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At least 613 records · Page 34
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Opinion: A critical evaluation of the evidence for aerosol invigoration of deep convection

Deep convective updraft invigoration via indirect effects of increased aerosol number concentration on cloud microphysics is frequently cited as a driver of correlations between aerosol and deep convection properties. Here, we critically evaluate the theoretical, modeling, and observational evidence for warm- and cold-phase invigoration pathways. Though warm-phase invigoration is plausible and theoretically supported via lowering of the supersaturation with increased cloud droplet concentration in polluted conditions, the significance of this effect depends on substantial supersaturation changes in real-world convective clouds that have not been observed. Much of the theoretical support for cold-phase invigoration depends on unrealistic assumptions of instantaneous freezing and unloading of condensate in growing, isolated updrafts. When applying more realistic assumptions, impacts on buoyancy from enhanced latent heating via fusion in polluted conditions are largely canceled by greater condensate loading. Many foundational observational studies supporting invigoration have several fundamental methodological flaws that render their findings incorrect or highly questionable. Thus, much of the evidence for invigoration has come from numerical modeling, but different models and setups have produced a vast range of results. Furthermore, modeled aerosol impacts on deep convection are rarely tested for robustness, and microphysical biases relative to observations persist, rendering many results unreliable for application to the real world. Without clear theoretical, modeling, or observational support, and given that enervation rather than invigoration may occur for some deep convective regimes and environments, it is entirely possible that the overall impact of cold-phase invigoration is negligible. Substantial mesoscale variability of dominant thermodynamic controls on convective updraft strength coupled with substantial updraft and aerosol variability in any given event are poorly quantified by observations and present further challenges to isolating aerosol effects. Observational isolation and quantification of convective invigoration by aerosols is also complicated by limitations of available cloud condensation nuclei and updraft speed proxies, aerosol correlations with meteorological conditions, and cloud impacts on aerosols. Furthermore, many cloud processes, such as entrainment and condensate fallout, modulate updraft strength and aerosol–cloud interactions, varying with cloud life cycle and organization, but these processes remain poorly characterized. Considering these challenges, recommendations for future observational and modeling research related to aerosol invigoration of deep convection are provided.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Chemical properties and single-particle mixing state of soot aerosol in Houston during the TRACER campaign

Abstract. A high-resolution soot particle aerosol mass spectrometer (SP-AMS) was used to selectively measure refractory black carbon (rBC) and its associated coating material using both the ensemble size-resolved mass spectral mode and the event trigger single particle (ETSP) mode in Houston, Texas, in summer 2022. This study was conducted as part of the Department of Energy Atmospheric Radiation Measurement (ARM) program's TRacking Aerosol Convection interactions ExpeRiment (TRACER) field campaign. The study revealed an average (±1σ) rBC concentration of 103 ± 176 ng m−3. Additionally, the coatings on the BC particles were primarily composed of organics (59 %; 219 ± 260 ng m−3) and sulfate (26 %; 94 ± 55 ng m−3). Positive matrix factorization (PMF) analysis of the ensemble mass spectra of BC-containing particles resolved four distinct types of soot aerosol, including an oxidized organic aerosol (OOABC,PMF) factor associated with processed primary organic aerosol, an inorganic sulfate factor (SO4,BC,PMF), an oxidized rBC factor (O-BCPMF), and a mixed mineral dust–biomass burning aerosol factor with significant contribution from potassium (K-BBBC,PMF). Additionally, K-means clustering analysis of the single-particle mass spectra identified eight different clusters, including soot particles enriched in hydrocarbon-like organic aerosol (HOABC,ETSP), sulfate (SO4,BC,ETSP), two types of rBC, OOA (OOABC,ETSP), chloride (ClBC,ETSP), and nitrate (NO3,BC,ETSP). The single-particle measurements demonstrate substantial variation in BC coating thickness with coating-to-rBC mass ratios ranging from 0.1 to 100. The mixing state index (χ), which denotes the degree of homogeneity of the soot aerosol, varied from 4 % to 94 % with a median of 40 %, indicating that the aerosol population lies in between internal and external mixing but has large temporal and source type variability. In addition, a significant fraction of BC-containing particles, a majority enriched with oxidized organics and sulfate, exhibit sufficiently high κ values and diameters conducive to activation as cloud nuclei under atmospherically relevant supersaturation conditions. This finding bears significance in comprehending the aging processes of rBC-containing particles and their activation into cloud droplets. Our analysis highlights the complex nature of soot aerosol and underscores the need to comprehend its variability across different environments for accurate assessment of climate change.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

