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This paper presents cirrus cloud observations made with the High Spectral Resolution Lidar (HSRL) and the Volume Imaging Lidar (VIL). The HSRL was redesigned to use an iodine absorption filter in place of the Fabry-Perot etalon that was used for spectral separation of the aerosol and molecular lidar returns. These modifications, which improve both sensitivity and calibration stability, are described.
Dust optical properties over North Africa and the Arabian Peninsula are extracted from the quality assured multi-year datasets obtained at 14 sites of the Aerosol Robotic Network (AERONET). We select the data with (a) large aerosol optical depth (AOD >= 0.4 at 440 nm) and (b) small Angstrom exponent (A(sub ext)<= 0.2) for retaining high accuracy and reducing interference of non-dust aerosols. The result indicates that the major fraction of high aerosol optical depth days are dominated by dust over these sites even though it varies depending on location and time. We have found that the annual mean and standard deviation of single scattering albedo, asymmetry parameter, real refractive index, and imaginary refractive index for Saharan and Arabian desert dust is 0.944 +/- 0.005, 0.752 +/- 0.014, 1.498 +/- 0.032, and 0.0024 +/- 0.0034 at 550 nm wavelength, respectively. Dust aerosol selected by this method is less absorbing than the previously reported values over these sites. The weaker absorption of dust from this study is consistent with the studies using remote sensing techniques from satellite. These results can help to constrain uncertainties in estimating global dust shortwave radiative forcing.
Volcanoes are natural phenomena that have global environmental impacts. Satellite remote sensing can help classify volcanic eruptions and track the dispersion of emissions. We assess multiple volcanic eruptions in Iceland (Eyjafjallajökull 2010, Grímsvötn 2011 and Holuhraun 2014-2015), using space-borne observations to infer information about the geological dynamics of each volcano and the properties and evolution of plume particles. We derive qualitative constraints on plume particle size, shape and light-absorption characteristics from Multi-angle Imaging SpectroRadiometer (MISR) space-borne imagery. With the MISR Research Algorithm (RA), we distinguish sulfate/water-dominated volcanic plumes from Holuhraun and ash-dominated plumes from Eyjafjallajökull and Grímsvötn, and even identify subtler changes in ash particle size and light-absorption within plumes. Additionally, plume heights are retrieved geometrically from MISR. These are combined with surface thermal anomalies from the MODerate resolution Imaging Spectroradiometer (MODIS) and SO2 concentrations derived from the Ozone Monitoring Instrument (OMI) to synthesize eruption remote-sensing chronologies. Signals related to differences in particle properties are identified and linked to evolving magma composition at Eyjafjallajökull. The results illustrate the potential to distinguish qualitative differences in eruptive magma composition based on particle light absorption and plume profile from remote-sensing. For the sulfate-rich Holuhraun plumes, the influence of aerosol hygroscopic growth during transport is inferred from such data. Three processes appear to dominate plume evolution in Iceland: downwind aerosol formation; particle hydration; and particle deposition. This work demonstrates enhanced MISR capabilities, and more generally, remote-sensing analysis that can be applied globally, especially where suborbital volcano observations are limited or entirely absent.
Global distributions of albedo susceptibility for areas covered by liquid clouds are presented for 4 months in 2005. The susceptibility estimates are based on expanded definitions presented in a companion paper and include relative cloud droplet number concentration (CDNC) changes, perturbations in cloud droplet asymmetry parameter and single-scattering albedo, atmospheric/surface effects, and incorporation of the full solar spectrum. The cloud properties (optical thickness and effective radius) used as input in the susceptibility calculations come from MODIS Terra and Aqua Collection 5 gridded data. Geographical distributions of susceptibility corresponding to absolute ( absolute cloud susceptibility ) and relative ( relative cloud susceptibility ) CDNC changes are markedly different indicating that the detailed nature of the cloud microphysical perturbation is important for determining the radiative forcing associated with the first indirect aerosol effect. However, both types of susceptibility exhibit common characteristics such as significant reductions when perturbations in single-scattering properties are omitted, significant increases when atmospheric absorption and surface albedo effects are ignored, and the tendency to decrease with latitude, to be higher over ocean than over land, and to be statistically similar between the morning and afternoon MODIS overpasses. The satellite-based susceptibility analysis helps elucidate the role of present-day cloud and land surface properties in indirect aerosol forcing responses. Our realistic yet moderate CDNC perturbations yield forcings on the order of 1-2 W/sq m for cloud optical property distributions and land surface spectral albedos observed by MODIS. Since susceptibilities can potentially be computed from model fields, these results have practical application in assessing the reasonableness of model-generated estimates of the aerosol indirect radiative forcing.
