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At least 307 records · Page 17

Influence of Humidity on the Aerosol Scattering Coefficient and Its Effect on the Upwelling Radiance During ACE-2

Aerosol scattering coefficients (sigma(sub sp)) have been measured over the ocean at different relative humidities (RH) as a function of attitude in the region surrounding the Canary Islands during the Second Aerosol Characterization Experiment (ACE-2) in June and July 1997. The data were collected by the University of Washington passive humidigraph (UWPH) mounted on the Pelican research aircraft. Concurrently, particle size distributions absorption coefficients and aerosol optical depth were measured throughout 17 flights. A parameterization of sigma(sub sp) as a function of RH was utilized to assess the impact of aerosol hydration on the upwelling radiance (normalized to the solar constant and cosine of zenith angle). The top of the atmosphere radiance signal was simulated at wavelengths corresponding to visible and near-infrared bands or the EOS-AM ("Terra") detectors, MODIS and MISR. The UWPH measured (sigma(sub sp)) at 2 RHs, one below and the other above ambient conditions. Ambient (sigma(sub sp)) was obtained by interpolation of these 2 measurements. The data were stratified in terms of 3 types of aerosols: Saharan dust, clean marine (marine boundary layer background) and polluted marine aerosols (i.e., 2- or 1-day old polluted aerosols advected from Europe). An empirical relation for the dependence of (sigma(sub sp)) on RH, defined by (sigma(sub sp))(RH) = k. ((1 - RH/100)(exp -gamma), was used with the hygroscopic exponent gamma derived from the data. The following gamma values were obtained for the 3 aerosol types: gamma(dust) = 0.23 +/- 0.05, gamma(clean marine) = 0.69 +/- 0.06 and gamma(polluted marine) = 0.57 + 0.06. Based on the measured (gamma)(s), the above equation was utilized to derive aerosol models with different hygroscopicities. The satellite simulation signal code 6S was used to compute the upwelling radiance corresponding to each of those aerosol models at several ambient humidities. For the pre-launch estimated precision of the sensors and the assumed viewing geometry of the instrument, the simulations suggest that the spectral and angular dependence of the reflectance measured by MISR is not sufficient to distinguish aerosol models with various different combinations of values ror dry composition. y and ambient RH. A similar behavior is observed for MODIS at visible wavelengths. However, the 2100 nm band of MODIS appears to be able to differentiate between at least some aerosol models with different aerosol hygroscopicity given the MODIS calibration error requirements. This result suggests the possibility of retrieval of aerosol hygroscopicity by MODIS.

Gasso, B. S.↗

Influence of Humidity On the Aerosol Scattering Coefficient and Its Effect on the Upwelling Radiance During ACE-2

Aerosol scattering coefficients (sigma(sub sp)) have been measured over the ocean at different relative humidities (RH) as a function of altitude in the region surrounding the Canary Islands during the Second Aerosol Characterization Experiment (ACE-2) in June and July 1997. The data were collected by the University of Washington passive humidigraph (UWPH) mounted on the Pelican research aircraft. Concurrently, particle size distributions, absorption coefficients and aerosol optical depth were measured throughout 17 flights. A parameterization of sigma(sub sp) as a function of RH was utilized to assess the impact of aerosol hydration on the upwelling radiance (normalized to the solar constant and cosine of zenith angle). The top of the atmosphere radiance signal was simulated at wavelengths corresponding to visible and near-infrared bands of the EOS (Earth Observing System) AM-1 (Terra) detectors, MODIS (Moderate Resolution Imaging Spectroradiometer) and MISR (Multi-angle Imaging Spectroradiometer). The UWPH measured sigma(sub sp) at two RHs, one below and the other above ambient conditions. Ambient sigma(sub sp) was obtained by interpolation of these two measurements. The data were stratified in terms of three types of aerosols: Saharan dust, clean marine (marine boundary layer background) and polluted marine aerosols (i.e., two- or one-day old polluted aerosols advected from Europe). An empirical relation for the dependence of sigma(sub sp) on RH, defined by sigma(sub sp)(RH) = k.(1 - RH/100)(sup gamma), was used with the hygroscopic exponent gamma derived from the data. The following gamma values were obtained for the 3 aerosol types: gamma(dust) = 0.23 +/- 0.05, gamma(clean marine) = 0.69 +/- 0.06 and gamma(polluted marine) = 0.57 +/- 0.06. Based on the measured gammas, the above equation was utilized to derive aerosol models with different hygroscopicities. The satellite simulation signal code 6S was used to compute the upwelling radiance corresponding to each of those aerosol models at several ambient humidities. For the prelaunch estimated precision of the sensors and the assumed viewing geometry of the instrument, the simulations suggest that the spectral and angular dependence of the reflectance measured by MISR is not sufficient to distinguish aerosol models with various different combinations of values for dry composition, gamma and ambient RH. A similar behavior is observed for MODIS at visible wavelengths. However, the 2100 nm band of MODIS appears to be able to differentiate between at least same aerosol models with different aerosol hygroscopicity given the MODIS calibration error requirements. This result suggests the possibility of retrieval of aerosol hygroscopicity by MODIS.

