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The Measurement of Aerosol Optical Properties using Continuous Wave Cavity Ring-Down Techniques

Large uncertainties in the effects that aerosols have on climate require improved in situ measurements of extinction coefficient and single-scattering albedo. This paper describes the use of continuous wave cavity ring-down (CW-CRD) technology to address this problem. The innovations in this instrument are the use of CW-CRD to measure aerosol extinction coefficient, the simultaneous measurement of scattering coefficient, and small size suitable for a wide range of aircraft applications. Our prototype instrument measures extinction and scattering coefficient at 690 nm and extinction coefficient at 1550 nm. The instrument itself is small (60 x 48 x 15 cm) and relatively insensitive to vibrations. The prototype instrument has been tested in our lab and used in the field. While improvements in performance are needed, the prototype has been shown to make accurate and sensitive measurements of extinction and scattering coefficients. Combining these two parameters, one can obtain the single-scattering albedo and absorption coefficient, both important aerosol properties. The use of two wavelengths also allows us to obtain a quantitative idea of the size of the aerosol through the Angstrom exponent. Minimum sensitivity of the prototype instrument is 1.5 x 10(exp -6)/m (1.5 M/m). Validation of the measurement of extinction coefficient has been accomplished by comparing the measurement of calibration spheres with Mie calculations. This instrument and its successors have potential to help reduce uncertainty currently associated with aerosol optical properties and their spatial and temporal variation. Possible applications include studies of visibility, climate forcing by aerosol, and the validation of aerosol retrieval schemes from satellite data.

Strawa, Anthony W.↗

The Measurement of Aerosol Optical Properties Using Continuous Wave Cavity Ring-Down Techniques

Large uncertainties in the effects that aerosols have on climate require improved in-situ measurements of extinction coefficient and single-scattering albedo. This abstract describes the use of continuous wave cavity ring-down (CW-CRD) technology to address this problem. The innovations in this instrument are the use of CW-CRD to measure aerosol extinction coefficient, the simultaneous measurement of scattering coefficient, and small size suitable for a wide range of aircraft applications. Our prototype instrument measures extinction and scattering coefficient at 690 nm and extinction coefficient at 1550 nm. The instrument itself is small (60 x 48 x 15 cm) and relatively insensitive to vibrations. The prototype instrument has been tested in our lab and used in the field. While improvements in performance are needed, the prototype has been shown to make accurate and sensitive measurements of extinction and scattering coefficients. Combining these two parameters, one can obtain the single-scattering albedo and absorption coefficient, both important aerosol properties. The use of two wavelengths also allows us to obtain a quantitative idea of the size of the aerosol through the Angstrom exponent. Minimum sensitivity of the prototype instrument is 1.5 x 10(exp -6)/m (1.5/Mm). Validation of the measurement of extinction coefficient has been accomplished by comparing the measurement of calibration spheres with Mie calculations. This instrument and its successors have potential to help reduce uncertainty currently associated with aerosol optical properties and their spatial and temporal variation. Possible applications include studies of visibility, climate forcing by aerosol, and the validation of aerosol retrieval schemes from satellite data.

Strawa, A. W.↗

Assessing the link between aerosol mixing state, structure and composition and their optical properties: Ascension Island as a testbed for the South‐East Atlantic aerosol regimes

