are automatically calculated for altitude, latitude, longitude, flight leg distance, cumulative distance, flight leg time, cumulative time, and satellite overpass intersections. The resultant flight plan is then generated in KML and quickly posted to the Google Earth-based RTMM for interested scientists to view the planned flight track and then compare it to the actual real time flight progress. A description of the system architecture, components, and applications along with reviews and animations of RTMM during the field campaigns, plus planned enhancements and future opportunities will be presented.

Goodman, Michael↗

Spatio-Temporal Variability of Atmospheric CO2 as Observed from In-Situ Measurements over North America during NASA Field Campaigns (2004-2008)

Regional-scale measurements were made over the eastern United States (Intercontinental Chemical Transport Experiment - North America (INTEX-NA), summer 2004); Mexico (Megacity Initiative: Local and Global Research Observations (MILAGRO), March 2006); the eastern North Pacific and Alaska (INTEX-B May 2006); and the Canadian Arctic (Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS), spring and summer 2008). For these field campaigns, instrumentation for the in situ measurement of CO2 was integrated on the NASA DC-8 research aircraft providing high-resolution (1 second) data traceable to the WMO CO2 mole fraction scale. These observations provide unique and definitive data sets via their intermediate-scale coverage and frequent vertical profiles (0.1 - 12 km) for examining the variability CO2 exhibits above the Earth s surface. A bottom-up anthropogenic CO2 emissions inventory (1deg 1deg) and processing methodology has also been developed for North America in support of these airborne science missions. In this presentation, the spatio-temporal distributions of CO2 and CO column values derived from the campaign measurements will be examined in conjunction with the emissions inventory and transport histories to aid in the interpretation of the CO2 observations.

Choi, Yonghoon↗

Chapter 13. Atmospheric Dynamics and Meteorology

Titan, after Venus, is the second example in the solar system of an atmosphere with a global cyclostrophic circulation, but in this case a circulation that has a strong seasonal modulation in the middle atmosphere. Direct measurement of Titan's winds, particularly observations tracking the Huygens probe at 10 deg S, indicate that the zonal winds are mostly in the sense of the satellite's rotation. They generally increase with altitude and become cyclostrophic near 35 km above the surface. An exception to this is a sharp minimum centered near 75 km, where the wind velocity decreases to nearly zero. Zonal winds derived from temperatures retrieved from Cassini orbiter measurements, using the thermal wind equation, indicate a strong winter circumpolar vortex, with maximum winds of 190 m/s at mid northern latitudes near 300 km. Above this level, the vortex decays. Curiously, the stratospheric zonal winds and temperatures in both hemispheres are symmetric about a pole that is offset from the surface pole by about 4 deg. The cause of this is not well understood, but it may reflect the response of a cyclostrophic circulation to the onset between the equator, where the distance to the rotation axis is greatest, and the seasonally varying subsolar latitude. The mean meridional circulation can be inferred from the temperature field and the meridional distribution of organic molecules and condensates and hazes. Both the warm temperatures near 400 km and the enhanced concentration of several organic molecules suggest subsidence in the north polar region during winter and early spring. Stratospheric condensates are localized at high northern latitudes, with a sharp cut-off near 50 deg N. Titan's winter polar vortex appears to share many of the same characteristics of isolating high and low-latitude air masses as do the winter polar vortices on Earth that envelop the ozone holes. Global mapping of temperatures, winds, and composition in the troposphere, by contrast, is incomplete. The few suitable discrete clouds that have been found for tracking indicate smaller velocities than aloft, consistent: with the Huygens measurements, Along the descent trajectory, the Huygens measurements indicate eastward zonal winds down to 7 km, where they shift westward, and then eastward again below 1 km dawn to the surface. The low-latitude dune fields seen in Cassini RADAR images have been interpreted as longitudinal dunes occurring in a mean eastward zonal wind. This is not like Earth, where the low-latitude winds are westward above the surface. Because the net zonal-mean time-averaged torque exerted by the surface on the atmosphere should vanish, there must be westward flow over part of the surface; the question is where and when. The meridional contrast in tropospheric temperatures deduced from radio occultations at low, mid, and high latitudes. is small, approximately 5 K at the tropopause and approximately 3 K at the surface. This implies efficient heat transport, probably by axisymmetric meridional circulations. The effect of the methane "hydrological" cycle on the atmospheric circulation is not well constrained by existing measurements, Understanding the mature of the surface-atmosphere coupling will be critical to elucidating the atmospheric transports of momentum, heat, and volatiles.