Gasso, S.↗

Comparison of GFED3, QFED2 and FEER1 Biomass Burning Emissions Datasets in a Global Model

Biomass burning contributes about 40% of the global loading of carbonaceous aerosols, significantly affecting air quality and the climate system by modulating solar radiation and cloud properties. However, fire emissions are poorly constrained in models on global and regional levels. In this study, we investigate 3 global biomass burning emission datasets in NASA GEOS5, namely: (1) GFEDv3.1 (Global Fire Emissions Database version 3.1); (2) QFEDv2.4 (Quick Fire Emissions Dataset version 2.4); (3) FEERv1 (Fire Energetics and Emissions Research version 1.0). The simulated aerosol optical depth (AOD), absorption AOD (AAOD), angstrom exponent and surface concentrations of aerosol plumes dominated by fire emissions are evaluated and compared to MODIS, OMI, AERONET, and IMPROVE data over different regions. In general, the spatial patterns of biomass burning emissions from these inventories are similar, although the strength of the emissions can be noticeably different. The emissions estimates from QFED are generally larger than those of FEER, which are in turn larger than those of GFED. AOD simulated with all these 3 databases are lower than the corresponding observations in Southern Africa and South America, two of the major biomass burning regions in the world.

biomass burning↗

Hyperspectral modeling for extracting aerosols from aircraft/satellite data

Sensitivity studies using the Airborne Visible/Infrared Imaging Spectrometer (AVIRIS) bands are currently under investigation. The objective of this research is to develop improved algorithms for the determination of aerosol type (e.g., presently described by S(sub 12). Preliminary computer calculations were made using LOWTRAN 7, which is the most advanced atmospheric code of the Air Force Geophysics Laboratory. LOWTRAN 7 permits the calculation of atmospheric transmission and absorption caused by aerosols and molecules along a non-homogeneous path for a variety of aerosol models. The calculations used the Navy Aerosol Model (NAM), which was constructed for the marine environment using a three component size distribution model. Calculations of the total transmittance (L(sub T)), the path radiance (L(sub P)), and the reflected radiance (L(sub r)) were made as a function of wavelength (lambda) from 0.4 to 2.4 microns for each of the 224 10 nm wide AVIRIS bands. These calculations were made for various types of atmospheres for the troposphere (0-2 km).

Hickman, G. Daniel↗

Physical and Optical/Radiative Properties of Arctic Aerosols: Potential Effects on Arctic Climate

We have determined the abundance of light-scattering sulfuric acid (H2SO4/H2O) and light-absorbing black carbon aerosol (BCA) in Spring 1992 in the Arctic atmosphere by airborne in situ sampling with impactors, and measured particle sizes and morphologies by scanning electron microscopy. The mass of BCA in the Arctic troposphere is one percent of the total aerosol, reduced to one part in 104 in the stratosphere. A Mie algorithm permits the calculation of the optical properties of the various aerosol components, and an algorithm developed by Ackerman and Toon and modified to serve our needs lets us calculate the optical effects of the black carbon aerosol that is mixed internally with the sulfuric acid aerosol. It follows that the effect of internally-mixed BCA on the aerosol scattering and absorption properties depends on its location within the droplet. BCA concentrated near the droplet surface has a greater effect on absorption of solar radiation than does the same amount of BCA located near its center. Single scatter albedos of the combined system are omega(sub 0)=1.0 in the post-Pinatubo Arctic stratosphere, and as low as 0.94 in the troposphere. The aerosol has the potential to regionally warm the Arctic earth-atmosphere system, because of the high surface albedo of the snow-covered Arctic.