High sensitivity of simulated fog properties to parameterized aerosol activation in case studies from ParisFog

Aerosols influence fog properties such as visibility and lifetime by affecting fog droplet number concentrations (N d ). Numerical weather prediction (NWP) models often represent aerosol–fog interactions using highly simplified approaches. Incorporating prognostic size-resolved aerosol microphysics from climate models could allow them to simulate N d and aerosol–fog interactions without incurring excessive computational expense. However, microphysics code designed for coarse spatial resolution may struggle with sub-kilometer-scale grid spacings. Here, we test the ability of the UK Met Office Unified Model to simulate aerosol and fog properties during case studies from the ParisFog field campaign in 2011. We examine the sensitivity of fog properties to variations in N d caused by modifications to simulated aerosol activation. Our model, with a 500 m horizontal resolution and interactive aerosol and cloud microphysics, significantly underpredicts N d , although it only slightly underestimates the cloud condensation nuclei concentration. With an updated version of the Abdul-Razzak and Ghan (2000) activation scheme, we produce N d that are more consistent with those predicted by a cloud parcel model under fog-like conditions. We activate droplets only by adiabatic cooling. We incorporate more realistic hygroscopicities for sulfate and organic aerosols and explore the sensitivity of simulated N d to unresolved updrafts. We find that both N d and simulated fog liquid water content are very sensitive to the updated activation scheme but remain less affected by the update to hygroscopicities. Our improvements offer insights into the physical processes regulating N d in stable conditions, potentially laying foundations for improved operational fog forecasts that incorporate interactive aerosol simulations or aerosol climatologies.

Ghosh, Pratapaditya [Carnegie Mellon University, P↗
DOE OSTI2025

Weak influence of anthropogenic emissions on aerosol, cloud, and rain in the wet season of the Amazon rainforest

Anthropogenic emissions have been shown to affect new particle formation, aerosol concentrations, and clouds. Such effects vary with region, environmental conditions, and cloud types. In the wet season of Amazonia, anthropogenic emissions emitted from Manaus, Brazil, can significantly increase the cloud condensation nuclei (CCN) concentrations compared to the background of mainly natural aerosols. However, the regional response of cloud and rain to anthropogenic emissions in Amazonia remains very uncertain. Here, we aim to quantify how aerosol concentration, cloud, and rain respond to changes in anthropogenic emissions through parameterized new particle formation and primary aerosol emission in the Manaus region and to understand the underlying mechanisms. We ran the atmosphere-only configuration of the HadGEM3 climate model with a nested regional domain that covers most of the rainforest region (720 km by 1200 km with 3 km resolution) under scaled regional emissions. The 7 d simulations show that, in the areas that are affected by anthropogenic emissions, when aerosol and precursor gas emissions are doubled from the baseline emission inventories, aerosol number concentrations increase by 13 %. The nucleation rate that involves sulfuric acid and biogenic compounds generally increases with pollution levels. However, nucleation is suppressed very close to the pollution source, resulting in lower nucleation and soluble Aitken mode aerosol number concentrations. We also found that doubling the anthropogenic emission can increase the cloud droplet number concentrations ( N d ) by 9 %, but cloud water and rain mass mixing ratios do not change significantly. Even very strong reductions in aerosol number concentrations by a factor of 4, which is an unrealistic condition, cause only a 4 % increase in rain over the domain. If we assume our simulation has a fine enough grid resolution and an accurate representation of the relevant atmospheric processes, the simulated weak and non-linear response of cloud and rain properties to linearly scaled anthropogenic emissions suggests that the interactions among aerosol, cloud, and precipitation in the Amazonian convective environment are buffered by microphysical processes. It also implies that the convective environment is resilient to the changes in Nd that occur in response to localized anthropogenic aerosol perturbations.

