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At least 199 records · Page 11

Dust-planetary boundary layer interactions amplified by entrainment and advections

Mineral dust contributes to more than half of the global aerosol loading. However, the radiative impacts of dust aerosols on planetary boundary layer (PBL) structure have not been explored sufficiently. During a typical dust storm event over Tarim Basin, dust aerosols exhibit a well-mixed distribution during the daytime in spite of a shallow layer of dust particles accumulated at higher altitudes. By contrast, nocturnal dust plumes are located near the surface due to stable stratification. We demonstrate that these differentiated vertical distributions determine the spatial heterogeneity of dust loading, radiative fluxes and PBL height variations. Dust aerosols cause daytime PBL suppression and nighttime PBL promotion through modulating surface and atmospheric radiative budgets. Specifically, dust-induced cooling effect within PBL directly inhibits the daytime PBL development. PBL suppression effect is then amplified by entrainment processes resulting in excessively low PBL height, especially for dust particles below but near the PBL top. Dust plumes weaken updrafts from PBL and downdrafts of the free atmosphere, which further reduce the entrainment mixing through attenuating horizontal and vertical advection, and eventually amplify PBL suppression. At night, near-surface dust aerosols stimulate a warm and unstable lower atmosphere, generate warm advection heating and promote the PBL development. Our study highlights the importance of specifying entrainment parameters and nighttime advection activities in quantifying the dust-PBL interactions.

54 ENVIRONMENTAL SCIENCES↗

A Satellite-Based Estimate of Combustion Aerosol Cloud Microphysical Effects over the Arctic Ocean

Climate predictions for the rapidly changing Arctic are highly uncertain, largely due to a poor understanding of the processes driving cloud properties. In particular, cloud fraction (CF) and cloud phase (CP) have major impacts on energy budgets, but are poorly represented in most models, often because of uncertainties in aerosol–cloud interactions. Here, we use over 10 million satellite observations coupled with aerosol transport model simulations to quantify large scale microphysical effects of aerosols on CF and CP over the Arctic Ocean during polar night, when direct and semi-direct aerosol effects are minimal. Combustion aerosols over sea ice are associated with very large (~10W/sq.m) differences in longwave cloud radiative effects at the sea ice surface. However, co-varying meteorological changes on factors such as CF likely explain the majority of this signal. For example, combustion aerosols explain at most 40% of the CF differences between the full dataset and the clean-condition subset, compared to between 57% and 91% of the differences that can be predicted by co-varying meteorology. After normalizing for meteorological regime, aerosol microphysical effects have small but significant impacts on CF, CP, and precipitation frequency on an Arctic-wide scale. These effects indicate that dominant aerosol–cloud microphysical mechanisms are related to the relative fraction of liquid-containing clouds, with implications for a warming Arctic.

Zamora, Lauren M.↗

Validating and Improving Long-Term Aerosol Data Records from SeaWiFS

Natural and anthropogenic aerosols influence the radiative balance of the Earth through direct and indirect interactions with incoming solar radiation. However, the quantification of these interactions and their ultimate effect on the Earth's climate still have large uncertainties. This is partly due to the limitations of current satellite data records which include short satellite lifetimes, retrieval algorithm uncertainty, or insufficient calibration accuracy. We have taken the first steps in overcoming this hurdle with the production and public release of an aerosol data record using the radiances from the Sea-viewing Wide Field-of-View Sensor (Sea WiFS). Sea WiFS was launched in late 1997 and provided exceptionally well-calibrated top-of-atmosphere radiance data until December 2010, more than 13 years. We have partnered this data with an expanded Deep Blue aerosol retrieval algorithm. In accordance with Deep Blue's original focus, the latest algorithm retrieves aerosol properties not only over bright desert surfaces, but also over oceans and vegetated surfaces. With this combination of a long time series and global algorithm, we can finally identify the changing patterns of regional aerosol loading and provide insight into longterm variability and trends of aerosols on regional and global scales. In this work, we provide an introduction to Sea WiFS, the current algorithms, and our aerosol data records. We have validated the data over land and ocean with ground measurements from the Aerosol Robotic Network (AERONET) and compared them with other satellites such as MODIS and MISR. Looking ahead to the next data release, we will also provide details on the implemented and planned algorithm improvements, and subsequent validation results.