Pueschel, R. F.↗

Vertical Profiles of Light Scattering, Light Absorption, and Single Scattering Albedo during the Dry, Biomass Burning Season in Southern Africa and Comparisons of In Situ and Remote Sensing Measurements of Aerosol Optical Depths

Airborne in situ measurements of vertical profiles of aerosol light scattering, light absorption, and single scattering albedo (omega (sub 0)) are presented for a number of locations in southern Africa during the dry, biomass burning season. Features of the profiles include haze layers, clean air slots, and marked decreases in light scattering in passing from the boundary layer into the free troposphere. Frequency distributions of omega (sub 0) reflect the strong influence of smoke from biomass burning. For example, during a period when heavy smoke was advected into the region from the north, the mean value of omega (sub 0) in the boundary layer was 0.81 +/- 0.02 compared to 0.89 +/- 0.03 prior to this intrusion. Comparisons of layer aerosol optical depths derived from the in situ measurements with those measured by a Sun photometer aboard the aircraft show excellent agreement.

Magi, Brian I.↗

Saharan dust effects on North Atlantic sea surface skin Temperatures

Saharan dust outbreaks frequently propagate westward over the Atlantic Ocean; accurate quantification of the dust aerosol scattering and absorption effect on the surface radiative fluxes (SRF) is fundamental to understanding critical climate feedbacks. By exploiting large sets of measurements from many ship campaigns in conjunction with reanalysis products, this study characterizes the sensitivity of the SRF and skin Sea‐Surface Temperature (SSTskin) to the Saharan dust aerosols using models of the atmospheric radiative transfer and thermal skin effect. Saharan dust outbreaks can decrease the surface shortwave radiation up to 190 W/sq.m, and an analysis of the corresponding SST(skin) changes using a thermal skin model suggests dust‐induced cooling effects as large as −0.24 K during daytime and a warming effect of up of 0.06 K during daytime and nighttime respectively. Greater physical insight into the radiative transfer through an aerosol‐burdened atmosphere will substantially improve the predictive capabilities of weather and climate studies on a regional basis.

Saharan Dust↗

A Strong Anthropogenic Black Carbon Forcing Constrained by Pollution Trends Over China

Estimates of the effective radiative forcing from aerosol-radiation interaction (ERF ari ) of anthropogenic Black Carbon (BC) have been disputable and require better constraints. Here we find a substantial decline in atmospheric absorption of −5.79Wm −2 decade −1 over eastern central China (ECC) responding to recent anthropogenic BC emission reductions. By combining the observational finding with advances from Coupled Model Intercomparison Project phase6 (CMIP6), we identify an emergent constraint on the ERF ari of anthropogenic BC. We show that across CMIP6 models the simulated trends correlate well with simulated annual mean shortwave atmospheric absorption by anthropogenic BC over China. Making use of this emergent relationship allows us to constrain the aerosol absorption optical depth of anthropogenic BC and further provide a constrained range of 2.4–3.0 Wm −2 for its top-of-atmosphere ERF ari over China, higher than existing estimates. Furthermore, our work supports a strong warming effect of BC over China, and highlights the need to improve BC simulations over source regions.

CMIP6 models↗

Global Aerosol Radiative Forcing Derived from Sea WiFS-Inferred Aerosol Optical Properties

Aerosol optical properties inferred from the Sea-viewing Wide Field-of-view Sensor (SeaWiFS) radiance measurements are used to compute the aerosol shortwave radiative forcing using a radiative transfer model. The aerosol optical thickness at the wavelength of 865-nm is taken from the SeaWIFS archive. It is found that the nominal optical thickness over oceans ranges from 0.1 to 0.2. Using a maritime aerosol model and the radiances measured at the various SeaWiFS channels, the Angstrom exponent is determined to be 0.2174, the single-scattering albedo to be 0.995, and the asymmetry factor to be 0.786. The radiative transfer model has eight bands in the visible and ultraviolet spectral regions and three bands in the near infrared. It includes the absorption due to aerosols, water vapor, carbon dioxide, and oxygen, and the scattering due to aerosols and gases (Rayleigh scattering). The radiative forcing is computed over global oceans for four months (January, April, July, and October, 1998) to represent four seasons. It is found that the aerosol radiative forcing is large and changes significantly with seasons near the continents with large-scale forest fires and desert dust. Averaged over oceans and the four months, the aerosol radiative forcing is approximately 7 W/sq m at the top of the atmosphere. This large radiative forcing is expected to have a significant cooling effect on the Earth's climate as implied from simulations of a number of general circulation models.