Forest and savanna fires are a major source of pollution over the globe. Such fire events emit to the atmosphere a considerable amount of “fluffy” fractal black looking particles that are often referred to as black carbon (BC) or soot aerosols. In fact, BC particles (aerosols) emitted from savanna and agricultural fires over the African continent play an important role in the region’s and the global climate. These fires occur each year between July and October, which is referred to as the biomass burning (BB) season and are considered among the globe's largest man-made emission sources of BC particles. However, during these fire events, not only BC particles are emitted, but also other types of particles and gases that can interact with each other to create new particles, generating a slew of particles often generally referred to as BB aerosols. Although the majority of the fire emissions occur inland in the sub-Saharan part of Africa, their effect reaches far beyond the continent due to the prevailing easterly winds, which transport those aerosols over the South-East Atlantic (SEA) ocean, off the west-coast of Africa. The reason why these particles are so important to the regional and global climate is that they absorb sunlight radiation, which overall warms the climate. However, the magnitude of this warming effect is highly uncertain and depends upon a multitude of aspects. Our overarching goal for this project was to better understand the changes in the aerosol properties as they transport from fire sources downstream toward the ocean and how this can eventually affect the earth's radiative budget in terms of warming or cooling. Following the above, our work here was focused on the investigation of the African BB aerosol plumes mixing state (mixing of BB aerosols and other aerosol types), composition and size distribution as they transport from the African continent towards the SEA ocean, and their link with some of the commonly measurable bulk optical properties such as mass absorption coefficient (MAC) and single scattering albedo (SSA). We utilized three field missions that were conducted over the SEA ocean between 2016 and 2018. Specifically, we used (1) ground-based measurements from the DOE ARM Mobile Facility (AMF1), which was deployed at Ascension Island (ASI) for the LASIC (Layered Atlantic Smoke Interactions with Clouds) campaign between June 2016 and October 2017, (2) airborne measurements from the UK CLARIFY (Clouds and Aerosol Radiative impacts and Forcing) campaign during Aug-Sep-2017, and (3) airborne measurements from the ORACLES (Observations of Aerosols above Clouds and their interactions) campaign during Aug-2017, and Sep-Oct-2018. The three campaigns cover a relatively large region, from the western African coast on the east towards Ascension Island in the middle of the SEA to the west. We used the data gathered by these campaigns to find how BB properties and composition change from near emission sources (the ORACLES campaign flights) downstream (the CLARIFY flights and the ground based LASIC measurements). We used particle trajectory following methodologies to connect the measurements from the different campaigns, which allowed us to follow a certain aerosol plume (airmass) from near-source towards Ascension Island. We found out that atmospheric aging processes governed by the UV light from the sun (photochemistry) and cloud processes (aqueous chemistry) govern the changes seen in the particle composition during the transport were more dominant in dictating aerosol composition than specific emission composition or source types. We assessed how aerosol optical properties change during the BB season and what are the main drivers of this change. We found that the enhanced ratio of BC to CO is well correlated with single scattering albedo (SSA) and mass absorption coefficient (MACBC), providing a simple way to estimate the aerosol optical characteristics in the south-eastern Atlantic Ocean. From the analysis of the location of BB, the primary source fuel, the water content in the fuel, combined with the mean cloud cover and precipitation in the transport areas of the BB plume, we conclude that the increase in BC/CO from June to August is likely to be caused by burning becoming more flaming (hot fires), and the decrease in BC/CO in September and October may be caused by smoldering (colder) fires. We found that aerosol hygroscopicity increases with decreasing altitude below 2km, and that enhanced BB hygroscopicity at lower altitudes is mainly due to a lower organic aerosol (OA) fraction, increased sulfate fraction, and greater hygroscopicity parameter of OA at lower altitudes.

54 ENVIRONMENTAL SCIENCES↗

Sensitivity of Photolysis Frequencies and Key Tropospheric Oxidants in a Global Model to Cloud Vertical Distributions and Optical Properties

Clouds affect tropospheric photochemistry through modification of solar radiation that determines photolysis frequencies. As a follow-up study to our recent assessment of the radiative effects of clouds on tropospheric chemistry, this paper presents an analysis of the sensitivity of such effects to cloud vertical distributions and optical properties (cloud optical depths (CODs) and cloud single scattering albedo), in a global 3-D chemical transport model (GEOS-Chem). GEOS-Chem was driven with a series of meteorological archives (GEOS1- STRAT, GEOS-3 and GEOS-4) generated by the NASA Goddard Earth Observing System data assimilation system. Clouds in GEOS1-STRAT and GEOS-3 have more similar vertical distributions (with substantially smaller CODs in GEOS1-STRAT) while those in GEOS-4 are optically much thinner in the tropical upper troposphere. We find that the radiative impact of clouds on global photolysis frequencies and hydroxyl radical (OH) is more sensitive to the vertical distribution of clouds than to the magnitude of column CODs. With random vertical overlap for clouds, the model calculated changes in global mean OH (J(O1D), J(NO2)) due to the radiative effects of clouds in June are about 0.0% (0.4%, 0.9%), 0.8% (1.7%, 3.1%), and 7.3% (4.1%, 6.0%), for GEOS1-STRAT, GEOS-3 and GEOS-4, respectively; the geographic distributions of these quantities show much larger changes, with maximum decrease in OH concentrations of approx.15-35% near the midlatitude surface. The much larger global impact of clouds in GEOS-4 reflects the fact that more solar radiation is able to penetrate through the optically thin upper-tropospheric clouds, increasing backscattering from low-level clouds. Model simulations with each of the three cloud distributions all show that the change in the global burden of ozone due to clouds is less than 5%. Model perturbation experiments with GEOS-3, where the magnitude of 3-D CODs are progressively varied from -100% to 100%, predict only modest changes (<5%) in global mean OH concentrations. J(O1D), J(NO2) and OH3 concentrations show the strongest sensitivity for small CODs and become insensitive at large CODs due to saturation effects. Caution should be exercised not to use in photochemical models a value for cloud single scattering albedo lower than about 0.999 in order to be consistent with the current knowledge of cloud absorption at the ultraviolet wavelengths.