Smoke aerosol, organic and black carbon particles suspended in the air, can absorb and reflect solar radiation to space, i.e., direct radiative forcing. Depending on the ratio of scattering to absorption, and the surface spectral properties, the net smoke effect can be warming or cooling of the climate system. Data from the Airborne Visible/Infrared Imaging Spectrometer (AVIRIS) flown on the ER-2 at altitude of 20km, and of the AERONET ground based sun/sky radiometers are used to assess the smoke aerosol optical thickness over the land and the direct radiative forcing at the top of the atmosphere and at ground level, respectively. The data are collected during the Smoke, Clouds, and Radiation - Brazil (SCAR-B) experiment. In contrast to model results of the smoke effect, we show using the AVIRIS data, that even though the surface albedo is high (0.17 - average on the solar spectrum) and the smoke single scattering albedo is low (0.88), smoke does increase the instantaneous reflectance of sunlight to space by 30-40 W/m2 for an increase in the smoke optical thickness of 0.5. The AERONET data are used to derive, simultaneously, the effect of smoke on the downward radiation. Models using spectrally averaged smoke optical properties and averaged surface reflectance, predicted very small smoke forcing. The reason is that smoke is mainly opaque in short wavelengths (e.g.<0.7 micron) while the surface is mainly bright in longer wavelengths (>0.7 micron). Modeling the effect of smoke on climate forcing cannot be done using the spectrally average properties. It requires the knowledge of the smoke and surface spectral properties.
Smoke aerosol, organic and black carbon particles suspended in the air, are capable to absorb and reflect solar radiation to space - direct radiative forcing. Depending on the ratio of scattering to absorption, and on the surface spectral properties, the net smoke effect can be warming or cooling of the climate system. Data from the AVIRIS spectrometer flown on the ER-2 at altitude of 20 km, and of the AERONET ground based sun/sky radiometers are used to assess the smoke aerosol optical thickness over the land and the direct radiative forcing at the top of the atmosphere and at ground level, respectively. The data are collected during the SCAR-B experiment in Brazil. In contrast to model results of the smoke effect, we show using the AVIRIS data, that even though the surface albedo is high (0.17 - average on the solar spectrum) and the smoke single scattering albedo is low (0.88), smoke does increase the instantaneous reflectance of sunlight to space by 30-40 W/m(exp 2) for an increase in the smoke optical thickness of 0.5. The AERONET data are used to derive, simultaneously, the effect of smoke on the downward radiation. Models using spectrally averaged smoke optical properties and averaged surface reflectance, predicted very small smoke forcing. The reason is that smoke is mainly opaque in short wavelengths (e.g.< 0.7 micron) while the surface is mainly bright in longer wavelengths (> 0.7 micron). Modeling the effect of smoke on climate forcing cannot be done using the spectrally average properties. It requires the knowledge of the smoke and surface spectral properties.