Chou, Ming-Dah↗

Modeled and observed properties related to the direct aerosol radiative effect of biomass burning aerosol over the southeastern Atlantic

Biomass burning smoke is advected over the southeastern Atlantic Ocean between July and October of each year. This smoke plume overlies and mixes into a region of persistent low marine clouds. Model calculations of climate forcing by this plume vary significantly in both magnitude and sign. NASA EVS-2 (Earth Venture Suborbital-2) ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) had deployments for field campaigns off the west coast of Africa in 3 consecutive years (September 2016, August 2017, and October 2018) with the goal of better characterizing this plume as a function of the monthly evolution by measuring the parameters necessary to calculate the direct aerosol radiative effect. Here, this dataset and satellite retrievals of cloud properties are used to test the representation of the smoke plume and the underlying cloud layer in two regional models (WRF-CAM5 and CNRM-ALADIN) and two global models (GEOS and UM-UKCA). The focus is on the comparisons of those aerosol and cloud properties that are the primary determinants of the direct aerosol radiative effect and on the vertical distribution of the plume and its properties. The representativeness of the observations to monthly averages are tested for each field campaign, with the sampled mean aerosol light extinction generally found to be within 20 % of the monthly mean at plume altitudes. When compared to the observations, in all models, the simulated plume is too vertically diffuse and has smaller vertical gradients, and in two of the models (GEOS and UM-UKCA), the plume core is displaced lower than in the observations. Plume carbon monoxide, black carbon, and organic aerosol masses indicate underestimates in modeled plume concentrations, leading, in general, to underestimates in mid-visible aerosol extinction and optical depth. Biases in mid-visible single scatter albedo are both positive and negative across the models. Observed vertical gradients in single scatter albedo are not captured by the models, but the models do capture the coarse temporal evolution, correctly simulating higher values in October (2018) than in August (2017) and September (2016). Uncertainties in the measured absorption Ångstrom exponent were large but propagate into a negligible (<4 %) uncertainty in integrated solar absorption by the aerosol and, therefore, in the aerosol direct radiative effect. Model biases in cloud fraction, and, therefore, the scene albedo below the plume, vary significantly across the four models. The optical thickness of clouds is, on average, well simulated in the WRF-CAM5 and ALADIN models in the stratocumulus region and is underestimated in the GEOS model; UM-UKCA simulates cloud optical thickness that is significantly too high. Overall, the study demonstrates the utility of repeated, semi-random sampling across multiple years that can give insights into model biases and how these biases affect modeled climate forcing. The combined impact of these aerosol and cloud biases on the direct aerosol radiative effect (DARE) is estimated using a first-order approximation for a subset of five comparison grid boxes. A significant finding is that the observed grid box average aerosol and cloud properties yield a positive (warming) aerosol direct radiative effect for all five grid boxes, whereas DARE using the grid-box-averaged modeled properties ranges from much larger positive values to small, negative values. It is shown quantitatively how model biases can offset each other, so that model improvements that reduce biases in only one property (e.g., single scatter albedo but not cloud fraction) would lead to even greater biases in DARE. Across the models, biases in aerosol extinction and in cloud fraction and optical depth contribute the largest biases in DARE, with aerosol single scatter albedo also making a significant contribution.