Liu, Hongyu↗

Updated MISR Dark Water Research Aerosol Retrieval Algorithm - Part 1: Coupled 1.1 km Ocean Surface Chlorophyll a Retrievals with Empirical Calibration Corrections

As aerosol amount and type are key factors in the 'atmospheric correction' required for remote-sensing chlorophyll alpha concentration (Chl) retrievals, the Multi-angle Imaging SpectroRadiometer (MISR) can contribute to ocean color analysis despite a lack of spectral channels optimized for this application. Conversely, an improved ocean surface constraint should also improve MISR aerosol-type products, especially spectral single-scattering albedo (SSA) retrievals. We introduce a coupled, self-consistent retrieval of Chl together with aerosol over dark water. There are time-varying MISR radiometric calibration errors that significantly affect key spectral reflectance ratios used in the retrievals. Therefore, we also develop and apply new calibration corrections to the MISR top-of-atmosphere (TOA) reflectance data, based on comparisons with coincident MODIS (Moderate Resolution Imaging Spectroradiometer) observations and trend analysis of the MISR TOA bidirectional reflectance factors (BRFs) over three pseudo-invariant desert sites. We run the MISR research retrieval algorithm (RA) with the corrected MISR reflectances to generate MISR-retrieved Chl and compare the MISR Chl values to a set of 49 coincident SeaBASS (SeaWiFS Bio-optical Archive and Storage System) in situ observations. Where Chl(sub in situ) less than 1.5 mg m(exp -3), the results from our Chl model are expected to be of highest quality, due to algorithmic assumption validity. Comparing MISR RA Chl to the 49 coincident SeaBASS observations, we report a correlation coefficient (r) of 0.86, a root-mean-square error (RMSE) of 0.25, and a median absolute error (MAE) of 0.10. Statistically, a two-sample Kolmogorov- Smirnov test indicates that it is not possible to distinguish between MISR Chl and available SeaBASS in situ Chl values (p greater than 0.1). We also compare MODIS-Terra and MISR RA Chl statistically, over much broader regions. With about 1.5 million MISR-MODIS collocations having MODIS Chl less than 1.5 mg m(exp -3), MISR and MODIS show very good agreement: r = 0.96, MAE = 0.09, and RMSE = 0.15. The new dark water aerosol/Chl RA can retrieve Chl in low-Chl, case I waters, independent of other imagers such as MODIS, via a largely physical algorithm, compared to the commonly applied statistical ones. At a minimum, MISR's multi-angle data should help reduce uncertainties in the MODIS-Terra ocean color retrieval where coincident measurements are made, while also allowing for a more robust retrieval of particle properties such as spectral single-scattering albedo.

Limbacher, James A.↗

Soot and Sulfuric Acid from Aircraft: Is There Enough to Cause Detrimental Environmental E-kCTSs?

