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Cloud Spatial Structure and 3D Radiative Transfer

Cloud radiative properties are sensitive to drop size and other parameters of cloud micro-structure, but also to cloud shape, spacing, and other parameters of cloud macro-structure, including internal fractal structure. New information on cloud structure is being derived from a variety of cloud radars and lidars. Ongoing field programs such as DoE/ARM are improving the measurement and modelling of physical and radiative properties of clouds. A parallel effort is underway to improve cloud remote sensing, especially from the new suite of EOS (Earth Observing System) instruments which are beginning to provide higher spectral, spatial resolution, and/or angular resolution. Key parameters for improving pixel-scale retrievals are cloud thickness and photon mean-free-path, which together determine the scale of "radiative smoothing" of cloud fluxes and radiances. This scale has been observed as a change in the spatial spectrum of Landsat cloud radiances, and was also recently found with the Goddard micropulse lidar, by searching for returns from directions nonparallel to the incident beam. "Offbeam" Lidar returns are now being used to estimate the cloud "radiative Green's function", (G). G depends on cloud thickness and may be used to retrieve that important quantity. G is also being applied to improving simple estimates of cloud radiative properties that are based on the "Independent Pixel Approximation" or IPA. This and other measurements of 3D transfer in clouds, coupled with Monte Carlo and other 3D transfer methods, are beginning to provide a better understanding of the dependence of radiation on cloud inhomogeneity, and to suggest new retrieval and parameterization algorithms which take account of cloud inhomogeneity. An international "Intercomparison of 3D Radiation Codes" or I3RC, program is underway to coordinate and evaluate the variety of 3D radiative transfer methods now available, and to make them more widely available. Information is on the Web at: http://climate.gsfc.nasa.gov/I3RC. Input consists of selected cloud fields derived from data sources such as radar, microwave and satellite, and from models involved in the GEWEX Cloud Systems Studies. Output is selected radiative quantities that characterize the large-scale properties of the fields of radiative fluxes and heating. Several example cloud fields will be used to illustrate the effects of cloud inhomogeneity and 3D radiation.

Cahalan, Robert F.↗

Cloud Spatial Structure and 3D Radiative Transfer

Cloud radiative properties are sensitive to drop size and other parameters of cloud micro-structure, but also to cloud shape, spacing, and other parameters of cloud macro-structure, including internal fractal structure. New information on cloud structure is being derived from a variety of cloud radars and lidars. Ongoing field programs such as DoE/ARM (atmospheric radiation measurement) are improving the measurement and modelling of physical and radiative properties of clouds. A parallel effort is underway to improve cloud remote sensing, especially from the new suite of EOS (Earth observing system) instruments which are beginning to provide higher spectral, spatial resolution, and/or angular resolution. Key parameters for improving pixel-scale retrievals are cloud thickness and photon mean-free-path, which together determine the scale of 'radiative smoothing' of cloud fluxes and radiances. This scale has been observed as a change in the spatial spectrum of Landsat cloud radiances, and was also recently found with the Goddard micropulse lidar, by searching for returns from directions nonparallel to the incident beam. 'Offbeam' Lidar returns are now being used to estimate the cloud 'radiative Green's function' (G). G depends on cloud thickness and may be used to retrieve that important quantity. G is also being applied to improving simple estimates of cloud radiative properties that are based on the 'Independent Pixel Approximation' or IPA. This and other measurements of 3D (three dimensional) transfer in clouds, coupled with Monte Carlo and other 3D transfer methods, are beginning to provide a better understanding of the dependence of radiation on cloud inhomogeneity, and to suggest new retrieval and parameterization algorithms which take account of cloud inhomogeneity. An international 'Intercomparison of 3D Radiation Codes' (I3RC) program is underway to coordinate and evaluate the variety of 3D radiative transfer methods now available, and to make them more widely available. Information is on the Web at: http://climate.gsfc.nasa.gov/I3RC. Input consists of selected cloud fields derived from data sources such as radar, microwave and satellite, and from models involved in the GEWEX Cloud Systems Studies. Output is selected radiative quantities that characterize the large-scale properties of the fields of radiative fluxes and heating. Several example cloud fields will be used to illustrate the effects of cloud inhomogeneity and 3D radiation.