Flasar, F. M.↗

Visualizing Airborne and Satellite Imagery

Remote sensing is a process able to provide information about Earth to better understand Earth's processes and assist in monitoring Earth's resources. The Cloud Absorption Radiometer (CAR) is one remote sensing instrument dedicated to the cause of collecting data on anthropogenic influences on Earth as well as assisting scientists in understanding land-surface and atmospheric interactions. Landsat is a satellite program dedicated to collecting repetitive coverage of the continental Earth surfaces in seven regions of the electromagnetic spectrum. Combining these two aircraft and satellite remote sensing instruments will provide a detailed and comprehensive data collection able to provide influential information and improve predictions of changes in the future. This project acquired, interpreted, and created composite images from satellite data acquired from Landsat 4-5 Thematic Mapper (TM) and Landsat 7 Enhanced Thematic Mapper plus (ETM+). Landsat images were processed for areas covered by CAR during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCT AS), Cloud and Land Surface Interaction Campaign (CLASIC), Intercontinental Chemical Transport Experiment-Phase B (INTEXB), and Southern African Regional Science Initiative (SAFARI) 2000 missions. The acquisition of Landsat data will provide supplemental information to assist in visualizing and interpreting airborne and satellite imagery.

Bierwirth, Victoria A.↗

Simultaneous Retrieval of Aerosol and Surface Optical Properties from Combined Airborne- and Ground-Based Direct and Diffuse Radiometric Measurements

This paper presents a new method for simultaneously retrieving aerosol and surface reflectance properties from combined airborne and ground-based direct and diffuse radiometric measurements. The method is based on the standard Aerosol Robotic Network (AERONET) method for retrieving aerosol size distribution, complex index of refraction, and single scattering albedo, but modified to retrieve aerosol properties in two layers, below and above the aircraft, and parameters on surface optical properties from combined datasets (Cloud Absorption Radiometer (CAR) and AERONET data). A key advantage of this method is the inversion of all available spectral and angular data at the same time, while accounting for the influence of noise in the inversion procedure using statistical optimization. The wide spectral (0.34-2.30 m) and angular range (180 ) of the CAR instrument, combined with observations from an AERONET sunphotometer, provide sufficient measurement constraints for characterizing aerosol and surface properties with minimal assumptions. The robustness of the method was tested on observations made during four different field campaigns: (a) the Southern African Regional Science Initiative 2000 over Mongu, Zambia, (b) the Intercontinental Transport Experiment-Phase B over Mexico City, Mexico (c) Cloud and Land Surface Interaction Campaign over the Atmospheric Radiation Measurement (ARM) Central Facility, Oklahoma, USA, and (d) the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) over Elson Lagoon in Barrow, Alaska, USA. The four areas are dominated by different surface characteristics and aerosol types, and therefore provide good test cases for the new inversion method.