Wang, Xuemei [University of Leeds (United Kingdom)↗
DOE OSTI2021

Rapid measurement of RH-dependent aerosol hygroscopic growth using a humidity-controlled fast integrated mobility spectrometer (HFIMS)

Abstract. The ability of aerosol particles to uptake water (hygroscopic growth) is an important determinant of aerosol optical properties and radiative effects. Aerosol hygroscopic growth is traditionally measured by humidified tandem differential mobility analyzers (HTDMA), in which size-selected dry particles are exposed to elevated relative humidity (RH), and the size distribution of humidified particles is subsequently measured using a scanning mobility particle sizer. As a scanning mobility particle sizer can measure only one particle size at a time, HTDMA measurements are time consuming, and ambient measurements are often limited to a single RH level. Pinterich et al. (2017b) showed that fast measurements of aerosol hygroscopic growth are possible using a humidity-controlled fast integrated mobility spectrometer (HFIMS). In HFIMS, the size distribution of humidified particles is rapidly captured by a water-based fast integrated mobility spectrometer (WFIMS), leading to a factor of ∼10 increase in measurement time resolution. In this study we present a prototype HFIMS that extends fast hygroscopic growth measurements to a wide range of atmospherically relevant RH values, allowing for more comprehensive characterizations of aerosol hygroscopic growth. A dual-channel humidifier consisting of two humidity conditioners in parallel is employed such that aerosol RH can be quickly stepped among different RH levels by sampling from alternating conditioners. The measurement sequence is also optimized to minimize the transition time between different particle sizes. The HFIMS is capable of measuring aerosol hygroscopic growth of six particle diameters under five RH levels ranging from 20 % to 85 % (30 separate measurements) every 25 min. The performance of this HFIMS is characterized and validated using laboratory-generated ammonium sulfate aerosol standards. Measurements of ambient aerosols are shown to demonstrate the capability of HFIMS to capture the rapid evolution of aerosol hygroscopic growth and its dependence on both size and RH.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Novel estimation of aerosol processes with particle size distribution measurements: a case study with the TOMAS algorithm v1.0.0

Atmospheric aerosol microphysical processes are a significant source of uncertainty in predicting climate change. Specifically, aerosol nucleation, emissions, and growth rates, which are simulated in chemical transport models to predict the particle size distribution, are not understood well. However, long-term size distribution measurements made at several ground-based sites across Europe implicitly contain information about the processes that created those size distributions. This work aims to extract that information by developing and applying an inverse technique to constrain aerosol emissions as well as nucleation and growth rates based on hourly size distribution measurements. We developed an inverse method based upon process control theory into an online estimation technique to scale aerosol nucleation, emissions, and growth so that the model–measurement bias in three measured aerosol properties exponentially decays. The properties, which are calculated from the measured and predicted size distributions, used to constrain aerosol nucleation, emission, and growth rates are the number of particles with a diameter between 3 and 6 nm, the number with a diameter greater than 10 nm, and the total dry volume of aerosol ( N 3–6 , N 10 , V dry ), respectively. In this paper, we focus on developing and applying the estimation methodology in a zero-dimensional “box” model as a proof of concept before applying it to a three-dimensional simulation in subsequent work. The methodology is first tested on a dataset of synthetic and perfect measurements that span diverse environments in which the true particle emissions, growth, and nucleation rates are known. The inverse technique accurately estimates the aerosol microphysical process rates with an average and maximum error of 2 % and 13 %, respectively. Next, we investigate the effect that measurement noise has on the estimated rates. The method is robust to typical instrument noise in the aerosol properties as there is a negligible increase in the bias of the estimated process rates. Finally, the methodology is applied to long-term datasets of in situ size distribution measurements in western Europe from May 2006 through June 2007. At Melpitz, Germany, and Hyytiälä, Finland, the average diurnal profiles of estimated 3 nm particle formation rates are reasonable, having peaks near noon local time with average peak values of 1 and 0.15 cm –3 s –1 , respectively. The normalized absolute error in estimated N 3–6 , N 10 , and V dry at three European measurement sites is less than 15 %, showing that the estimation framework developed here has potential to decrease model–measurement bias while constraining uncertain aerosol microphysical processes.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1989