Aerosol from aircraft can affect the environment in three ways: First, soot aerosol has been implicated to cause Icing-tern ozone depletion at mid-latitudes in the lower stratosphere at a rate of approx. 5% per decade. This effect is in addition and unrelated to the polar ozone holes which are strongly influenced by heterogeneous chemistry on polar stratospheric clouds. Second, the most obvious effect of jet aircraft is the formation of visible contrails in the upper troposphere. The Salt Lake City region experienced an 8% increase in cirrus cloud cover over a 15-year period which covariates with an increase in regional commercial air traffic. If soot particles act as freezing nuclei to cause contrail formation heterogeneously, they would be linked to a secondary effect to cloud modification that very likely is climatologically important. Third, a buildup of soot aerosol could reduce the single scatter albedo of stratospheric aerosol from 0.993+0.004 to 0.98, a critical value that has been postulated to separate stratospheric cooling from warming. Thus arises an important question: Do aircraft emit sufficient amounts of soot to have detrimental effects and warrant emission controls? During the 1996 SUCCESS field campaign, we sampled aerosols in the exhaust wake of a Boeing 757 aircraft and determined emission indices for sulfuric acid (EI(sub H2SO4) = 9.0E-2 and 5.0E-1 g/kg (sub FUEL) for 75 and 675 ppm fuel-sulfur, respectively) and soot aerosol (2.2E-3 less than EI(sub SOOT) = l.lE-2 g/kg (sub FUEL)). The soot particle analysis accounted for their fractal nature, determined electron-microscopically, which enhanced the surface area by a factor of 26 and the volume 11-fold over equivalent-volume spheres. The corresponding fuel-sulfur to H2SO4 conversion efficiency was 10% (for 675 ppmm fuel-S) and 37% (for 75 ppmm fuel-S). Applying the H2SO4 emission index to the 1990 fuel use by the worlds commercial fleets of 1.3E11 kg, a conversion efficiency of 30% of 500 ppmm fuel-S would have led to an annual contribution to the atmospheric sulfur budget by aircraft of 2.E7 kg H2SO4. This is about one part in 1.E4 of anthropogenic sulfate from other sources. The soot emission index given above yielded a 1990 injection of soot aerosol by aircraft of 1.E6 kg. Thus, soot amounts to only five percent of the aerosol generated by aircraft. Its reactivity with ozone would have to be 20 times that of sulfuric acid particles to make it chemically significant. Nevertheless, the findings, of stratospheric soot loadings commensurate with aircraft fuel consumption, based on the emission index given above and the assumption of stratospheric residence times of the order of one year implicate aircraft as stratospheric polluters. A trend similar to soot of H2SO4 aerosol loading could not be deciphered, neither from in situ measurements nor SAGE II satellite extinction, against the "noise" due to volcanic eruptions. Observation of soot particles at 20 km altitude which, if emitted by aircraft were generated at 10-12 km altitude, suggests a displacement of those particles against gravity. Because eddy mixing is virtually absent in the lower stratosphere and isentropic mixing explains lofting to only about 15 km, radiometric forces acting on morphologically and chemically asymmetric soot particles must be considered a possibility. The consequence could be an extended residence time of soot against that of sulfuric acid aerosol that would lower the single scatter albedo with time.

Pueschel, R. F.↗

Overview of ACE-Asia Spring 2001 Investigations On Aerosol-Radiation Interactions

ACE-Asia's extensive measurements from land, ocean, air and space quantified aerosol-radiation interactions. Results from each platform type, plus satellite-suborbital combinations, include: 1. Time series of multiwavelength aerosol optical depth (ADD), Angstrom exponent (alpha), single-scattering albedo (SSA), and size distribution from AERONET radiometry at 13 stations. In China and Korea AOD and alpha were strongly anticorrelated (reflecting transient dust events); dust volume-size modes peaked near 8 microns diameter; and SSA(dust) greater than SSA(pollution). 2. Calculations and measurements of photosynthetically active radiation and aerosols in China yield 24-h average downward surface radiative forcing per AOD(500 nm) of -27 W/sq m (400-700 nm). 3. The Hawaii-Japan cruise sampled a gradient with AOD(500 nm) extremes of 0.1 and 1.1. Shipboard measurements showed that adding dust to pollution increased SSA(550 nm, 55% RH), typically from -0.91 to approx. 0.97. Downwelling 8-12 micron radiances showed aerosol effects, especially in the major April dust event, with longwave forcing estimated at -5 to 15 W/sq m. 4. Extinction profiles from airborne sunphotometry and total-direct-diffuse radiometry show wavelength dependence often varying strongly with height, reflecting layering of dust-dominated over pollution-dominated aerosols. Comparing sunphotometric extinction profiles to those from in situ measurements (number and composition vs size, or scattering and absorption) shows layer heights agree, but extinction sometimes differs. 5. Airborne solar spectral flux radiometry yields absorption spectra for layers. Combining with AOD spectra yields best-fit aerosol single scattering albedo spectra. 6. Visible, NIR and total solar fluxes combined with AOD give radiative forcing efficiencies at surface and aloft.