Gatebe, C. K.↗

Analysis of Snow Bidirectional Reflectance from ARCTAS Spring-2008 Campaign

The spring 2008 Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) experiment was one of major intensive field campaigns of the International Polar Year aimed at detailed characterization of atmospheric physical and chemical processes in the Arctic region. A part of this campaign was a unique snow bidirectional reflectance experiment on the NASA P-3B aircraft conducted on 7 and 15 April by the Cloud Absorption Radiometer (CAR) jointly with airborne Ames Airborne Tracking Sunphotometer (AATS) and ground-based Aerosol Robotic Network (AERONET) sunphotometers. The CAR data were atmospherically corrected to derive snow bidirectional reflectance at high 1 degree angular resolution in view zenith and azimuthal angles along with surface albedo. The derived albedo was generally in good agreement with ground albedo measurements collected on 15 April. The CAR snow bidirectional reflectance factor (BRF) was used to study the accuracy of analytical Ross-Thick Li-Sparse (RTLS), Modified Rahman-Pinty-Verstraete (MRPV) and Asymptotic Analytical Radiative Transfer (AART) BRF models. Except for the glint region (azimuthal angles phi less than 40 degrees), the best fit MRPV and RTLS models fit snow BRF to within 0.05. The plane-parallel radiative transfer (PPRT) solution was also analyzed with the models of spheres, spheroids, randomly oriented fractal crystals, and with a synthetic phase function. The latter merged the model of spheroids for the forward scattering angles with the fractal model in the backscattering direction. The PPRT solution with synthetic phase function provided the best fit to measured BRF in the full range of angles. Regardless of the snow grain shape, the PPRT model significantly over-/underestimated snow BRF in the glint/backscattering regions, respectively, which agrees with other studies. To improve agreement with experiment, we introduced a model of macroscopic snow surface roughness by averaging the PPRT solution over the slope distribution function and by adding a simple model of shadows. With macroscopic roughness described by two parameters, the AART model achieved an accuracy of about plus or minus 0.05 with a possible bias of plus or minus 0.03 in the spectral range 0.4-2.2 micrometers. This high accuracy holds at view zenith angles below 55-60 degrees covering the practically important range for remote sensing applications, and includes both glint and backscattering directions.

Lyapustin, A.↗

Taking the Pulse of PyroCumulus Clouds

Forest fires can burn large areas, but can also inject smoke into the upper troposphere/lower stratosphere (UT/LS), where stakes are even higher for climate, because emissions tend to have a longer lifetime, and can produce significant regional and even global climate effects, as is the case with some volcanoes. Large forest fires are now believed to be more common in summer, especially in the boreal regions, where pyrocumulus (pyroCu), and occasionally pyrocumuionimbus (pyroCb) clouds are formed, which can transport emissions into the UT/LS. A major difficulty in developing realistic fire plume models is the lack of observational data within fire plumes that resolves structure at a few 100 m scales, which can be used to validate these models. Here, we report detailed airborne radiation measurements within strong pyroCu taken over boreal forest fires in Saskatchewan, Canada during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) summer field campaign in 2008. We find that the angular distribution of radiance within the pyroCu is closely related to the diffusion domain in water clouds and can be described by very similar simple cosine functions. We demonstrate with Monte Carlo simulations that radiation transport in pyroCu is inherently a 3D phenomenon and must account for particle absorption. However, the simple cosine function promises to offer an easy solution for climate models. The presence of a prominent smoke core, defined by strong extinction in the UV, VIS and NIR, suggests that the core might be an important pathway for emission transport to the upper troposphere and lower stratosphere. We speculate that this plume injection core is generated and sustained by complex processes not yet well understood, but not necessarily related directly to the intense fires that originally initiated the plume rise.

Gatebe, C. K.↗

Combined Retrievals of Boreal Forest Fire Aerosol Properties with a Polarimeter and Lidar