This work relates to the development of sensors that measure specific aerosol properties. These properties are in the form of integrated moment distributions, i.e., total surface area, total mass, etc., or mathematical combinations of these moment distributions. Specifically, the innovation involves two fundamental features: a computational tool to design and optimize such sensors and the embodiment of these sensors in actual practice. The measurement of aerosol properties is a problem of general interest. Applications include, but are not limited to, environmental monitoring, assessment of human respiratory health, fire detection, emission characterization and control, and pollutant monitoring. The objectives for sensor development include increased accuracy and/or dynamic range, the inclusion in a single sensor of the ability to measure multiple aerosol properties, and developing an overall physical package that is rugged, compact, and low in power consumption, so as to enable deployment in harsh or confined field applications, and as distributed sensor networks. Existing instruments for this purpose include scattering photometers, direct-reading mass instruments, Beta absorption devices, differential mobility analyzers, and gravitational samplers. The family of sensors reported here is predicated on the interaction of light and matter; specifically, the scattering of light from distributions of aerosol particles. The particular arrangement of the sensor, e.g. the wavelength(s) of incident radiation, the number and location of optical detectors, etc., can be derived so as to optimize the sensor response to aerosol properties of practical interest. A key feature of the design is the potential embodiment as an extremely compact, integrated microsensor package. This is of fundamental importance, as it enables numerous previously inaccessible applications. The embodiment of these sensors is inherently low maintenance and high reliability by design. The novel and unique features include the underlying computational underpinning that allows the optimization for specific applications, and the physical embodiment that affords the construction of a compact, durable, and reliable integrated package. The advantage appears in the form of increased accuracy relative to existing instruments, and the applications enabled by the physical attributes of the resulting configuration
Abstract. From June to October, southern Africa produces one-third of the global biomass burning (BB) emissions by widespread fires. BB aerosols are transported westward over the south-eastern Atlantic with the mid-tropospheric winds, resulting in significant radiative effects. Ascension Island (ASI) is located midway between Africa and South America. From June 2016 to October 2017, a 17-month in situ observation campaign on ASI found a low single-scattering albedo (SSA) as well as a high mass absorption cross-section of black carbon (MACBC), demonstrating the strong absorbing marine boundary layer in the south-eastern Atlantic. Here we investigate the monthly variations of critical optical properties of BB aerosols, i.e. SSA and MACBC, during the BB seasons and the driving factors behind these variations. Both SSA and MACBC increase from June to August and decrease in September and October. The average SSA during the BB seasons is 0.81 at 529 nm wavelength, with the highest mean ∼ 0.85 in October and the lowest ∼ 0.78 in August. The absorption enhancement (Eabs) derived from the MACBC shows similar trends with SSA, with the average during the whole of the BB seasons at ∼ 1.96 and ∼ 2.07 in 2016 and 2017, respectively. As the Eabs is higher than the ∼ 1.5 commonly adopted value by climate models, this result suggests the marine boundary layer in the south-eastern Atlantic is more absorbing than model simulations. We find the enhanced ratio of BC to CO (ΔBC/ΔCO, equal to BC/ΔCO as the BC background concentration is considered to be 0) is well correlated with SSA and MACBC, providing a simple way to estimate the aerosol optical characteristics in the south-eastern Atlantic. The exponential function we proposed can approximate SSA and MACBC with BC/ΔCO, and when BC/ΔCO is small it can capture the rapid growth of SSA as BC/ΔCO decreases. BC/ΔCO is influenced by combustion conditions and aerosol scavenging. 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/ΔCO from June to August is likely to be caused by burning becoming more flaming. The reduction in the water content of fuels may be responsible for the change in the burning conditions from June to August. The decrease in BC/ΔCO in September and October may be caused by two factors, one being a lower proportion of flaming conditions, possibly associated with a decrease in mean surface wind speed in the burning area, and the other being an increase in precipitation in the BB transport pathway, leading to enhanced aerosol scavenging, which ultimately results in an increase in SSA and MACBC.