Light scattering characteristics of various aerosol types derived from multiple wavelength lidar observations

The present study demonstrates the potential of a multiple-wavelength lidar for discriminating between several aerosol types on the basis of the wavelength dependence of the aerosol backscatter coefficient. The two-component lidar equation was solved under the assumption of similarity in the derived profiles of backscatter coefficients for each wavelength. It is shown that a three-wavelength lidar system operating at 300, 600, and 1064nm can provide unique information for discriminating between various aerosol types (continental, maritime, Saharan-dust, stratospheric aerosols in a tropopause fold event, and tropical forest aerosols). Mie calculations were made using in situ aerosol data and aerosol models to compare with the lidar results. The disagreement between the theoretical and empirical results in some cases was substantial. These differences may be partly due to uncertainties in the lidar data analysis and aerosol characteristics and also due to the conventional assumption of aerosol sphericity for the aerosol Mie calculations.

Sasano, Yasuhiro↗
NASA NTRS1991

Tropospheric ozone and aerosols measured by airborne lidar during the 1988 Arctic boundary layer experiment

Ozone (O3) and aerosol distributions were measured from an aircraft using a differential absorption lidar (DIAL) system as part of the 1988 NASA Global Tropospheric Experiment - Arctic Boundary Layer Experiment (ABLE-3A) to study the sources and sinks of gases and aerosols over the tundra regions of Alaska during the summer. The tropospheric O3 budget over the Arctic was found to be strongly influenced by stratospheric intrusions. Regions of low aerosol scattering and enhanced O3 mixing ratios were usually correlated with descending air from the upper troposphere or lower stratosphere. Several cases of continental polar air masses were examined during the experiment. The aerosol scattering associated with these air masses was very low, and the atmospheric distribution of aerosols was quite homogeneous for those air masses that had been transported over the ice for greater than or = 3 days. The transition in O3 and aerosol distributions from tundra to marine conditions was examined several times. The aerosol data clearly show an abrupt change in aerosol scattering properties within the mixed layer from lower values over the tundra to generally higher values over the water. The distinct differences in the heights of the mixed layers in the two regions was also readily apparent. Several cases of enhanced O3 were observed during ABLE-3 in conjunction with enhanced aerosol scattering in layers in the free atmosphere. Examples are presented of the large scale variations of O3 and aerosols observed with the airborne lidar system from near the surface to above the tropopause over the Arctic during ABLE-3.

Browell, Edward V.↗
NASA NTRS1995

Aerosol effects and corrections in the Halogen Occultation Experiment

The eruptions of Mt. Pinatubo in June 1991 increased stratospheric aerosol loading by a factor of 30, affecting chemistry, radiative transfer, and remote measurements of the stratosphere. The Halogen Occultation Experiment (HALOE) instrument on board Upper Atmosphere Research Satellite (UARS) makes measurements globally for inferring profiles of NO2, H2O, O3, HF, HCl, CH4, NO, and temperature in addition to aerosol extinction at five wavelengths. Understanding and removing the aerosol extinction is essential for obtaining accurate retrievals from the radiometer channels of NO2, H2O and O3 in the lower stratosphere since these measurements are severely affected by contaminant aerosol absorption. If ignored, aerosol absorption in the radiometer measurements is interpreted as additional absorption by the target gas, resulting in anomalously large mixing ratios. To correct the radiometer measurements for aerosol effects, a retrieved aerosol extinction profile is extrapolated to the radiometer wavelengths and then included as continuum attenuation. The sensitivity of the extrapolation to size distribution and composition is small for certain wavelength combinations, reducing the correction uncertainty. The aerosol corrections extend the usable range of profiles retrieved from the radiometer channels to the tropopause with results that agree well with correlative measurements. In situations of heavy aerosol loading, errors due to aerosol in the retrieved mixing ratios are reduced to values of about 15, 25, and 60% in H2O, O3, and NO2, respectively, levels that are much less than the correction magnitude.