Russell, P. B.↗

Clouds, hazes, and the stratospheric methane abundance in Neptune

Analysis of high-spatial-resolution (approximately 0.8 arcsec) methane band and continuum imagery of Neptune's relatively homogeneous Equatorial Region yields significant constraints on (1) the stratospheric gaseous methane mixing ratio (f(sub CH4, S)), (2) the column abundances and optical properties of stratospheric and tropospheric hydrocarbon hazes, and (3) the wavelength-dependent single-scattering albedo of the 3-bar opaque cloud. From the center-to-limb behavior of the 7270-A and 8900-A CH4 bands, the stratospheric methane mixing ratios is limited to f(sub CH4, S) less than 1.7 x 10(exp -3), with a nominal value of f(sub CH4, S) = 3.5 x 10(exp -4), one to two orders of magnitude less than pre-Voyager estimates, but in agreement with a number of recent ultraviolet and thermal infrared measurements, and largely in agreement with the tropopause mixing ratio implied by Voyager temperature measurements. Upper limits to the stratospheric haze mass column abundance and 6190-A and 8900-A haze opacities are 0.61 micrograms/sq cm and 0.075 and 0.042, respectively, with nominal values of 0.20 micrograms/sq cm and 0.025 and 0.014 for the 0.2 micrometers radius particles preferred by the recent Voyager PPS analysis of Pryor et al. (1992). The tropospheric CH4 haze opacities are comparable to that found in the stratosphere, i.e., upper limits of 0.104 and 0.065 at 6190 A and 8900 A, respectively, with nominal values of 0.085 and 0.058. This indicates a column abundance less than 11.0 micrograms/sq cm, corresponding to the methane gas content within a well-mixed 3% methane tropospheric layer only 0.1 cm thick near the 1.5-bar CH4 condensation level. Conservative scattering is ruled out for the opaque cloud near 3 bars marking the bottom of the visible atmosphere. Specifically, we find cloud single-scattering albedos of 0.915 +/- 0.006 at 6340 A, 0.775 +/- 0.012 at 7490 A, and 0.803 +/- 0.010 at 8260 A. Global models utilizing a complete global spectrum confirm the red-absorbing character of the 3-bar cloud. The global-mean model has approximately 7.7 times greater stratospheric aerosol content than the Equatorial Region. An analysis of stratospheric haze precipitation rates indicates a steady-state haze production rate of 0.185-1.5 x 10(exp -14) g/sq cm/s, in agreement with recent theoretical photochemical estimates. Finally, reanalysis of the Voyager PPS 7500-A phase angle data utilizing the f(sub CH4, S) value derived here confirms the Pryor et al. result of a tropospheric CH4 haze opacity of a few tenths in the 22-30 degs S latitude region, several times that of the Equatorial Region or of the globe. The factor-of-10 reduction in f(sub CH4, S) below that assumed by Pryor et al. implies decreased gas absorption and consequently a decrease in the forward-scattering component of tropospheric aerosols.

Baines, Kevin H.↗

Albedos of homogeneous semi-infinite canopies - Comparison of two-stream analytic and numerical solutions

The albedo of plant canopies is treated as a problem in radiative transfer. Albedos calcualted from an iterative multistream numerical model are compared with those calculated with an analytic two-stream solution. With the assumption of a randomly homogeneous distribution of leaf positions and orientations and isotropic scattering by individual leaves, the single-scattering albedo of the canopy can be found analytically. This single-scattering solution is incorporated into the two-stream solution and used to benchmark the multistream numerical model in the single-scattering limit. Relative errors so established in the multistream model are O(0.3 percent) or less. The two-stream model is also found to be remarkably accurate, with the error in multiply scattered radiation O(5 percent) or less, corresponding to absolute errors in visible albedo of less than 0.001 and near-infrared albedo of less than or equal to 0.01. Thus the two-stream model should be adequate for many purposes, such as climate modeling, provided the assumptions of homogeneous canopy and isotropic scattering are not too unrealistic.

Dickinson, Robert E.↗

Effective Albedo of Vegetated Terrain at L-Band

This paper derives an explicit expression for an effective albedo of vegetated terrain from the zero- and multiple- order radiative transfer (RT) model comparison. The formulation establishes a direct physical link between the effective vegetation parameterization and the theoretical description of absorption and scattering within the canopy. The paper will present an evaluation of the derived albedo for corn canopies with data taken during an experiment at Alabama A&M Winfield A. Thomas Agricultural Research Station near Huntsville, Alabama in June, 1998. The test site consisted of two 50-m x 60-m plots - one with a bare surface and the other with grass cover - and four 30-m x 50-m plots of corn at different planting densities. One corn field was planted at a full density of 9.5 plants/sq m while the others were planted at 1/3, 1/2 and 2/3 of the full density. The fields were observed with a truck-mounted L-band radiometer at incident angle of 15 degree for the period of two weeks. Soil moisture (SM) changed daily due to irrigation and natural rainfall. Variations in gravimetric SM from 18 % to 34 % were seen during this period. Ground truth data, including careful characterization of the corn size and orientation statistics, and its dielectric, was also collected and used to simulate the effective albedo for the vegetation. The single-scattering albedo is defined as the fractional power scattered from individual vegetation constituents with respect to canopy extinction. It represents single-scattering properties of vegetation elements only, and is independent of ground properties. The values of the albedo get higher when there is dense vegetation (i.e. forest, mature corn, etc.) with scatterers, such as branches and trunks (or stalks in the case of corn), which are large with respect to the wavelength. This large albedo leads to a reduction in brightness temperature in the zero-order RT solution (known as tau-omega model). Higher-order multiple-scattering RT solutions are required for proper representation of scattering within vegetation. In this paper, an expression for an effective albedo for the whole canopy including the ground is derived for use in the zero-order RT model-based SM retrieval. This effective albedo takes into account of all the processes taking place within the canopy, including multiple-scattering. This new formulation will be presented and its importance for microwave SM retrieval will be evaluated for corn canopies in conjunction with the detailed ground truth data obtained during the experiment at Alabama in 1998. Emphasis will be placed on examining how the radiometer response to SM is modified by the corn canopy scattering under different field conditions. A semi-empirical parameterization of the effective albedo will be investigated through analysis of SM and vegetation water content effects on the effective albedo.