Absorbing aerosols play an important, but uncertain, role in the global climate. Much of this uncertainty is due to a lack of adequate aerosol measurements. While great strides have been made in observational capability in the previous years and decades, it has become increasingly apparent that this development must continue. Scanning polarimeters have been designed to help resolve this issue by making accurate, multi-spectral, multi-angle polarized observations. This work involves the use of the Research Scanning Polarimeter (RSP). The RSP was designed as the airborne prototype for the Aerosol Polarimetery Sensor (APS), which was due to be launched as part of the (ultimately failed) NASA Glory mission. Field observations with the RSP, however, have established that simultaneous retrievals of aerosol absorption and vertical distribution over bright land surfaces are quite uncertain. We test a merger of RSP and High Spectral Resolution Lidar (HSRL) data with observations of boreal forest fire smoke, collected during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS). During ARCTAS, the RSP and HSRL instruments were mounted on the same aircraft, and validation data were provided by instruments on an aircraft flying a coordinated flight pattern. We found that the lidar data did indeed improve aerosol retrievals using an optimal estimation method, although not primarily because of the constraints imposed on the aerosol vertical distribution. The more useful piece of information from the HSRL was the total column aerosol optical depth, which was used to select the initial value (optimization starting point) of the aerosol number concentration. When ground based sun photometer network climatologies of number concentration were used as an initial value, we found that roughly half of the retrievals had unrealistic sizes and imaginary indices, even though the retrieved spectral optical depths agreed within uncertainties to independent observations. The convergence to an unrealistic local minimum by the optimal estimator is related to the relatively low sensitivity to particles smaller than 0.1 ( m) at large optical thicknesses. Thus, optimization algorithms used for operational aerosol retrievals of the fine mode size distribution, when the total optical depth is large, will require initial values generated from table look-ups that exclude unrealistic size/complex index mixtures. External constraints from lidar on initial values used in the optimal estimation methods will also be valuable in reducing the likelihood of obtaining spurious retrievals.

Knobelspiesse, K.↗

The Response of Lower Atmospheric Ozone to ENSO in Aura Measurements and a Chemistry-Climate Simulation

The El Nino-Southern Oscillation (ENSO) is the dominant mode of tropical variability on interannual time scales. ENSO appears to extend its influence into the chemical composition of the tropical troposphere. Recent work has revealed an ENSO-induced wave-1 anomaly in observed tropical tropospheric column ozone. This results in a dipole over the western and eastern tropical Pacific, whereby differencing the two regions produces an ozone anomaly with an extremely high correlation to the Nino 3.4 Index. We have successfully reproduced this feature using the Goddard Earth Observing System Version 5 (GEOS-5) general circulation model coupled to a comprehensive stratospheric and tropospheric chemical mechanism forced with observed sea surface temperatures over the past 25 years. An examination of the modeled ozone field reveals the vertical contributions of tropospheric ozone to the column over the western and eastern Pacific region. We will show composition sensitivity in observations from NASA s Aura satellite Microwave Limb Sounder (MLS) and the Tropospheric Emissions Spectrometer (TES) and a simulation to provide insight into the vertical structure of these ENSO-induced ozone changes. The ozone changes due to the Quasi-Biennial Oscillation (QBO) in the extra-polar upper troposphere and lower stratosphere in MLS measurements will also be discussed.

Oman, L. D.↗

Source Attributions of Pollution to the Western Arctic During the NASA ARCTAS Field Campaign

We use the NASA GEOS-5 transport model with tagged tracers to investigate the contributions of different regional sources of CO and black carbon (BC) to their concentrations in the Western Arctic (i.e., 50-90 deg N and 190- 320 deg E) in spring and summer 2008. The model is evaluated by comparing the results with airborne measurements of CO and BC from the NASA Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) field campaigns to demonstrate the strengths and limitations of our simulations. We also examine the reliability of tagged CO tracers in characterizing air mass origins using the measured fossil fuel tracer of dichloromethane and the biomass burning tracer of acetonitrile. Our tagged CO simulations suggest that most of the enhanced CO concentrations (above background level from CH4 production) observed during April originate from Asian anthropogenic emissions. Boreal biomass burning emissions and Asian anthropogenic emissions are of similar importance in July domain wise, although the biomass burning CO fraction is much larger in the area of the ARCTAS field experiments. The fraction of CO from Asian anthropogenic emissions is larger in spring than in summer. European sources make up no more than 10% of CO levels in the campaign domain during either period. Comparisons of CO concentrations along the flight tracks with regional averages from GEOS-5 show that the alongtrack measurements are representative of the concentrations within the large domain of the Western Arctic in April but not in July.