Cahalan, Robert F.↗

The response of the Amazon ecosystem to the photosynthetically active radiation fields: integrating impacts of biomass burning aerosol and clouds in the NASA GEOS Earth system model

The Amazon experiences fires every year, and the resulting biomass burning aerosols, together with cloud particles, influence the penetration of sunlight through the atmosphere, increasing the ratio of diffuse to direct photosynthetically active radiation (PAR) reaching the vegetation canopy and thereby potentially increasing ecosystem productivity. In this study, we use the NASA Goddard Earth Observing System (GEOS) model with coupled aerosol, cloud, radiation, and ecosystem modules to investigate the impact of Amazon biomass burning aerosols on ecosystem productivity, as well as the role of the Amazon's clouds in tempering this impact. The study focuses on a 7-year period (2010–2016) during which the Amazon experienced a variety of dynamic environments (e.g., La Niña, normal years, and El Niño). The direct radiative impact of biomass burning aerosols on ecosystem productivity – called here the aerosol diffuse radiation fertilization effect – is found to increase Amazonian gross primary production (GPP) by 2.6 % via a 3.8 % increase in diffuse PAR (DFPAR) despite a 5.4 % decrease in direct PAR (DRPAR) on multiyear average during burning seasons. On a monthly basis, this increase in GPP can be as large as 9.9 % (occurring in August 2010). Consequently, the net primary production (NPP) in the Amazon is increased by 1.5 %, or ~92 Tg C yr -1 – equivalent to ~37 % of the average carbon lost due to Amazon fires over the 7 years considered. Clouds, however, strongly regulate the effectiveness of the aerosol diffuse radiation fertilization effect. The efficiency of this fertilization effect is the highest in cloud-free conditions and linearly decreases with increasing cloud amount until the cloud fraction reaches ~0.8, at which point the aerosol-influenced light changes from being a stimulator to an inhibitor of plant growth. Nevertheless, interannual changes in the overall strength of the aerosol diffuse radiation fertilization effect are primarily controlled by the large interannual changes in biomass burning aerosols rather than by changes in cloudiness during the studied period.

54 ENVIRONMENTAL SCIENCES↗

The Response of the Amazon Ecosystem to the Photosynthetically Active Radiation Fields: Integrating Impacts of Biomass Burning Aerosol and Clouds in the NASA GEOS Earth System Model

The Amazon experiences fires every year, and the resulting biomass burning aerosols, together with cloud particles, influence the penetration of sunlight through the atmosphere, increasing the ratio of diffuse to direct photosynthetically active radiation (PAR) reaching the vegetation canopy and thereby potentially increasing ecosystem productivity. In this study, we use the NASA Goddard Earth Observing System (GEOS) model with coupled aerosol, cloud, radiation, and ecosystem modules to investigate the impact of Amazon biomass burning aerosols on ecosystem productivity, as well as the role of the Amazon’s clouds in tempering this impact. The study focuses on a seven-year period (2010-2016) during which the Amazon experienced a variety of dynamic environments (e.g., La Niña, normal years, and El Niño). The direct radiative impact of biomass burning aerosols on ecosystem productivity—called here the aerosol diffuse radiation fertilization effect —is found to increase Amazonian Gross Primary Production (GPP) by 2.6% via a 3.8% increase in diffuse PAR (DFPAR) despite a 5.4% decrease in direct PAR (DRPAR) on multiyear average during burning seasons. On a monthly basis, this increase in GPP can be as large as 9.9% (occurring in August 2010). Consequently, the net primary production (NPP) in Amazon is increased by 1.5%, or ~92 Tg C a-1– equivalent to ~37% of the average carbon lost due to Amazon fires over the seven years considered. Clouds, however, strongly regulate the effectiveness of the aerosol diffuse radiation fertilization effect. The efficiency of this fertilization effect is the highest in cloud-free conditions and linearly decreases with increasing cloud amount until the cloud fraction reaches ~0.8, at which point the aerosol-influenced light changes from being a stimulator to an inhibitor of plant growth. Nevertheless, interannual changes in the overall strength of the aerosol diffuse radiation fertilization effect are primarily controlled by the large interannual changes in biomass burning aerosols rather than by changes in cloudiness during the studied period.

biomass burning aerosols on ecosystem productivity↗

High Vertically Resolved Atmospheric and Surface/Cloud Parameters Retrieved with Infrared Atmospheric Sounding Interferometer (IASI)