Kurum, Mehmet↗

Environmental Snapshots for Satellite Multi-Angle Aerosol Retrieval Validation During the ACE-Asia Field Campaign

On five occasions spanning the ACE-Asia field experiment in spring 2001, the multi-angle imaging MISR instrument, flying aboard the NASA Earth Observing System s Terra satellite, took quarter-kilometer data over a 400-km-wide swath, coincident with high-quality observations by multiple instruments on two or more participating surface and airborne platforms. The cases capture a range of clean, polluted, and dusty aerosol conditions. They represent some of the best opportunities during ACE- Asia for comparative studies among intensive and extensive aerosol observations in their environmental context. We inter-compare related measurements and discuss the implications of apparent discrepancies for each case, at a level of detail appropriate to the analysis of satellite observations. With a three-stage optical modeling process, we synthesize data from multiple sources into layer-by-layer snapshots that summarize what we know about the state of the atmosphere and surface at key locations during each event, to be used for satellite vicarious calibration and aerosol retrieval validation. Aerosols within a few kilometers of the surface were composed primarily of pollution and Asian dust mixtures, as expected. Accumulation and coarse-mode particle size distributions varied little among the events studied, but column aerosol optical depth changed by more than a factor of four, and the near-surface proportion of dust ranged from about 25% to 50%. The amount of absorbing material in the sub-micron fraction was highest when near-surface winds crossed Beijing and the Korean Peninsula, and was considerably lower for all other cases. Ambiguities remain in segregating size distributions by composition; having simultaneous single scattering albedo measurements at more than a single wavelength would significantly reduce the resulting optical model uncertainties, as would integral constraints from surface and atmospheric radiative flux observations. The consistency of component particle micro-physical properties among the five events, even in this relatively complex aerosol environment, suggests that global, satellite-derived maps of aerosol-air-mass-type extent, combined with targeted in situ measurements, can provide a detailed global picture of aerosol behavior. Further joint satellite and in situ analysis is needed to assess the spatial variability of both intensive and extensive aerosol properties within aerosol air masses in two spatial dimensions.

Kahn, Ralph↗

Retrieval of Aerosol Microphysical Properties from AERONET Photo-Polarimetric Measurements. 2: A New Research Algorithm and Case Demonstration

A new research algorithm is presented here as the second part of a two-part study to retrieve aerosol microphysical properties from the multispectral and multiangular photopolarimetric measurements taken by Aerosol Robotic Network's (AERONET's) new-generation Sun photometer. The algorithm uses an advanced UNified and Linearized Vector Radiative Transfer Model and incorporates a statistical optimization approach.While the new algorithmhas heritage from AERONET operational inversion algorithm in constraining a priori and retrieval smoothness, it has two new features. First, the new algorithmretrieves the effective radius, effective variance, and total volume of aerosols associated with a continuous bimodal particle size distribution (PSD) function, while the AERONET operational algorithm retrieves aerosol volume over 22 size bins. Second, our algorithm retrieves complex refractive indices for both fine and coarsemodes,while the AERONET operational algorithm assumes a size-independent aerosol refractive index. Mode-resolved refractive indices can improve the estimate of the single-scattering albedo (SSA) for each aerosol mode and thus facilitate the validation of satellite products and chemistry transport models. We applied the algorithm to a suite of real cases over Beijing_RADI site and found that our retrievals are overall consistent with AERONET operational inversions but can offer mode-resolved refractive index and SSA with acceptable accuracy for the aerosol composed by spherical particles. Along with the retrieval using both radiance and polarization, we also performed radiance-only retrieval to demonstrate the improvements by adding polarization in the inversion. Contrast analysis indicates that with polarization, retrieval error can be reduced by over 50% in PSD parameters, 10-30% in the refractive index, and 10-40% in SSA, which is consistent with theoretical analysis presented in the companion paper of this two-part study.