Bettenhausen, Corey↗

Aerosol Radiative Effects on Deep Convective Clouds and Associated Radiative Forcing

The aerosol radiative effects (ARE) on the deep convective clouds are investigated by using a spectral-bin cloud-resolving model (CRM) coupled with a radiation scheme and an explicit land surface model. The sensitivity of cloud properties and the associated radiative forcing to aerosol single-scattering albedo (SSA) are examined. The ARE on cloud properties is pronounced for mid-visible SSA of 0.85. Relative to the case excluding the ARE, cloud fraction and optical depth decrease by about 18% and 20%, respectively. Cloud droplet and ice particle number concentrations, liquid water path (LWP), ice water path (IWP), and droplet size decrease significantly when the ARE is introduced. The ARE causes a surface cooling of about 0.35 K and significantly high heating rates in the lower troposphere (about 0.6K/day higher at 2 km), both of which lead to a more stable atmosphere and hence weaker convection. The weaker convection and the more desiccation of cloud layers explain the less cloudiness, lower cloud optical depth, LWP and IWP, smaller droplet size, and less precipitation. The daytime-mean direct forcing induced by black carbon is about 2.2 W/sq m at the top of atmosphere (TOA) and -17.4 W/sq m at the surface for SSA of 0.85. The semi-direct forcing is positive, about 10 and 11.2 W/sq m at the TOA and surface, respectively. Both the TOA and surface total radiative forcing values are strongly negative for the deep convective clouds, attributed mostly to aerosol indirect forcing. Aerosol direct and semi-direct effects are very sensitive to SSA. Because the positive semi-direct forcing compensates the negative direct forcing at the surface, the surface temperature and heat fluxes decrease less significantly with the increase of aerosol absorption (decreasing SSA). The cloud fraction, optical depth, convective strength, and precipitation decrease with the increase of absorption, resulting from a more stable and dryer atmosphere due to enhanced surface cooling and atmospheric heating.

Fan, J.↗

3D Radiative Transfer Effects in Multi-Angle/Multi-Spectral Radio-Polarimetric Signals from a Mixture of Clouds and Aerosols Viewed by a Non-Imaging Sensor

When observing a spatially complex mix of aerosols and clouds in a single relatively large field-of-view, nature entangles their signals non-linearly through polarized radiation transport processes that unfold in the 3D position and direction spaces. In contrast, any practical forward model in a retrieval algorithm will use only 1D vector radiative transfer (vRT) in a linear mixing technique. We assess the difference between the observed and predicted signals using synthetic data from a high-fidelity 3D vRT model with clouds generated using a Large Eddy Simulation model and an aerosol climatology. We find that this difference is signal--not noise--for the Aerosol Polarimetry Sensor (APS), an instrument developed by NASA. Moreover, the worst case scenario is also the most interesting case, namely, when the aerosol burden is large, hence hase the most impact on the cloud microphysics and dynamics. Based on our findings, we formulate a mitigation strategy for these unresolved cloud adjacency effects assuming that some spatial information is available about the structure of the clouds at higher resolution from "context" cameras, as was planned for NASA's ill-fated Glory mission that was to carry the APS but failed to reach orbit. Application to POLDER (POLarization and Directionality of Earth Reflectances) data from the period when PARASOL (Polarization and Anisotropy of Reflectances for Atmospheric Sciences coupled with Observations from a Lidar) was in the A-train is briefly discussed.