Abstract. While gas-phase reactions are well established to have significant impacts on the mass concentration, chemical composition, and optical properties of secondary organic aerosol (SOA), the aqueous-phase aging of SOA remains poorly understood. In this study, we performed a series of long-duration photochemical aging experiments to investigate the evolution of the composition and light absorption of the aqueous SOA (aqSOA) from guaiacyl acetone (GA), a semivolatile phenolic carbonyl that is common in biomass burning smoke. The aqSOA was produced from reactions of GA with hydroxyl radical (•OH-aqSOA) or a triplet excited state of organic carbon (3C∗-aqSOA) and was then photoaged in water under conditions that simulate sunlight exposure in northern California for up to 48 h. The effects of increasing aqueous-phase •OH or 3C∗ concentration on the photoaging of the aqSOA were also studied. High-resolution aerosol mass spectrometry (HR-AMS) and UV–Vis spectroscopy were utilized to characterize the composition and the light absorptivity of the aqSOA and to track their changes during aging. Compared to •OH-aqSOA, the 3C∗-aqSOA is produced more rapidly and shows less oxidation, a greater abundance of oligomers, and higher light absorption. Prolonged photoaging promotes fragmentation and the formation of more volatile and less light-absorbing products. More than half of the initial aqSOA mass is lost, and substantial photobleaching occurs after 10.5 h of prolonged aging under simulated sunlight illumination for 3C∗-aqSOA and 48 h for •OH-aqSOA. By performing positive matrix factorization (PMF) analysis of the combined HR-AMS and UV–Vis spectral data, we resolved three generations of aqSOA with distinctly different chemical and optical properties. The first-generation aqSOA shows significant oligomer formation and enhanced light absorption at 340–400 nm. The second-generation aqSOA is enriched in functionalized GA species and has the highest mass absorption coefficients in 300–500 nm, while the third-generation aqSOA contains more fragmented products and is the least light absorbing. These results suggest that intermediately aged phenolic aqSOA is more light absorbing than other generations, and that the light absorptivity of phenolic aqSOA results from a competition between brown carbon (BrC) formation and photobleaching, which is dependent on aging time. Although photoaging generally increases the oxidation of aqSOA, a slightly decreased O/C of the •OH-aqSOA is observed after 48 h of prolonged photoaging with additional •OH exposure. This is likely due to greater fragmentation and evaporation of highly oxidized compounds. Increased oxidant concentration accelerates the transformation of aqSOA and promotes the decay of BrC chromophores, leading to faster mass reduction and photobleaching. In addition, compared with •OH, photoaging by 3C∗ produces more low-volatility functionalized products, which counterbalances part of the aqSOA mass loss due to fragmentation and evaporation.
Black carbon (BC) plays an important role in the climate system because of its strong warming effect, yet the magnitude of this effect is highly uncertain owing to the complex mixing state of aerosols. Here we build a unified theoretical framework to describe BC’s mixing states, linking dynamic processes to BC coating thickness distribution, and show its self-similarity for sites in diverse environments. The size distribution of BC-containing particles is found to follow a universal law and is independent of BC core size. A new mixing state module is established based on this finding and successfully applied in global and regional models, which increases the accuracy of aerosol climate effect estimations. Our theoretical framework links observations with model simulations in both mixing state description and light absorption quantification.
The system control and signal conditioning electronics of the NASA three laser airborne differential absorption lidar (DIAL) system are described. The multipurpose DIAL system was developed for the remote measurement of gas and aerosol profiles in the troposphere and lower stratosphere. A brief description and photographs of the majority of electronics units developed under this contract are presented. The precision control system; which includes a master control unit, three combined NASA laser control interface/quantel control units, and three noise pulse discriminator/pockels cell pulser units; is described in detail. The need and design considerations for precision timing and control are discussed. Calibration procedures are included.
The effects of the atmosphere on propagating radiation must be known in order to calibrate an in orbit sensor using ground based measurements. A set of model atmosphere parameters, applicable to the White Sands (New Mexico) area is defined with particular attention given to those parameters which are required as input to the Herman Code. The radial size distribution, refractive index, vertical distribution, and visibility of aerosols are discussed as well as the molecular absorbers in the visible and near IR wavelength which produce strong absorption lines. Solar irradiance is also considered.