Black Carbon↗

Radiative Characteristics of Clouds Embedded in Smoke Derived from Airborne Multiangular Measurements

Clouds in the presence of absorbing aerosols result in their apparent darkening, observed at the top of atmosphere (TOA), which is associated with the radiative effects of aerosol absorption. Owing to the large radiative effect and potential impacts on regional climate, above-cloud aerosols have recently been characterized in multiple satellite-based studies. While satellite data are particularly useful in showing the radiative impact of above-cloud aerosols at the TOA, recent literature indicates large uncertainties in satellite retrievals of above-cloud aerosol optical depth (AOD) and single scattering albedo (SSA), which are among the most important parameters in the assessment of associated radiative effects. In this study, we analyze radiative characteristics of clouds in the presence of wildfire smoke using airborne data primarily from NASA's Cloud Absorption Radiometer, collected during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites campaign in Canada during the 2008 summer season. We found a strong positive reflectance (R) gradient in the UV-visible (VIS)-near infrared (NIR) spectrum for clouds embedded in dense smoke, as opposed to an (expected) negative gradient for cloud-free smoke and a flat spectrum for smoke-free cloud cover. Several cases of clouds embedded in thick smoke were found, when the aircraft made circular/spiral measurements, which not only allowed the complete characterization of angular distribution of smoke scattering but also provided the vertical distribution of smoke and clouds (within 0.5-5 km). Specifically, the largest darkening by smoke was found in the UV/VIS, with R(sub 0.34 microns) reducing to 0.2 (or 20%), in contrast to 0.8 at NIR wavelengths (e.g., 1.27 microns). The observed darkening is associated with large AODs (0.5-3.0) and moderately low SSA (0.85-0.93 at 0.53 microns), resulting in a significantly large instantaneous aerosol forcing efficiency of 254 +/- 47 W/sq m/τ. Our observations of smoke-cloud radiative interactions were found to be physically consistent with theoretical plane-parallel 1-D and Monte Carlo 3-D radiative transfer calculations, capturing the observed gradient across UV-VIS-NIR. Results from this study offer insights into aerosol-cloud radiative interactions and may help in better constraining satellite retrieval algorithms.

absorbing aerosols↗

Evaluating Model Parameterizations of Submicron Aerosol Scattering and Absorption with in situ Data from ARCTAS 2008

Accurate modeling of the scattering and absorption of ultraviolet and visible radiation by aerosols is essential for accurate simulations of atmospheric chemistry and climate. Closure studies using in situ measurements of aerosol scattering and absorption can be used to evaluate and improve models of aerosol optical properties without interference from model errors in aerosol emissions, transport, chemistry, or deposition rates. Here we evaluate the ability of four externally mixed, fixed size distribution parameterizations used in global models to simulate submicron aerosol scattering and absorption at three wavelengths using in situ data gathered during the 2008 Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. The four models are the NASA Global Modeling Initiative (GMI) Combo model, GEOS-Chem v9- 02, the baseline configuration of a version of GEOS-Chem with online radiative transfer calculations (called GC-RT), and the Optical Properties of Aerosol and Clouds (OPAC v3.1) package. We also use the ARCTAS data to perform the first evaluation of the ability of the Aerosol Simulation Program (ASP v2.1) to simulate submicron aerosol scattering and absorption when in situ data on the aerosol size distribution are used, and examine the impact of different mixing rules for black carbon (BC) on the results. We find that the GMI model tends to overestimate submicron scattering and absorption at shorter wavelengths by 10-23 percent, and that GMI has smaller absolute mean biases for submicron absorption than OPAC v3.1, GEOS-Chem v9-02, or GC-RT. However, the changes to the density and refractive index of BC in GCRT improve the simulation of submicron aerosol absorption at all wavelengths relative to GEOS-Chem v9-02. Adding a variable size distribution, as in ASP v2.1, improves model performance for scattering but not for absorption, likely due to the assumption in ASP v2.1 that BC is present at a constant mass fraction throughout the aerosol size distribution. Using a core-shell mixing rule in ASP overestimates aerosol absorption, especially for the fresh biomass burning aerosol measured in ARCTAS-B, suggesting the need for modeling the time-varying mixing states of aerosols in future versions of ASP.

Alvarado, Matthew J.↗