Hervig, Mark E.↗
NASA NTRS1996

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.↗
NASA NTRS1998

LASE measurements of aerosols and water vapor during TARFOX

The TARFOX (Tropospheric Aerosol Radiative Forcing Observational Experiment) intensive field campaign was designed to reduce uncertainties in estimates of the effects of anthropogenic aerosols on climate by measuring direct radiative effects and the optical, physical, and chemical properties of aerosols [1]. TARFOX was conducted off the East Coast of the United States between July 10-31, 1996. Ground, aircraft, and satellite-based sensors measured the sensitivity of radiative fields at various atmospheric levels to aerosol optical properties (i.e., optical thickness, phase function, single-scattering albedo) and to the vertical profile of aerosols. The LASE (Lidar Atmospheric Sensing Experiment) instrument, which was flown on the NASA ER-2 aircraft, measured vertical profiles of total scattering ratio and water vapor during a series of 9 flights. These profiles were used in real-time to help direct the other aircraft to the appropriate altitudes for intensive sampling of aerosol layers. We have subsequently used the LASE aerosol data to derive aerosol backscattering and extinction profiles. Using these aerosol extinction profiles, we derived estimates of aerosol optical thickness (AOT) and compared these with measurements of AOT from both ground and airborne sun photometers and derived from the ATSR-2 (Along Track and Scanning Radiometer 2) sensor on ERS-2 (European Remote Sensing Satellite-2). We also used the water vapor mixing ratio profiles measured simultaneously by LASE to derive precipitable water vapor and compare these to ground based measurements.

Ferrare, Richard A.↗
NASA NTRS1999

Physical and Chemical Characterization of Particles in the Upper Troposphere and Lower Stratosphere: Microanalysis of Aerosol Impactor Samples

Herein is reported activities to support the characterization of the aerosol in the upper troposphere (UT) and lower stratosphere (LS) collected during the Airborne Southern Hemisphere Ozone Experiment/Measurements for Assessing the Effects of Stratospheric Aircraft (ASHOE/MAESA) missions in 1994. Through a companion proposal, another group was to measure the size distribution of aerosols in the 0.008 to 2 micrometer diameter range and to collect for us impactor samples of particles larger than about 0.02 gm. In the first year, we conducted laboratory studies related to particulate deposition patterns on our collection substrates, and have performed the analysis of many ASHOE/MAESA aerosol samples from 1994 using analytical electron microscopy (AEM). We have been building an "aerosol climatology" with these data that documents the types and relative abundances of particles observed at different latitudes and altitudes. The second year (and non-funded extension periods) saw continued analyses of impactor aerosol samples, including more ASHOE/MAESA samples, some northern hemisphere samples from the NASA Stratospheric Photochemistry Aerosols and Dynamics Expedition (SPADE) program for comparison, and a few aerosol samples from the NASA Stratospheric TRacers of Atmospheric Transport (STRAT) program. A high-resolution field emission microscope was used for the analysis and re-analysis of a number of samples to determine if this instrument was superior in performance to our conventional electron microscope. In addition, some basic laboratory studies were conducted to determine the minimum detectable and analyzable particle size for different types of aerosols. In all, 61 aerosol samples were analyzed, with a total of over 30,000 individual particle analyses. In all analyzed samples, sulfate particles comprised the major aerosol number fraction. It must be stressed that particles composed of more than one species, for example sulfate and organic carbon, were classified according to the major fraction. Thus, many of the particles classified as sulfate may have contained significant mass fractions of carbonaceous or other material. These particles for the most part did not show two physical phases, however. Nonsulfate particles were classified according to the physical and chemical characteristics of each particle, and were grouped into the major nonsulfate particle classes, including C-rich, crustal, metallic, and salts. Our UT and LS sample analyses indicate a maximum for crustal and C-rich particle abundance in the Northern Hemisphere upper troposphere, and a salt particle maximum in the Southern Hemisphere upper troposphere. Metallic particles are clearly more prevalent in the troposphere than in the stratosphere, but interhemispheric differences appear small.