The Joint Airborne IASI Validation Experiment (JAIVEx) was conducted during April 2007 mainly for validation of the IASI on the MetOp satellite. IASI possesses an ultra-spectral resolution of 0.25/cm and a spectral coverage from 645 to 2760/cm. Ultra-spectral resolution infrared spectral radiance obtained from near nadir observations provide atmospheric, surface, and cloud property information. An advanced retrieval algorithm with a fast radiative transfer model, including cloud effects, is used for atmospheric profile and cloud parameter retrieval. This physical inversion scheme has been developed, dealing with cloudy as well as cloud-free radiance observed with ultraspectral infrared sounders, to simultaneously retrieve surface, atmospheric thermodynamic, and cloud microphysical parameters. A fast radiative transfer model, which applies to the cloud-free and/or clouded atmosphere, is used for atmospheric profile and cloud parameter retrieval. A one-dimensional (1-d) variational multi-variable inversion solution is used to improve an iterative background state defined by an eigenvector-regression-retrieval. The solution is iterated in order to account for non-linearity in the 1-d variational solution. It is shown that relatively accurate temperature and moisture retrievals are achieved below optically thin clouds. For optically thick clouds, accurate temperature and moisture profiles down to cloud top level are obtained. For both optically thin and thick cloud situations, the cloud top height can be retrieved with relatively high accuracy (i.e., error < 1 km). Preliminary retrievals of atmospheric soundings, surface properties, and cloud optical/microphysical properties with the IASI observations are obtained and presented. These retrievals will be further inter-compared with those obtained from airborne FTS system, such as the NPOESS Airborne Sounder Testbed - Interferometer (NAST-I), dedicated dropsondes, radiosondes, and ground based Raman Lidar. The capabilities of satellite ultra-spectral sounder such as the IASI are investigated indicating a high vertical structure of atmosphere is retrieved.

Zhou, Daniel K.↗

Atmospheric, Cloud, and Surface Parameters Retrieved from Satellite Ultra-spectral Infrared Sounder Measurements

An advanced retrieval algorithm with a fast radiative transfer model, including cloud effects, is used for atmospheric profile and cloud parameter retrieval. This physical inversion scheme has been developed, dealing with cloudy as well as cloud-free radiance observed with ultraspectral infrared sounders, to simultaneously retrieve surface, atmospheric thermodynamic, and cloud microphysical parameters. A fast radiative transfer model, which applies to the clouded atmosphere, is used for atmospheric profile and cloud parameter retrieval. A one-dimensional (1-d) variational multivariable inversion solution is used to improve an iterative background state defined by an eigenvector-regression-retrieval. The solution is iterated in order to account for non-linearity in the 1-d variational solution. This retrieval algorithm is applied to the MetOp satellite Infrared Atmospheric Sounding Interferometer (IASI) launched on October 19, 2006. IASI possesses an ultra-spectral resolution of 0.25 cm(exp -1) and a spectral coverage from 645 to 2760 cm(exp -1). Preliminary retrievals of atmospheric soundings, surface properties, and cloud optical/microphysical properties with the IASI measurements are obtained and presented.

Zhou, Daniel K.↗

Current Sounding Capability From Satellite Meteorological Observation With Ultraspectral Infrared Instruments