54 ENVIRONMENTAL SCIENCES↗

Characterization of Aerosols over the Indochina Peninsula from Satellite-Surface Observations During Biomass Burning Pre-Monsoon Season

This paper presents characterization of aerosols over the Indochina peninsular regions of Southeast Asia during pre-monsoon season from satellite and ground-based radiometric observations. Our analysis focuses on the seasonal peak period in aerosol loading and biomass burning, prior to the onset of the Asian summer monsoon, as observed in the inter-annual variations of Aerosol Optical Depth (AOD) and fire count data from MODIS. Multi-year (2007-2011) analysis of spaceborne lidar measurements, from CALIOP, indicates presence of aerosols mostly within boundary layer, however extending to elevated altitudes to approx. 4 km over northern regions of Indochina, encompassing Myanmar, northern Thailand and southern China. In addition, a strong gradient in aerosol loading and vertical distribution is observed from the relatively clean equatorial conditions to heavy smoke-laden northern regions (greater aerosol extinction and smaller depolarization ratio). Based on column-integrated ground-based measurements from four AERONET locations distributed over Thailand, the regional aerosol loading is found to be significantly absorbing with spectral single scattering albedo (SSA) below 0.91+/-0.02 in the 440-1020 nm range, with lowest seasonal mean SSA (most absorbing aerosol) over the northern location of Chiang Mai (SSA approx. 0.85) during pre-monsoon season. The smoke-laden aerosol loading is found to exhibit a significant diurnal pattern with higher AOD departures during early morning observations relative to late afternoon conditions (peak difference of more than 15% amplitude). Finally, satellite-based aerosol radiative impact is assessed using CERES shortwave Top-of-Atmosphere flux, in conjunction with MODIS AOD. Overall, a consistency in the aerosol-induced solar absorption characteristic is found among selected regions from ground-based sunphotometer-derived spectral SSA retrievals and satellite-based radiative forcing analysis.

Indochina↗

North Atlantic Aerosol Single Scattering Albedos: TARFOX and ACE-2 Results and Their Relation to Radiative Effects Derived from Satellite Optical Depths

Bergstrom and Russell estimated direct solar radiative flux changes caused by atmospheric aerosols over the mid-latitude North Atlantic Ocean under cloud-free and cloudy conditions. They excluded African dust aerosols, primarily by restricting calculations to latitudes 25-60 N. As inputs they used midvisible aerosol optical depth (AOD) maps derived from AVHRR satellite measurements and aerosol intensive properties determined primarily in the 1996 IGAC Troposheric Aerosol Radiative Forcing Observational Experiment (TARFOX). Those aerosol intensive properties, which included optical depth wavelength dependence and spectra of single scattering albedo (SSA) and scattering asymmetry parameter, were also checked against initial properties from the 1997 North Atlantic Aerosol Characterization Experiment (ACE 2). Bergstrom and Russell investigated the sensitivity of their derived flux changes to assumed input parameters, including midvisible AOD, SSA, and scattering asymmetry parameter. Although the sensitivity of net flux change at the tropopause to SSA was moderate over the ocean (e.g., a SSA uncertainty of 0.07 produced a flux-change uncertainty of 21%), the sensitivity over common land surfaces can be much larger. Also, flux changes within and below the aerosol layer, which affect atmospheric stability, heating rates, and cloud formation and persistence, are quite sensitive to aerosol SSA. Therefore, this paper focuses on the question: "What have we learned from TARFOX and ACE 2 regarding aerosol single scattering albedo?" Three techniques were used in TARFOX to determine midvisible SSA. One of these derived SSA as a best-fit parameter in comparing radiative flux changes measured by airborne pyranometer to those computed from aerosol properties. Another technique combined airborne measurements of aerosol scattering and absorption by nephelometer and absorption photometer. A third technique obtained SSA from best-fit complex refractive indices derived by comparing vertical profiles of lidar backscatter, sunphotometer extinction, and relative size distribution. In ACE 2 midvisible SSA was determined both as a best-fit parameter in comparing measured and calculated flux changes at the surface and by combining nephelometer and absorption photometer measurements. The nephelometer/absorption-photometer results were obtained on the ACE 2 ship (10 m asl), at the Sagres, Portugal site at 50 m asl, and also on the Pelican aircraft. This paper presents and compares the TARFOX and ACE 2 SSA results from the above techniques for different situations (e.g., marine vs continental flows, "clean" vs polluted conditions). It also discusses the strengths and limitations of the techniques, including whether they describe the aerosol in its ambient state or as perturbed by sampling processes; whether they describe the aerosol at the surface, as a function of altitude, or integrated over a column; the ease of acquiring representative data sets; results obtained in tests of consistency with radiative flux changes, and the likelihood of various artifacts and errors.