Sheridan, Patrick J.↗
NASA NTRS1999

Principles in Remote Sensing of Aerosol from MODIS Over Land and Ocean

The well-calibrated spectral radiances measured by MODIS will be processed to retrieve daily aerosol properties that include optical thickness and mass loading over land and optical thickness, the mean particle size of the dominant mode and the ratio between aerosol modes over ocean. In addition, after launch, aerosol single scattering albedo will be calculated as an experimental product. The retrieval process over land is based on a dark target method that identifies appropriate targets in the mid-IR channels and uses an empirical relationship found between the mid-ER and the visible channels to estimate surface reflectance in the visible from the mid-HZ reflectance measured by satellite. The method employs new aerosol models for industrial, smoke and dust aerosol. The process for retrieving aerosol over the ocean makes use of the wide spectral band from 0.55-2.13 microns and a look-up table constructed from combinations of five accumulation modes and five coarse modes. Both the over land and over ocean algorithms have been validated with satellite and airborne radiance measurements. We estimate that MODIS will be able to measure aerosol optical thickness (t) to within 0.05 +/- 0.2t over land and to within 0.05 +/- 0.05t over ocean. Much of the earth's surface is located far from aerosol sources and experience very low aerosol optical thickness. Will the accuracy expected from MODIS retrievals be sufficient to measure the global aerosol direct and indirect forcing? We are attempting to answer this question using global model results and cloud climatology.

Remer, L. A.↗
NASA NTRS1999

Vertical Distribution of Aerosol in the Troposphere

The paper addresses the issue of the vertical distribution of aerosol in the troposphere and the relation to causative mechanisms. The focus is on visible wavelength, aerosol extinction cross sections. A background on the state of knowledge will be presented, but the emphasis is on experimental results from several field programs, The GLOBE project (GLobal aerosol Backscatter Experiment) involved a series of flights by the NASA DC-8 throughout the Pacific basin region with comprehensive in situ and multi-spectral lidar aerosol distribution measurements. The data has been extensively analyzed. The results show the existence of a background mode for aerosol loading in the troposphere and a pattern of distribution for transport and boundary layer aerosol for the Pacific region. The ARM (Atmospheric Radiation Measurement) program, operates surface based monitoring sites. For several years at sites in the central great plains and northern coast of Alaska of North America and a site in the tropical western Pacific have been acquiring comprehensive radiation measurements including multispectral aerosol optical thickness and near continuous lidar profiling. Data have been analyzed for typical and special case aerosol events including smoke aerosol from biomass burning for the tropical West Pacific site. Measurements with continuous lidar and multispectral were similarly acquired from a site at Tenerife, Canary Islands during the Aerosol Characterization Experiment and include analysis of the Saharan dust layer. Various measurements will be compared and summarized.