Ultraspectral resolution infrared spectral radiance obtained from near nadir observations provide atmospheric, surface, and cloud property information. The intent of the measurement of tropospheric thermodynamic state and trace abundances is the initialization of climate models and the monitoring of air quality. The NPOESS Airborne Sounder Testbed-Interferometer (NAST-I), designed to support the development of future satellite temperature and moisture sounders, aboard high altitude aircraft has been collecting data throughout many field campaigns. An advanced retrieval algorithm developed with NAST-I is now applied to satellite data collected with the Atmospheric InfraRed Sounder (AIRS) on the Aqua satellite launched on 4 May 2002 and the Infrared Atmospheric Sounding Interferometer (IASI) on the MetOp satellite launched on October 19, 2006. These instruments possess an ultra-spectral resolution, for example, both IASI and NAST-I have ~0.25 cm-1 and a spectral coverage from 645 to 2760 cm-1. The retrieval algorithm with a fast radiative transfer model, including cloud effects, is used for atmospheric profile and cloud parameter retrieval. The physical inversion scheme has been developed, dealing with cloudy as well as cloud-free radiance observed with ultraspectral infrared sounders, to simultaneously retrieve surface, atmospheric thermodynamic, and cloud microphysical parameters. A fast radiative transfer model, which applies to the clouded atmosphere, is used for atmospheric profile and cloud parameter retrieval. A one-dimensional (1-d) variational multi-variable inversion solution is used to improve an iterative background state defined by an eigenvector-regression-retrieval. The solution is iterated in order to account for non-linearity in the 1-d variational solution. It is shown that relatively accurate temperature and moisture retrievals can be achieved below optically thin clouds. For optically thick clouds, accurate temperature and moisture profiles down to cloud top level are obtained. For both optically thin and thick cloud situations, the cloud top height can be retrieved with relatively high accuracy (i.e., error less than 1 km). Retrievals of atmospheric soundings, surface properties, and cloud microphysical properties with the AIRS and IASI observations are obtained and presented. These retrievals are further inter-compared with those obtained from airborne FTS system, such as the NPOESS Airborne Sounder Testbed? Interferometer (NAST I), dedicated dropsondes, radiosondes, and ground based Raman Lidar. The capabilities of satellite ultra-spectral sounder such as the AIRS and IASI are investigated. These advanced satellite ultraspectral infrared instruments are now playing an important role in satellite meteorological observation for numerical weather prediction.

Zhou, Daniel K.↗

Global Atmospheric Aerosol Modeling

Global aerosol models are used to study the distribution and properties of atmospheric aerosol particles as well as their effects on clouds, atmospheric chemistry, radiation, and climate. The present article provides an overview of the basic concepts of global atmospheric aerosol modeling and shows some examples from a global aerosol simulation. Particular emphasis is placed on the simulation of aerosol particles and their effects within global climate models.

Hendricks, Johannes↗

Aircraft-Measured Indirect Cloud Effects from Biomass Burning Smoke in the Arctic and Subarctic

The incidence of wildfires in the Arctic and subarctic is increasing; in boreal North America, for example, the burned area is expected to increase by 200-300 over the next 50-100 years, which previous studies suggest could have a large effect on cloud microphysics, lifetime, albedo, and precipitation. However, the interactions between smoke particles and clouds remain poorly quantified due to confounding meteorological influences and remote sensing limitations. Here, we use data from several aircraft campaigns in the Arctic and subarctic to explore cloud microphysics in liquid-phase clouds influenced by biomass burning. Median cloud droplet radii in smoky clouds were 50 smaller than in background clouds. Based on the relationship between cloud droplet number (N(liq))/ and various biomass burning tracers (BBt/ across the multi-campaign dataset, we calculated the magnitude of subarctic and Arctic smoke aerosol-cloud interactions (ACI, where ACI = (1/3) x dln(N(liq))/dln(BBt)) to be 0.12 out of a maximum possible value of 0.33 that would be obtained if all aerosols were to nucleate cloud droplets. Interestingly, in a separate subarctic case study with low liquid water content (0.02 gm/ cu m) and very high aerosol concentrations (2000-3000 cu m) in the most polluted clouds, the estimated ACI value was only 0.06. In this case, competition for water vapor by the high concentration of CCN strongly limited the formation of droplets and reduced the cloud albedo effect, which highlights the importance of cloud feedbacks across scales. Using our calculated ACI values, we estimate that the smoke-driven cloud albedo effect may decrease shortwave radiative flux by 2 and 4 W/sq or more under some low and homogeneous cloud cover conditions in the subarctic, although the changes should be smaller in high surface albedo regions of the Arctic. We lastly show evidence to suggest that numerous northern latitude background Aitken particles can interact with combustion particles, perhaps impacting their properties as cloud condensation and ice nuclei. However, the influence of background particles on smoke-driven indirect effects is currently unclear.