Russell, P. B.↗

Studies of optical and chemical properties of aged and fresh biomass burning absorbing aerosols for climate models

Particulate emissions from burning fuels from sub-Saharan Africa is currently poorly characterized. With increasing population and industrialization, emissions are expected to grow. Optical methods for measuring light absorption in the ultraviolet (UV) and visible (vis) regions of the spectrum are crucial for understanding the optical properties of BB aerosols (Bond and Bergstrom, 2006; Lack and Cappa, 2010; Moschos et al., 2021). One such instrument is the dual-spot AE33 model aethalometer is a common filter-based instrument that can be used to measure aerosol absorption properties (Hansen et al., 1984). This instrument has many figures of merit; however, the method's limitations include potential biases from scattering within the filter material, multiple scattering effects of the particles, filter loading (i.e. particle shadowing), and the need for wavelength-specific correction factors (Cλ), which depend on accurate intercomparison with other in situ techniques (Bond et al., 1999; Collaud Coen et al., 2010). This work aims to: 1. Optically characterize BB aerosol generated from African fuel 2. Correct the aethalometer at multiple wavelengths 3. Parametrize these correction factors. 4. Combusting the same fuels with two difference tube furnace systems assess the general applicability of this flexible means of producing BB aerosol. This was accomplished by conducting laboratory studies at Los Alamos National Laboratory (LANL) and North Carolina A&T State University (NCA&T), where aethalometer measurements were compared to in situ optical measurements. Mass cross sections of BB aerosol from these under-studied fuels will be determined along with their wavelength dependence.

09 BIOMASS FUELS↗

Leveraging machine learning to enhance aerosol classification using Single-Particle Mass Spectrometry

Advancing automated classification of atmospheric aerosols from Single-Particle Mass Spectrometry (SPMS) data remains challenging due to overlapping ion signatures, compositional diversity, and limited labeled data. This study evaluates supervised and semi-supervised learning frameworks to enhance aerosol identification by jointly leveraging labeled and unlabeled spectra. Four models were compared: a supervised Support Vector Machine (SVM), a self-training SVM, a stacked autoencoder classifier, and a stacked autoencoder trained using a temporal-ensembling Mean Teacher approach. All models achieved high and stable accuracies (90.0 %–91.1 %), surpassing previous results on the same dataset (87 %) and matching the performance of state-of-the-art deep learning methods. Despite small global metric differences (≤ 1 %), semi-supervised variants yielded up to 5 %–10 % improvements for compositionally rare particle types – such as soot (0.77 % of spectra, F1-score: 0.93–0.97) and hazelnut pollen (0.98 % of spectra, F1-score: 0.97–1.00) – equating to roughly ∼ 187 additional correctly classified spectra. These gains are scientifically significant, as such rare particles exert disproportionate influence on radiative absorption and ice nucleation processes; their improved detection reduces modeled uncertainties in aerosol absorption optical depth and mixed-phase cloud ice nucleation rates. The models' residual misclassifications (≈ 9 %) largely arise from true spectral overlap among chemically adjacent species (e.g., Na- vs. K-feldspar, coated vs. uncoated feldspars), reflecting physical compositional continuity rather than algorithmic error. Collectively, these findings demonstrate that leveraging unlabeled data to learn robust spectral representations and refine classification enhances both fidelity and interpretability, bridging data-driven analysis with aerosol–climate process understanding.

54 ENVIRONMENTAL SCIENCES↗

Modeling the Relationships Between Aerosol Properties and the Direct and Indirect Effects of Aerosols on Climate