aerosol retrieval algorithm↗

Analysis of Aerosol Type and Fine- and Coarse-mode Aerosol Direct Radiative Forcing over Regions in East and Southeast Asia Based on AERONET Version 3 Data

Based on the particle linear depolarization ratio (PLDR) and single-scattering albedo (SSA) values obtained for 1020 nm from Aerosol Robotic Network (AERONET) Version 3 Level 2.0 data collected in five regions, namely, northern China, Northwest Asia, the Tibetan Plateau, southern China and Southeast Asia, we classified seven types of aerosol (viz., purely dust, dust-dominated, pollution-dominated, non-absorbing [NA], weakly absorbing [WA], moderately absorbing [MA] and strongly absorbing [SA]) in order to assess the spatial and temporal distributions of their constituents and the radiative effects of their fine- and coarse-mode particles. The fine fraction dominated in northern China and also played a crucial role on the Tibetan Plateau and in southern China and Southeast Asia, whereas the coarse fraction prevailed in Northwest Asia. Furthermore, the fine-mode aerosol on the Tibetan Plateau exhibited its maximum radiative forcing efficiency (110.3 W m–2) during high concentrations of SA aerosol. Also, the lowest values for both the radiative forcing and the radiative forcing efficiency in southern China occurred during summer. Finally, the various aerosol constituents displayed distinct spatial and temporal distributions in Southeast Asia, with the SA aerosol contributing approximately 20% of the total aerosol on the Indochinese Peninsula and the NA and WA aerosol forming the largest percentages on the Malay Peninsula.

Particle linear depolarization ratio↗

The Sensitivity of SeaWiFS Ocean Color Retrievals to Aerosol Amount and Type

As atmospheric reflectance dominates top-of-the-atmosphere radiance over ocean, atmospheric correction is a critical component of ocean color retrievals. This paper explores the operational Sea-viewing Wide Field-of-View Sensor (SeaWiFS) algorithm atmospheric correction with approximately 13 000 coincident surface-based aerosol measurements. Aerosol optical depth at 440 nm (AOD(sub 440)) is overestimated for AOD below approximately 0.1-0.15 and is increasingly underestimated at higher AOD; also, single-scattering albedo (SSA) appears overestimated when the actual value less than approximately 0.96.AOD(sub 440) and its spectral slope tend to be overestimated preferentially for coarse-mode particles. Sensitivity analysis shows that changes in these factors lead to systematic differences in derived ocean water-leaving reflectance (Rrs) at 440 nm. The standard SeaWiFS algorithm compensates for AOD anomalies in the presence of nonabsorbing, medium-size-dominated aerosols. However, at low AOD and with absorbing aerosols, in situ observations and previous case studies demonstrate that retrieved Rrs is sensitive to spectral AOD and possibly also SSA anomalies. Stratifying the dataset by aerosol-type proxies shows the dependence of the AOD anomaly and resulting Rrs patterns on aerosol type, though the correlation with the SSA anomaly is too subtle to be quantified with these data. Retrieved chlorophyll-a concentrations (Chl) are affected in a complex way by Rrs differences, and these effects occur preferentially at high and low Chl values. Absorbing aerosol effects are likely to be most important over biologically productive waters near coasts and along major aerosol transport pathways. These results suggest that future ocean color spacecraft missions aiming to cover the range of naturally occurring and anthropogenic aerosols, especially at wavelengths shorter than 440 nm, will require better aerosol amount and type constraints.

single scattering albedo↗

Aerosols Optical and Radiative Properties in Indonesia Based on AERONET Version 3