Arctic↗

Multi-spectral window radiance observations of Cirrus from satellite and aircraft, November 2, 1986 Project FIRE

High resolution infrared radiance spectra achieved from the NASA ER2 airborne HIS experiment are used to analyze the spectral emissivity properties of cirrus clouds within the 8 to 12 micron atmospheric window region. Observations show that the cirrus emissivity generally decreases with increasing wavenumber (i.e., decreasing wavelength) within this band. A very abrupt decrease in emissivity (increase in brightness temperature) exists between 930/cm (10.8 microns) and 1000/cm (10.0 microns), the magnitude of the change being associated with the cirrus optical thickness as observed by lidar. The HIS observations are consistent with theoretical calculations of the spectral absorption coefficient for ice. The HIS observations imply that cirrus clouds can be detected unambiguously from the difference in brightness temperatures observed within the 8.2 and 11.0 micron window regions of the HIRS sounding radiometer flying on the operational NOAA satellites. This ability is demonstrated using simultaneous 25 km resolution HIRS observations and 1 km resolution AVHRR imagery achieved from the NOAA-9 satellite. Finally, the cirrus cloud location estimates combined with the 6.7 micron channel moisture imagery portray the boundaries of the ice/vapor phase of the upper troposphere moisture. This phase distinction is crucial for infrared radiative transfer considerations for weather and climate models, since upper tropospheric water vapor has little effect on the Earth's outgoing radiation whereas cirrus clouds have a very large attenuating effect.

Smith, William L.↗

Low-Level Liquid-Bearing Clouds Contribute to Seasonal Lower Atmosphere Stability and Surface Energy Forcing over a High-Mountain Watershed Environment

Measurements of atmospheric structure and surface energy budgets distributed along a high-altitude moun tain watershed environment near Crested Butte, Colorado, from two separate, but coordinated, field campaigns, Surface Atmosphere Integrated field Laboratory (SAIL) and Study of Precipitation, the Lower Atmosphere, and Surface for Hydrometeorology (SPLASH), are analyzed. This study identifies similarities and differences in how clouds influence the radiative budget over one snow-free summer season (2022) and two snow-covered seasons (2021/22; 2022/23) for this alpine location. A relationship between lower-tropospheric stability stratification and longwave radiative flux from the presence or absence of clouds is identified. When low clouds persisted, often with signatures of supercooled liquid in win ter, the lower troposphere experienced weaker stability, while radiatively clear skies that are less likely to be influenced by liquid droplets were associated with appreciably stronger lower-tropospheric stratification. Corresponding surface turbu lent heat fluxes partitioned differently based upon the cloud–stability stratification regime derived from early morning radiosounding profiles. Combined with the differences in the radiative budget largely resulting from dramatic seasonal dif ferences in surface albedo, the lower atmosphere stratification, surface energy budget, and near-surface thermodynamics are shown to be modified by the effective longwave radiative forcing of clouds. The diurnal evolution of thermodynamics and surface energy components varied depending on the early morning stratification state. Thus, the importance of quies cent versus synoptically active large-scale meteorology is hypothesized as a critical forcing for cloud properties and associ ated surface energy budget variations. The physical relationships between clouds, radiation, and stratification can provide a useful suite of metrics for process understanding and to evaluate numerical models in such an undersampled, highly com plex terrain environment.

54 ENVIRONMENTAL SCIENCES↗

Distribution and Radiative Forcing of Tropical Thin Cirrus Clouds

To understand the radiative impact of tropical thin cirrus clouds, the frequency of occurrence and optical depths of these clouds have been derived. Thin cirrus clouds are defined here as being those that are not detected by the operational Moderate Resolution Imaging Spectroradiometer (MODIS) cloud mask, corresponding to an optical depth value of approximately 0.3 or smaller, but that are detectable in terms of the cirrus reflectance product based on the MODIS 1.375-micron channel. With such a definition, thin cirrus clouds were present in more than 40% of the pixels flagged as clear sky by the operational MODIS cloud mask algorithm. It is shown that these thin cirrus clouds are frequently observed in deep convective regions in the western Pacific. Thin cirrus optical depths were derived from the cirrus reflectance product. Regions of significant cloud fraction and large optical depths were observed in the Northern Hemisphere during the boreal spring and summer and moved southward during the boreal autumn and winter. The radiative effects of tropical thin cirrus clouds were studied on the basis of the retrieved cirrus optical depths, the atmospheric profiles derived from the Atmospheric Infrared Sounder (AIRS) observations, and a radiative transfer model in conjunction with a parameterization of ice cloud spectral optical properties. To understand how these clouds regulate the radiation field in the atmosphere, the instantaneous net fluxes at the top of the atmosphere (TOA) and at the surface were calculated. The present study shows positive and negative net forcings at the TOA and at the surface, respectively. The positive (negative) net forcing at the TOA (surface) is due to the dominance of longwave (shortwave) forcing. Both the TOA and surface forcings are in a range of 0-20 W/sq m, depending on the optical depths of thin cirrus clouds.