Aerosols may affect climate directly by scattering and absorbing visible and infrared energy, They may also affect climate indirectly by modifying the properties of clouds through microphysical processes, and by altering abundances of radiatively important gases through heterogeneous chemistry. Researchers understand which aerosol properties control the direct effect of aerosols on the radiation budget. Unfortunately, despite an abundance of data on certain types of aerosols, much work remains to be done to determine the values of these properties. For instance we have little idea about the global distribution, seasonal variation, or interannual variability of the aerosol optical depth. Also we do not know the visible light absorption properties of tropical aerosols which may contain much debris from slash and burn agriculture. A positive correlation between aerosol concentrations and albedos of marine stratus clouds is observed, and the causative microphysics is understood. However, models suggest that it is difficult to produce new particles in the marine boundary layer. Some modelers have suggested that the particles in the marine boundary layer may originate in the free troposphere and be transported into the boundary layer. Others argue that the aerosols are created in the marine boundary layer. There are no data linking aerosol concentration and cirrus cloud albedo, and models suggest cirrus properties may not be very sensitive to aerosol abundance. There is clear evidence of a radiatively significant change in the global lower stratospheric ozone abundance during the past few decades. These changes are caused by heterogeneous chemical reactions occurring on the surfaces of particles. The rates of these reactions depend upon the chemical composition of the particles. Although rapid advances in understanding heterogeneous chemistry have been made, much remains to be done.

Toon, Owen B.↗

Online monitoring of lanthanide species with combined spectroscopy in flowing aqueous aerosol systems

Combined spectroscopic analysis through absorption and laser-induced breakdown spectroscopy (LIBS) was used to monitor Nd and Pr concentrations in a flowing aqueous system. A unique, online sampling approach was employed that allowed for an approximately closed analysis loop of liquids from a reservoir. Absorption spectroscopy was performed with an optical flow cell, and LIBS was performed on an aerosol stream. Multivariate calibrations based on combined absorption and LIBS signals were built for Nd and Pr and then used to monitor concentrations in mixed solutions in a series of spiking tests. In these tests, the concentrations of Nd and Pr in solution were intermittently changed while spectroscopic signals were monitored in real-time. The combined spectroscopic signals and multivariate models were successful in monitoring changing concentrations of lanthanide species with high accuracy and minimal latency. Root-mean squared error of predictions were 0.015 mol L −1 and 0.019 mol L −1 for Nd and Pr respectively, and these lanthanides were able to be monitored to an accuracy of < 0.2 wt%. This work demonstrates both the capabilities of a sampling system for online analysis of liquids and the capabilities of multimodal spectroscopic characterization for real-time, continuous tracking of species in potentially hazardous liquid systems.

absorbance spectroscopy↗

Global Aerosol Climatology Project: An Update

This paper outlines the methodology of interpreting channe1 1 and 2 AVHRR (Advanced Very High Resolution Radiometer) radiance data over the oceans and describes a detailed analysis of the sensitivity of monthly averages of retrieved aerosol parameters to the assumptions made in different retrieval algorithms. The analysis is based on using real AVHRR data and exploiting accurate numerical techniques for computing single and multiple scattering and spectral absorption of light in the vertically inhomogeneous atmospheric-ocean system. We show that two-channel algorithms can be expected tp provide significantly more biased retrievals of the aerosol optical thickness than one-channel algorithms and that imperfect cloud screening and calibration uncertainties are by far the largest sources of errors in the retrieved aerosol parameters. Both underestimating and overestimating aerosol absorption as well as the potentially strong variability of the real part of the aerosol refractive index may lead to regional and/or seasonal biases in optical thickness retrievals. The Angstrom exponent appears to be the most invariant aerosol size characteristic and should be retrieved along with optical thickness as the second aerosol parameter.

Mishchenko, Michael I.↗

Extinction of Laser Light Due to Arctic Haze Final Campaign Report

Recent changes in emission patterns may have altered the historical stability of light attenuation strengths within the Arctic and, more specifically, the polar dome. While there have been decades of past and ongoing research on how atmospheric constituents, such as aerosols, affect light absorption, the bulk of this work is focused on the visible region. In recent years, there has been renewed interest in understanding laser light propagation at wavelengths such as 1 and 2 µm in this area. There is a need to evaluate how specific environmental parameters affect the propagation of light in this wavelength region, in particular: the extinction, scattering, and absorption coefficients, and how they relate to particle concentration; cn 2 and refractive index variations. Seasonally dependent variations in particle concentrations and compositions introduce different absorption and scattering characteristics that, in conjunction with varying temperatures, index-of-refraction variations, and wind, can result in laser beam focus and irradiance degradation. Understanding the fundamental influence of these parameters with respect to the propagation of light across a wide spectral band could lead to new insights about the minimal required datastreams required to provide accurate light propagation forecasting.

54 ENVIRONMENTAL SCIENCES↗