Spinhirne, James↗
NASA NTRS1999

Path Radiance Techniques for Retrieving Aerosol Optical Thickness over Land

The key issue in retrieving aerosol optical thickness over land from shortwave satellite radiances is to identify and separate the signal due to scattering by a largely transparent aerosol layer from the noise due to reflection by the background surface, where the signal is relatively uniform compared to the highly inhomogeneous surface contribution. Sensitivity studies in aerosol optical thickness retrievals reveal that the apparent reflectance at the top of the atmosphere is very susceptible to the surface reflectance, especially when aerosol optical thickness is small. Uncertainties associated with surface reflectance estimation can greatly amplify the error of the aerosol optical thickness retrieval. To reduce these uncertainties, we have developed a "path radiance" method to retrieve aerosol optical thickness over land by extending the traditional technique that uses the "dark object" approach to extract the aerosol signal. This method uses the signature of the correlation of visible and mid-IR reflectance at the surface, and couples the correlation with the atmospheric effect. We have applied this method to a TM (Landsat Thematic Mapper) image acquired over the Oklahoma Southern Great Plains (SGP) site of DoE's ARM (Atmospheric Radiation Measurement) program on September 27, 1997, a very clear day during the first Landsat IOP (Intensive Observation Period). The retrieved mean aerosol optical thickness for TM band 1 at 0.49 micrometers and band 3 at 0.66 micrometers agree very well with the ground-based sun-photometer measurements at the ARM site. The ability to retrieve small aerosol optical thickness (such as 0.07 at 0.5 micrometers as in the example considered here) makes this path radiance technique promising. More importantly, the path radiance is relatively insensitive to surface inhomogeneity. The retrieved mean path radiances in reflectance units have very small standard deviations for both TM blue and red bands. This small variability of path radiance further supports the current aerosol retrieval method.

Wen, Guoyong↗
NASA NTRS1999

Current Status of Aerosol Retrievals from TOMS

Properties of atmospheric aerosols over all land and water surfaces are retrieved from TOMS measurements of backscattered radiances. The TOMS technique, uses observations at two wavelengths. In the near ultraviolet (330-380 nm) range, where the effects of gaseous absorption are negligible. The retrieved properties are optical depth and a measure of aerosol absorptivity, generally expressed as single scattering albedo. The main sources of error of the TOMS aerosol products are sub-pixel cloud contamination and uncertainty on the height above the surface of UV-absorbing aerosol layers. The first error source is related to the large footprint (50 x 50 km at nadir) of the sensor, and the lack of detection capability of sub-pixel size clouds. The uncertainty associated with the height of the absorbing aerosol layers, on the other hand, is related to the pressure dependence of the molecular scattering process, which is the basis of the near-UV method of absorbing aerosol detection. The detection of non-absorbing aerosols is not sensitive to aerosol layer height. We will report on the ongoing work to overcome both of these difficulties. Coincident measurements of high spatial resolution thermal infrared radiances are used to address the cloud contamination issue. Mostly clear scenes for aerosol retrieval are selected by examining the spatial homogeneity of the IR radiance measurements within a TOMS pixel. The approach to reduce the uncertainty associated with the height of the aerosol layer by making use of a chemical transport model will also be discussed.

Torres, O.↗
NASA NTRS2000

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

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

Russell, P. B.↗
NASA NTRS2000

North Atlantic Aerosol Properties for Radiative Impact Assessments. Derived from Column Closure Analyses in TARFOX and ACE-2

Aerosol effects on atmospheric radiative fluxes provide a forcing function that can change the climate in potentially significant ways. This aerosol radiative forcing is a major source of uncertainty in understanding the climate change of the past century and predicting future climate. To help reduce this uncertainty, the 1996 Tropospheric Aerosol Radiative Forcing Observational Experiment (TARFOX) and the 1997 Aerosol Characterization Experiment (ACE-2) measured the properties and radiative effects of aerosols over the Atlantic Ocean. Both experiments used remote and in situ measurements from aircraft and the surface, coordinated with overpasses by a variety of satellite radiometers. TARFOX focused on the urban-industrial haze plume flowing from the United States over the western Atlantic, whereas ACE-2 studied aerosols over the eastern Atlantic from both Europe and Africa. These aerosols often have a marked impact on satellite-measured radiances. However, accurate derivation of flux changes, or radiative forcing, from the satellite measured radiances or retrieved aerosol optical depths (AODs) remains a difficult challenge. Here we summarize key initial results from TARFOX and ACE-2, with a focus on closure analyses that yield aerosol microphysical models for use in improved assessments of flux changes. We show how one such model gives computed radiative flux sensitivities (dF/dAOD) that agree with values measured in TARFOX and preliminary values computed for the polluted marine boundary layer in ACE-2. A companion paper uses the model to compute aerosol-induced flux changes over the North Atlantic from AVHRR-derived AOD fields.

Russell, Philip A.↗