THIN CIRRUS CLOUDS↗

Contrasting aerosol effects on longwave cloud forcing in South East Asia and Amazon simulated with Community Atmosphere Model version 5.3

Aerosols modify cloud microphysical and radiative properties and thus impact the shortwave (SW) and longwave cloud forcing (LWCF). This study first reports the finding of contrasting aerosol effects on LWCF in South East Asia and Amazon in the Community Atmosphere Model version 5.3 (CAM5.3), which corresponds to the sum of LW indirect and semi-direct effects investigated in Ghan et al., (2012). A series of numerical experiments is conducted to decompose the complex aerosol effects on LWCF. Our analysis indicates that the cooling (negative aerosol effects on LWCF) in Amazon is due mainly to the aerosol effects on warm clouds and the inhibition of vertical motion by the aerosol-induced radiative cooling. In contrast, the warming (positive aerosol effects on LWCF) in South East Asia is due mainly to the aerosol effect on homogeneous freezing, thus reducing the ice particle size and prolonging the existence of ice cloud. Our results emphasize that a comprehensive analysis of integrated aerosol effects on both warm and ice clouds is necessary for better understanding the aerosol effects on LWCF.

54 ENVIRONMENTAL SCIENCES↗

Large contribution of organics to condensational growth and formation of cloud condensation nuclei (CCN) in the remote marine boundary layer

Marine low clouds strongly influence global climate, and their radiative effects are particularly susceptible to the concentration of cloud condensation nuclei (CCN). One major source of CCN is the condensational growth of pre-CCN particles, and sulfate has long been considered the major condensing species in the remote marine boundary layer. While some studies have suggested that secondary organic species can contribute to particle growth, its importance remains unclear. Here we present the first long-term observational evidence that organics play an important role in particle growth over remote oceans. To the contrary of traditional thinking, sulfate dominated condensational growth for only a small (~18 %) fraction of the 62 observed growth events, even fewer than the organic-dominated events (24 %). During most (58 %) growth events, the major condensing species included both organics and sulfate. Potential precursors of the secondary organics are volatile organic compounds from ocean biological activities and those produced by the air–sea interfacial oxidation. Our results indicate that the condensation of secondary organics contributes strongly to the growth of pre-CCN particles and thereby the CCN population over remote oceans.

54 ENVIRONMENTAL SCIENCES↗

Positive low cloud and dust feedbacks amplify tropical North Atlantic Multidecadal Oscillation

Abstract The Atlantic Multidecadal Oscillation (AMO) is characterized by a horseshoe pattern of sea surface temperature (SST) anomalies and has a wide range of climatic impacts. While the tropical arm of AMO is responsible for many of these impacts, it is either too weak or completely absent in many climate model simulations. Here we show, using both observational and model evidence, that the radiative effect of positive low cloud and dust feedbacks is strong enough to generate the tropical arm of AMO, with the low cloud feedback more dominant. The feedbacks can be understood in a consistent dynamical framework: weakened tropical trade wind speed in response to a warm middle latitude SST anomaly reduces dust loading and low cloud fraction over the tropical Atlantic, which warms the tropical North Atlantic SST. Together they contribute to the appearance of the tropical arm of AMO. Most current climate models miss both the critical wind speed response and two positive feedbacks though realistic simulations of them may be essential for many climatic studies related to the AMO.