APS↗

Baselining the Indirect Effect by Improving Quantification of Sea Spray and Marine Sources at Ascension Island (Final Report)

Oceans cover two-thirds of the Earth and understanding the interactions of aerosols with clouds in these large marine regions requires quantifying the man-made contributions to the budget of cloud-drop forming particles (known as cloud condensation nuclei, or CCN) relative to the non-manmade “baseline” conditions and understanding the meteorology of boundary layer clouds. Modeling studies have shown substantial uncertainties and sensitivities to natural marine CCN sources, meaning that to reduce uncertainties in indirect effects we must be able to better quantify the CCN budget in ocean regions. While models provide important constraints on these uncertainties, actually reducing uncertainties requires substantial observations in open-ocean and coastal regions in order to establish the baseline on which manmade emissions are added. The tropical South Atlantic Ocean is one of the least-sampled regions of the planet, making the comprehensive measurements of the Department of Energy Atmospheric Radiation Measurement Layered Atlantic Smoke Interactions with Clouds (LASIC) campaign provides the longest record of aerosol size distribution measurements from a differential mobility analyzer in a cloud-influenced marine location in the ARM database, with 17 months of ground-based aerosol size distribution measurements. This project addressed the research topic of Aerosol-Cloud Interactions (ACI) by supporting three publications from the LASIC measurements: 1. The ARM measurements were combined with a new value-added technique that was pioneered by the Russell group for quantifying sea salt. This quantification of sea salt uses supermicron scattering measurements for retrieving reasonable sea spray mass concentrations, providing the best-available, observationally-constrained estimate of the sea spray mode properties when supermicron size distribution measurements are not available. 2. The fitted modes of the distribution were used to investigate the signatures of cloud processing for very clean to very smoky aerosol conditions, revealing not only differences in the particles that activate in clouds but also in the mechanisms that control that droplet formation process. In clean air, the size required to form a cloud droplet is influenced by the number of particles, as well as how quickly particles take up water during growth in cloud. 3. Building on this aerosol characterization, cloud and meteorological conditions were used to evaluate aerosol-related changes in cloud albedo and optical depth. We introduced a new method of decomposing the impact of aerosols on clouds known as the Twomey effect by incorporating retrieved supersaturation from two independent sets of observations to constrain the feedback of aerosol particles on cloud properties. The method quantifies the reduction of the Twomey effect at high aerosol concentrations, which has never been explained quantitatively by observations. In addition, the results provide the first direct validation for the conditions observed in the tropical South Atlantic of a parcel-based approach that is embedded in many climate models. Together these findings illustrate how ARM extended field campaigns in stratocumulus-covered regions can be used to constrain ACI processes with direct observations, providing specific radiative effects without models. By making such process-specific constraints available to improve ACI in global climate models, ARM observations play a key role in supporting model development.

58 GEOSCIENCES↗

Sensitivity of Mesoscale Modeling of Smoke Direct Radiative Effect to the Emission Inventory: a Case Study in Northern Sub-Saharan African Region

An ensemble approach is used to examine the sensitivity of smoke loading and smoke direct radiative effect in the atmosphere to uncertainties in smoke emission estimates. Seven different fire emission inventories are applied independently to WRF-Chem model (v3.5) with the same model configuration (excluding dust and other emission sources) over the northern sub-Saharan African (NSSA) biomass-burning region. Results for November and February 2010 are analyzed, respectively representing the start and end of the biomass burning season in the study region. For February 2010, estimates of total smoke emission vary by a factor of 12, but only differences by factors of 7 or less are found in the simulated regional (15degW-42degE, 13degS-17degN) and monthly averages of column PM(sub 2.5) loading, surface PM(sub 2.5) concentration, aerosol optical depth (AOD), smoke radiative forcing at the top-of-atmosphere and at the surface, and air temperature at 2 m and at 700 hPa. The smaller differences in these simulated variables may reflect the atmospheric diffusion and deposition effects to dampen the large difference in smoke emissions that are highly concentrated in areas much smaller than the regional domain of the study. Indeed, at the local scale, large differences (up to a factor of 33) persist in simulated smoke-related variables and radiative effects including semi-direct effect. Similar results are also found for November 2010, despite differences in meteorology and fire activity. Hence, biomass burning emission uncertainties have a large influence on the reliability of model simulations of atmospheric aerosol loading, transport, and radiative impacts, and this influence is largest at local and hourly-to-daily scales. Accurate quantification of smoke effects on regional climate and air quality requires further reduction of emission uncertainties, particularly for regions of high fire concentrations such as NSSA.