This paper describes the airborne differential absorption lidar (DIAL) system developed at the NASA Langley Research Center for remote measurement of water vapor (H2O) and aerosols in the lower atmosphere. The airborne H2O DIAL system was flight tested aboard the NASA Wallops Flight Facility (WFF) Electra aircraft in three separate field deployments between 1989 and 1991. Atmospheric measurements were made under a variety of atmospheric conditions during the flight tests, and several modifications were implemented during this development period to improve system operation. A brief description of the system and major modifications will be presented, and the most significant atmospheric observations will be described.
Remote sensing of aerosol over land, from MODIS will be based on dark targets using mid-IR channels 2.1 and 3.9 micron. This approach was developed by Kaufman et al (1997), who suggested that dark surface reflectance in the red (0.66 micron -- rho(sub 0.66)) channel is half of that at 2.2 micron (rho(sub 2.2)), and the reflectance in the blue (0.49 micron - rho(sub 0.49)) channel is a quarter of that at 2.2 micron. Using this relationship, the surface reflectance in the visible channels can be predicted within Delta.rho(sub 0.49) approximately Delat.rho(sub 0.66) approximately 0.006 from rho(sub 2.2) for rho(sub 2.2) <= 0.10. This was half the error obtained using the 3.75 micron and corresponds to an error in aerosol optical thickness of Delat.tau approximately 0.06. These results, though applicable to several biomes (e.g. forests, and brighter lower canopies), have only been tested at one view angle - the nadir (theta = 0 deg). Considering the importance of the results in remote sensing of aerosols over land surfaces from space, we are validating the relationships for off-nadir view angles using Cloud Absorption Radiometer (CAR) data. The CAR data are available for channels between 0.3 and 2.3 micron and for different surface types and conditions: forest, tundra, ocean, sea-ice, swamp, grassland and over areas covered with smoke. In this study we analyzed data collected during the Smoke, Clouds, and Radiation - Brazil (SCAR-B) experiment to validate Kaufman et al.'s (1997) results for non-nadir view angles. We will show the correlation between rho(sub 0.472), rho(sub 0.675), and rho(sub 2.2) for view angles between nadir (0 deg) and 55 deg off-nadir, and for different viewing directions in the backscatter and forward scatter directions.
Environmental implications of climate change are complex and exhibit regional variations both within and between the polar regions. The increase of solar UV radiation flux over Antarctica due to stratospheric ozone depletion creates the optimal conditions for photochemical reactions on the snow. Modeling, laboratory, and indirect field studies suggest that snowpack process release gases to the atmosphere that can react on sea salt particles in remote regions such as Antarctica, modifying aerosol composition and physical properties of aerosols. Here, we present evidence of photochemical processing in West Antarctica aerosols using microscopic and chemical speciation of individual atmospheric particles. Individual aerosol particles collected at the Brazilian module Criosfera 1 were analyzed by scanning transmission X-ray microscopy with near edge X-ray absorption fine structure spectroscopy (STXM/NEXAFS) combined with computer controlled scanning electron microscopy (CCSEM) with energy-dispersive X-ray (EDX) microanalysis. The displacement of chlorine relative to sodium was observed over most of the sea salt particles. Particles with a chemical composition consistent with NaCl-NO3 contributed up to 30% of atmospheric particles investigated. Overall, this study provides evidence that the snowpack and particulate nitrate photolysis should be considered in dynamic partition equilibrium in the troposphere. Finally, these findings may assist in reducing modeling uncertainties and present new insights into the aerosol chemical composition in the polar environment.