58 GEOSCIENCES↗

Evaluation of four ground-based retrievals of cloud droplet number concentration in marine stratocumulus with aircraft in situ measurements

Abstract. Cloud droplet number concentration (Nd) is crucial for understanding aerosol–cloud interactions (ACI) and associated radiative effects. We present evaluations of four ground-based Nd retrievals based on comprehensive datasets from the Atmospheric Radiation Measurement (ARM) Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign. The Nd retrieval methods use ARM ENA observatory ground-based remote sensing observations from a micropulse lidar, Raman lidar, cloud radar, and the ARM NDROP (Droplet Number Concentration) value-added product (VAP), all of which also retrieve cloud effective radius (re). The retrievals are compared against aircraft measurements from the fast cloud droplet probe (FCDP) and the cloud and aerosol spectrometer (CAS) obtained from low-level marine boundary layer clouds on 12 flight days during summer and winter seasons. Additionally, the in situ measurements are used to validate the assumptions and characterizations used in the retrieval algorithms. Statistical comparisons of the probability distribution function (PDF) of the Nd and cloud re retrievals with aircraft measurements demonstrate that these retrievals align well with in situ measurements for overcast clouds, but they may substantially differ for broken clouds or clouds with low liquid water path (LWP). The retrievals are applied to 4 years of ground-based remote sensing measurements of overcast marine boundary layer clouds at the ARM ENA observatory to find that Nd (re) values exhibit seasonal variations, with higher (lower) values during the summer season and lower (higher) values during the winter season. The ensemble of various retrievals using different measurements and retrieval algorithms such as those in this paper can help to quantify Nd retrieval uncertainties and identify reliable Nd retrieval scenarios. Of the retrieval methods, we recommend using the micropulse lidar-based method. This method has good agreement with in situ measurements, less sensitivity to issues arising from precipitation and low cloud LWP and/or optical depth, and broad applicability by functioning for both daytime and nighttime conditions.

54 ENVIRONMENTAL SCIENCES↗

Mechanism of SOA formation determines magnitude of radiative effects

Secondary organic aerosol (SOA) nearly always exists as an internal mixture and the distribution of this mixture depends on the formation mechanism of SOA. A model is developed to examine the influence of using an internal mixing states based on the mechanism of formation and to estimate the radiative forcing of SOA in the future. For the present day, 66 % of SOA is internally mixed with sulfate, while 34 % is internally mixed with primary soot. When compared with using an external mixture, the direct effect of SOA is decreased, due to the decrease of total aerosol surface area and the increase of absorption efficiency. Aerosol number concentrations are sharply reduced and this is responsible for a large decrease in the cloud albedo effect. In total, internal mixing suppresses the radiative effect of SOA by a factor of >4 compared to treating SOA as an external mixture. The future SOA burden increases by 24% due to CO2 increases and climate change, leading to a total (direct plus cloud albedo) radiative forcing of -0.05 W m-2. When the combined effects of changes in climate, anthropogenic emissions and land use are included, the SOA forcing is -0.07 W m-2, even though the SOA burden only increases by 6.8%. This is caused by the substantial increase of SOA associated with sulfate in the Aitken mode. The Aitken mode increase contributes to the enhancement of first indirect radiative forcing, which dominates the total radiative forcing.

54 ENVIRONMENTAL SCIENCES↗

Radiative Effects of African Dust and Smoke Observed from CERES and CALIOP Data

Cloud and aerosol effects have a significant impact on the atmospheric radiation budget in the Tropical Atlantic because of the spatial and temporal extent of desert dust and smoke from biomass burning in the atmosphere. The influences of African dust and smoke aerosols on cloud radiative properties over the Tropical Atlantic Ocean were analyzed for the month of July for three years (2006-2008) using collocated data collected by the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) and Clouds and the Earth s Radiant Energy System (CERES) instruments on the CALIPSO and Aqua satellites. Aerosol layer height and type can be more accurately determined using CALIOP data, through parameters such as cloud and aerosol layer height, optical depth and depolarization ratio, than data from atmospheric imagers used in previous cloud-aerosol interaction studies. On average, clouds below 5 km had a daytime instantaneous shortwave (SW) radiative flux of 270.2 +/- 16.9 W/sq m and thin cirrus clouds had a SW radiative flux of 208.0 +/- 12.7 W/sq m. When dust aerosols interacted with clouds below 5 km, as determined from CALIPSO, the SW radiative flux decreased to 205.4 +/- 13.0 W/sq m. Similarly, smoke aerosols decreased the SW radiative flux of low clouds to a value of 240.0 +/- 16.6 W/sq m. These decreases in SW radiative flux were likely attributed to the aerosol layer height and changes in cloud microphysics. CALIOP lidar observations, which more accurately identify aerosol layer height than passive instruments, appear essential for better understanding of cloud-aerosol interactions, a major uncertainty in predicting the climate system.

Yorks, John E.↗