Sahel and sub-Saharan African region↗

Anomalies in the South American Monsoon Induced by Aerosols

We have investigated the direct effects of aerosols on the water cycle of the South American monsoon using the NASA finite-volume general circulation model (fvGCM). Global aerosol forcings are computed from radiative transfer functions derived from global distributions of five species of aerosols, i.e., dust, black carbon, organic carbon, sulphate and sea salt from the Goddard Chemistry Aerosol Radiation Transport (GOCART) model. Comparing fvGCM experiments without aerosol forcing, and with different combinations of aerosol forcing, we evaluate the impacts of aerosol direct heating on the onset, maintenance and evolution of the South American summer monsoon. We find that during the pre-monsoon season (September-October-November) Saharan dust contribute to heating of the atmosphere over the central and eastern equatorial Atlantic/Africa region through the elevated heat pump mechanism. The heating generates an anomalous Walker circulation with sinking motion, and low level northeasterlies over the Caribbean and northwestern South America. The low level flow is blocked by the Andes, and turn south and southeastward, increasing the low level jet (LLJ) along the eastern slope of the Andes. The increased LLJ transports more moisture from the Atlantic and the Amazon, enhancing the moisture convergence over subtropical land regions of South America. The moisture convergence was further accelerated by atmospheric heating by biomass burning over the Amazon. The net results of the dust and biomass heating are: a) an advance of the monsoon rainy season, b) an enhanced LLJ and c) a shifting the South America monsoon land precipitation equatorward, with increased rain over southern Brazil and reduced rain over the La Plata basin. ramifications of this elevated heating heat pump mechanism in aerosol monsoon water cycle on climate variability and change will be discussed. The ramifications of this "elevated heating heat pump" mechanism in aerosol monsoom water cycle on climate variability and change will be discussed.

Lau, K. M. William↗

Effect of Smoke on Cloud Formation during the Biomass Burning Season over the Amazon Basin

Aerosol absorption of sunlight reduces surface irradiation and heats the aerosol layer. The consequent changes in the temperature and humidity profiles can affect cloud formation extent and life time, which is called the semi-direct effect. We evaluate this aerosol semi-direct effect using data collected during the 2002 biomass burning season over the Amazon basin from the MODIS instrument on the Aqua satellite. MODIS measures the cloud coverage and the aerosol optical thickness among the clouds. We found that the radiative heating of the atmosphere and cooling of the surface due to the presence of the smoke decreases the cloud coverage. A very clear negative correlation emerges between the cloud fraction and the smoke optical depth. The results are compared to calculations using 1-D radiation model (M.D. Chou), and used to calculate this regional semi direct effect on climate forcing.

Koren, I.↗

The Roscoe Lidar: Initial Results from the Upward and Downward Looking Airborne Lidar from the ACCLIP and SABRE Campaigns

Backscatter lidars are a staple of airborne remote sensing and are primarily used in determining the altitude, vertical structure, and optical properties of clouds and aerosols. These airborne lidars typically observe in a downward direction which is sufficient for most tropospheric objectives. With more scientific attention being directed to upper tropospheric/lower stratospheric (UTLS) aerosols and recent volcanic and phrocumulonimbus events in the news, developing lidar instruments that can observe the UTLS will be vital in better understanding their composition and optical properties and determining their role in the planet's radiative balance. To meet this need, the downward and upward looking Roscoe lidar was developed and flown on two recent field campaigns: Stratospheric Aerosol processes, Budget, and Radiative Effects (SABRE) and Asian Summer Monsoon Chemical and CLimate Impact Project (ACCLIP) (both 2022). Building on its extensive Cloud Physics Lidar (CPL) heritage, we show that Roscoe can deliver CPL-like products in both the up and down-looking directions providing an unmatched vertical view of the atmosphere from an airborne platform. Future work can leverage Roscoe's updward looking view to quantify the optical properties and extinction of UTLS aerosols.