Heterogeneity in seasonal aerosol types due to different sources, local characteristics, and meteorology lead to different optical and radiative properties from one place to another. This study analyzes the long-term averages of aerosol optical and radiative properties obtained by the Aerosol Robotic Network (AERONET) version 3 at four sites in Indonesia representing fire prone areas (Palangka Raya, Pontianak, Jambi: 2012–2020), and urban-industrial (Bandung: 2009–2018). We examined the seasonal variation of aerosol optical depth (AOD), Angstrom Exponent (AE), Precipitable Water Vapor (PWV), and Single Scattering Albedo (SSA) combined with meteorological parameters at these Indonesian sites. Multiple clustering techniques from different relationships among various aerosol optical and radiative parameters was employed to further study the aerosol type in respect to different seasonality. The results exhibited a distinct seasonal pattern at all sites except Bandung, whereas AOD increased owing to forest and peat fire outbreaks during the dry season. The trend in AOD annual depicts an increase in Bandung as emission from urban/industrial increases episodically, while it depicts a decrease at the three biomass burning sites. As AOD increased, Palangka Raya, Pontianak, and Jambi exhibited wider ranges of observed AE (1.2–1.8) and high FMF (>0.8) in the dry burning period (June to October). On the other hand, Bandung has more aerosol distribution in the range of FMF values 0.6–1 and AE 1–1.6, compared with other sites, suggesting contribution of complex aerosol emission from different sources and likely due to the formation of secondary aerosol production from trace gases. Palangka Raya, Pontianak, and Jambi exhibited non-absorbing characteristics, as indicated by high SSA (>0.95), high FMF, and high EAE values (1.2–1.7) with no discrepancy in seasonal patterns, implying that biomass burning aerosols in Indonesia tend to cool the atmosphere with strong scattering rather than absorbing. At Bandung, aerosols mixed with slightly absorbing and non-absorbing aerosols owing to urban and industrial emissions. This study lays a foundation for further research on the contribution of aerosol radiative forcing to climate within the complex aerosol and cloud environments in Indonesia.

Aerosol optical depth↗

IPN Absorption Coefficients

The dataset contains aerosol light absorption and scattering coefficients measured by three single-wavelength Integrated Photoacoustic Nephelometers (IPN). The absorption coefficients were measured at 405, 721, and 1047 nm, while the scattering coefficients were measured at 405 and 721 nm. The single scattering albedo (SSA) at 405 and 721 nm were also calculated from the IPN measurements. The three IPNs shared a common inlet without impactor/cyclone in July; in August, a PM2.5 cyclone inlet was installed to reduce measurement noise and improve data quality. The 721-nm IPN experienced laser shutdown issues, causing missing of a large fraction of the 721-nm measurements, especially in July. As described before, the 721-nm laser issue was less frequent in August after the cyclone installation, improving the data completeness and quality. The IPN raw data were noisy, making identifying patterns and trends difficult; therefore, the hourly average data are recommended over the raw data. The hourly average data were cross-checked with the filter-based TAP and PSAP measurements, which showed that their patterns, trends, and peaks matched. However, due to the differences in working mechanisms and principles of the filter-based and photoacoustic particle-phase instruments, the IPN measurements are lower than the filter-based measurements despite that they have consistent patterns, trends, and peaks.

54 ENVIRONMENTAL SCIENCES↗

Temporal and spatial mapping of surface albedo and atmospheric dust opacity on Mars

The Mariner 9 and Viking provided abundant evidence that eolian processes are active over much of the surface of Mars. Past studies have demonstrated that variations in regional albedo and wind-streak patterns are indicative of sediment transport through a region, while thermal inertia data (derived from the Viking Infrared Thermal Mapper (IRTM) dataset) are indicative of the degree of surface mantling by dust deposits. The visual and thermal data are therefore diagnostic of whether net erosion or deposition of dust-storm fallout is taking place currently and whether such processes have been active in a region over the long term. These previous investigations, however, have not attempted to correct for the effects of atmospheric dust loading on observations of the martian surface, so quantitative studies of current sediment transport rates have included large errors due to uncertainty in the magnitude of this 'atmospheric component' of the observations. We have developed a radiative transfer model that allows the atmospheric dust opacity to be determined from IRTM thermal observations. Corrections for the effects of atmospheric dust loading on observations of surface albedo can also be modeled. This approach to determining 'dust-corrected surface albedo' incorporates the atmospheric dust opacity, the single-scattering albedo and particle phase function of atmospheric dust, and the bidirectional reflectance of the surface, and it accounts for variable lighting and viewing geometry.

Lee, S. W.↗

Temporal and spatial mapping of atmospheric dust opacity and surface albedo on Mars

The Mariner 9 and Viking missions provided abundant evidence that eolian processes are active over much of the surface of Mars. Past studies have demonstrated that variations in regional albedo and wind streak patterns are indicative of sediment transport through a region, while thermal inertia data (derived from the Viking Infrared Thermal Mapper (IRTM) datasets) are indicative of the degree of surface mantling by dust deposits. We are making use of the method developed by T. Z. Martin to determine dust opacity from IRTM thermal observations. We have developed a radiative transfer model that allows corrections for the effects of atmospheric dust loading on observations of surface albedo to be made. This approach to determining 'dust-corrected surface albedo' incorporates the atmospheric dust opacity, the single-scattering albedo and particle phase function of atmospheric dust, the bidirectional reflectance of the surface, and accounts for variable lighting and viewing geometry.

Lee, S. W.↗