This study develops an algorithm for representing detailed spectral features of vegetation albedo based on Moderate Resolution Imaging Spectrometer (MODIS) observations at 7 discrete channels, referred to as the MODIS Enhanced Vegetation Albedo (MEVA) algorithm. The MEVA algorithm empirically fills spectral gaps around the vegetation red edge near 0.7 micrometers and vegetation water absorption features at 1.48 and 1.92 micrometers which cannot be adequately captured by the MODIS 7 channels. We then assess the effects of applying MEVA in comparison to four other traditional approaches to calculate solar fluxes and aerosol direct radiative forcing (DRF) at the top of atmosphere (TOA) based on the MODIS discrete reflectance bands. By comparing the DRF results obtained through the MEVA method with the results obtained through the other four traditional approaches, we show that filling the spectral gap of the MODIS measurements around 0.7 micrometers based on the general spectral behavior of healthy green vegetation leads to significant improvement in the instantaneous aerosol DRF at TOA (up to 3.02Wm(exp -2) difference or 48% fraction of the aerosol DRF, .6.28Wm(exp -2), calculated for high spectral resolution surface reflectance from 0.3 to 2.5 micrometers for deciduous vegetation surface). The corrections of the spectral gaps in the vegetation spectrum in the near infrared, again missed by the MODIS reflectances, also contributes to improving TOA DRF calculations but to a much lower extent (less than 0.27Wm(exp -2), or about 4% of the instantaneous DRF). Compared to traditional approaches, MEVA also improves the accuracy of the outgoing solar flux between 0.3 to 2.5 micrometers at TOA by over 60Wm(exp -2) (for aspen 3 surface) and aerosol DRF by over 10Wm(exp -2) (for dry grass). Specifically, for Amazon vegetation types, MEVA can improve the accuracy of daily averaged aerosol radiative forcing in the spectral range of 0.3 to 2.5 micrometers at equator at the equinox by 3.7Wm(exp -2). These improvements indicate that MEVA can contribute to regional climate studies over vegetated areas and can help to improve remote sensing-based studies of climate processes and climate change.
Conference presentation for 38th Annual International Pittsburgh Coal Conference, Virtual, September 20–23, 2021. To better assess mitigation strategies for aerosol reduction to extend solvent life, the University of North Dakota Energy & Environmental Research Center (EERC) installed a pilot-scale CO 2 absorption system at a lignite-fired plant in central North Dakota. The pilot-scale system was operated using both commercial KS-1™ solvent and advanced KS-21™ solvent provided by Mitsubishi Heavy Industries (MHI). MHI’s proprietary amine emission reduction unit (AERU™) technology was installed downstream of the absorber columns to reduce solvent losses by recovering amines at the system outlet. Fine particulate loading was measured throughout the capture system with and without a WESP operating and using both solvents. Captured particulate was brought back to the EERC to be analyzed for chemical composition and to be examined by scanning electron microscopy for particulate structure. These variables were then correlated to performance of particulate control devices in reducing aerosol formation and solvent losses.
The MODIS Dark Target aerosol algorithm over Ocean (DT-O) uses spectral reflectance in the visible, near-IR and SWIR wavelengths to determine aerosol optical depth (AOD) and Angstrom Exponent (AE). Even though DT-O does have "dust-like" models to choose from, dust is not identified a priori before inversion. The "dust-like" models are not true "dust models" as they are spherical and do not have enough absorption at short wavelengths, so retrieved AOD and AE for dusty regions tends to be biased. The inference of "dust" is based on postprocessing criteria for AOD and AE by users. Dust aerosol has known spectral signatures in the near-UV (Deep blue), visible, and thermal infrared (TIR) wavelength regions. Multiple dust detection algorithms have been developed over the years with varying detection capabilities. Here, we test a few of these dust detection algorithms, to determine whether they can be useful to help inform the choices made by the DT-O algorithm. We evaluate the following methods: The multichannel imager (MCI) algorithm uses spectral threshold tests in (0.47, 0.64, 0.86, 1.38, 2.26, 3.9, 11.0, 12.0 micrometer) channels and spatial uniformity test [Zhao et al., 2010]. The NOAA dust aerosol index (DAI) uses spectral contrast in the blue channels (412nm and 440nm) [Ciren and Kundragunta, 2014]. The MCI is already included as tests within the "Wisconsin" (MOD35) Cloud mask algorithm.