Kenneth Christian↗

The Shortwave Radiative Flux Response to an Injection of Sea Salt Aerosols in the Gulf of Mexico

We report marine cloud brightening (MCB) has been proposed as a potential means of geoengineering the climate, temporarily providing cooling to offset some of the effects of climate change. Marine sky brightening (MSB), involving the direct scattering of sunlight from sea salt injection into the marine boundary layer, has been proposed as an additional geoengineering method that could work in areas that are not regularly cloudy. Here, we use a regional atmospheric model to simulate MCB and MSB over the Gulf of Mexico and nearby land, a highly populated and economically important region that is not characterized by persistent marine stratocumulus cloud cover. Injection of sea salt in the Aitken mode from a region in the central Gulf of Mexico equivalent to 10.8 Tg yr -1 produces an upwards 8.4 W m -2 radiative flux change across the region at the top of the atmosphere, largely due to cloud property changes. Comparatively, a similar mass injection in the accumulation mode produces a 3.1 W m -2 radiative flux change driven primarily by direct scattering. Injection of even larger particles produces a much smaller radiative flux change. Shortwave flux changes due to clouds are largely driven by an increase in cloud droplet number concentration and an increase in cloud liquid water path (each contributing about 45% to the flux change), with a much lower contribution from cloud fraction changes (10%).

54 ENVIRONMENTAL SCIENCES↗

Integrative Analysis of Desert Dust Size and Abundance Suggests Less Dust Climate Cooling

Desert dust aerosols affect Earths global energy balance through interactions with radiation, clouds, and ecosystems. But the magnitudes of these effects are so uncertain that it remains unclear whether atmospheric dust has a net warming or cooling effect on global climate. Consequently, it is still uncertain whether large changes in atmospheric dust loading over the past century have slowed or accelerated anthropogenic climate change, and the climate impact of possible future alterations in dust loading is similarly disputed. Here we use an integrative analysis of dust aerosol sizes and abundance to constrain the climatic impact of dust through direct interactions with radiation. Using a combination of observational, experimental, and model data, we find that atmospheric dust is substantially coarser than represented in current climate models. Since coarse dust warms global climate, the dust direct radiative effect (DRE) is likely less cooling than the 0.4 W m superscript 2 estimated by models in a current ensemble. We constrain the dust DRE to -0.20 (-0.48 to +0.20) W m superscript 2, which suggests that the dust DRE produces only about half the cooling that current models estimate, and raises the possibility that dust DRE is actually net warming the planet.

Atmospheric chemistry↗

Global Radiative Flux Profile Dataset: Revised and Extended

The third generation of the radiative flux profile data product, called ISCCP-FH, is described. The revisions over the previous generation (called ISCCP-FD) include improvements in the radiative model representation of gaseous and aerosol effects, as well as a refined statistical model of cloud vertical layer variations with cloud types, and increased spatial resolution. The new product benefits from the changes in the new H-version of the ISCCP cloud products (called ISCCP-H): higher spatial resolution, revised radiance calibration and treatment of ice clouds, treatment of aerosol effects, and revision of all the ancillary atmosphere and surface property products. The ISCCP-FH product is evaluated against more direct measurements from the Clouds and the Earth’s Radiant Energy System and the Baseline Surface Radiation Network products, showing some small, overall reductions in average flux uncertainties; but the main results are similar to ISCCP-FD: the ISCCP-FH uncertainties remain ≲10 Wm −2 at the top-of-atmosphere (TOA) and ≲15 Wm −2 at surface for monthly, regional averages. The long-term variations of TOA, surface and in-atmosphere net fluxes are documented and the possible transient cloud feedback implications of a long-term change of clouds are investigated. The cloud and flux variations from 1998 to 2012 suggest a positive cloud-radiative feedback on the oceanic circulation and a negative feedback on the atmospheric circulation. This example demonstrates that the ISCCP-FH product can provide useful diagnostic information about weather-to-interannual scale variations of radiation induced by changes in cloudiness as well as atmospheric and surface properties.

ISCCP-FH↗

Elucidating Processes Controlling Arctic Atmospheric Aerosol Sources, Aging, and Mixing States (Final Report)

Atmospheric aerosols play critical roles in the Earth’s energy budget, directly by scattering or absorbing solar and terrestrial radiation and indirectly by serving as seeds (nuclei) for cloud droplet and ice crystal formation and by depositing on snow and ice surface, thereby changing the surface albedo. These effects are dependent on aerosol particle size and chemical composition and impact the hydrological cycle as well. This project provided single-particle size and chemical composition measurements across the entire annual cycle in the high Arctic and in the Alaskan Arctic during fall – winter, addressing the most significant gaps in Arctic aerosol observational data. These needs were based on recent rapid sea ice loss across the entire Arctic, as well as the major annual delays in sea ice freeze-up during fall in the Chukchi Sea and increased wintertime sea ice fracturing in the Beaufort Sea, both off the North Slope of Alaska. Two DOE Atmospheric Radiation Measurement (ARM) field campaigns were conducted for atmospheric aerosol sampling. The Aerosols during the Polar Utqiagvik Night (APUN – ‘snow on ground’ in Iñupiaq) ARM field campaign at Utqagivik, Alaska was conducted from Oct. 28 – Dec. 22, 2018. Aerosol sizing instrumentation and a single-particle mass spectrometer were successfully deployed for size-resolved number concentration measurements and measurements of individual particle size and chemical composition, respectively. These results show the influence of locally-produced sea spray aerosol, with high cloud-forming potential, due to delayed sea ice freeze-up in the fall. During the 2019‐2020 international Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition, daily atmospheric aerosol particles were collected aboard the German icebreaker Polarstern in the Central Arctic from Nov. 2019 – Oct. 2020. Sea salt aerosol and marine organics were observed year-round during MOSAiC with varying morphologies and sources. These findings are important because most Arctic models do not include a sea spray aerosol source, despite this source increasing with declining sea ice extent. In addition to collecting new samples and data, this project also conducted further analysis of previously collected single-particle chemical composition measurements within the North Slope of Alaska oil fields and at Utqiaġvik, AK, during Aug. – Sep. 2015 and 2016 field campaigns. This work resulted in the discovery of chemical reactions of oil field combustion emissions occurring within fog droplets across the North Slope of Alaska and forming secondary aerosol, showing the impact of Arctic oil field emissions beyond black carbon aerosol and greenhouse gases. In addition, the distribution of chemical species across the aerosol population within the oil fields was quantified, using these data and a previously development framework. We also presented the first ambient evidence of the collision of two atmospheric particles resulting in formation of an organic-coated ammonium sulfate particle of marine origin, which has implications for cloud formation with declining sea ice extent. Overall, this project has elucidated connections between seawater biogeochemistry, resource extraction activities, atmospheric composition, clouds, and the energy budget of the Arctic region. The results of this project are expected to improve weather and sea ice forecasting for security and development in the Arctic and beyond.

54 ENVIRONMENTAL SCIENCES↗

Radiative effects of the arctic haze

During the recent Arctic Gas and Aerosols Sampling Project flight series, the absorption of solar radiation by the Arctic haze was measured directly for the first time. Absorpton was measured in three narrow band channels, and the measurements were used to calibrate a high resolution solar flux model, which was then used to compute atmospheric heating rates. Analyses of data from three flights with estimated optical depths of 0.26, 0.17, and 0.31 at 500 nm produced instantaneous solar heating rates of the order of 1.1 to 1.5 K/day. These rates are greater by a factor of 2 to 3 than heating in the absence of the haze. Possible climatic implications are briefly discussed.

Valero, F. P. J.↗

Exploring dimethyl sulfide (DMS) oxidation and implications for global aerosol radiative forcing

Abstract. Aerosol indirect radiative forcing (IRF), which characterizes how aerosols alter cloud formation and properties, is very sensitive to the preindustrial (PI) aerosol burden. Dimethyl sulfide (DMS), emitted from the ocean, is a dominant natural precursor of non-sea-salt sulfate in the PI and pristine present-day (PD) atmospheres. Here we revisit the atmospheric oxidation chemistry of DMS, particularly under pristine conditions, and its impact on aerosol IRF. Based on previous laboratory studies, we expand the simplified DMS oxidation scheme used in the Community Atmospheric Model version 6 with chemistry (CAM6-chem) to capture the OH-addition pathway and the H-abstraction pathway and the associated isomerization branch. These additional oxidation channels of DMS produce several stable intermediate compounds, e.g., methanesulfonic acid (MSA) and hydroperoxymethyl thioformate (HPMTF), delay the formation of sulfate, and, hence, alter the spatial distribution of sulfate aerosol and radiative impacts. The expanded scheme improves the agreement between modeled and observed concentrations of DMS, MSA, HPMTF, and sulfate over most marine regions, based on the NASA Atmospheric Tomography (ATom), the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA), and the Variability of the American Monsoon Systems (VAMOS) Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) measurements. We find that the global HPMTF burden and the burden of sulfate produced from DMS oxidation are relatively insensitive to the assumed isomerization rate, but the burden of HPMTF is very sensitive to a potential additional cloud loss. We find that global sulfate burden under PI and PD emissions increase to 412 Gg S (+29 %) and 582 Gg S (+8.8 %), respectively, compared to the standard simplified DMS oxidation scheme. The resulting annual mean global PD direct radiative effect of DMS-derived sulfate alone is −0.11 W m−2. The enhanced PI sulfate produced via the gas-phase chemistry updates alone dampens the aerosol IRF as anticipated (−2.2 W m−2 in standard versus −1.7 W m−2, with updated gas-phase chemistry). However, high clouds in the tropics and low clouds in the Southern Ocean appear particularly sensitive to the additional aqueous-phase pathways, counteracting this change (−2.3 W m−2). This study confirms the sensitivity of aerosol IRF to the PI aerosol loading and the need to better understand the processes controlling aerosol formation in the PI atmosphere and the cloud response to these changes.

54 ENVIRONMENTAL SCIENCES↗

Determination of the ground albedo and the index of absorption of atmospheric particulates by remote sensing. I - Theory

A statistical technique is developed for inferring the optimum values of the ground albedo and the effective imaginary term of the complex refractive index of atmospheric particulates. The procedure compares measurements of the ratio of the hemispheric diffuse to directly transmitted solar flux density at the earth's surface with radiative transfer computations of the same as suggested by Herman et al. (1975). A detailed study is presented which shows the extent to which the ratio of diffuse to direct solar radiation is sensitive to many of the radiative transfer parameters. Results indicate that the optical depth and size distribution of atmospheric aerosol particles are the two parameters which uniquely specify the radiation field to the point where ground albedo and index of absorption can be inferred. Varying the real part of the complex refractive index of atmospheric particulates as well as their vertical distribution is found to have a negligible effect on the diffuse-direct ratio. The statistical procedure utilizes a semi-analytic gradient search method from least-squares theory and includes a detailed error analysis.

King, M. D.↗

Radiative Effects of Aerosols

During the Atlantic Stratocumulus Transition Experiment (ASTEX) in June 1992, two descents in cloud-free regions allowed comparison of the change in aerosol optical depth as determined by an onboard total-direct-diffuse radiometer (TDDR) to the change calculated from measured size-resolved aerosol microphysics and chemistry. Both profiles included a pollution haze from Europe but the second also included the effect of a Saharan dust layer above the haze. The separate contributions of supermicrometer (coarse) and submicrometer (fine) aerosol were determined and thermal analysis of the pollution haze indicated that the fine aerosol was composed primarily of a sulfate/water mixture with a refractory soot-like core. The soot core increased the calculated extinction by about 10% in the most polluted drier layer relative to a pure sulfate aerosol but had significantly less effect at higher humidities. A 3 km descent through a boundary layer air mass dominated by pollutant aerosol with relative humidities (RH) 10-77% yielded a close agreement between the measured and calculated aerosol optical depths (550 nm) of 0.160 (+/- 0.07) and 0. 157 (+/- 0.034) respectively. During descent the aerosol mass scattering coefficient per unit sulfate mass varied from about 5 to 16 m(exp 2)/g and primarily dependent upon ambient RH. However, the total scattering coefficient per total fine mass was far less variable at about 4+/- 0.7 m(exp 2)/g. A subsequent descent through a Saharan dust layer located above the pollution aerosol layer revealed that both layers contributed similarly to aerosol optical depth. The scattering per unit mass of the coarse aged dust was estimated at 1.1 +/- 0.2 m(exp 2)/g. The large difference (50%) in measured and calculated optical depth for the dust layer exceeded measurements.

Valero, Francisco P. J.↗