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Shock-induced devolatization of calcium sulfate and implications for K-T extinctions

Calcium sulfate devolatization during the impact at Chicxulub, Mexico and dispersal in the stratosphere of the resultant sulfuric acid aerosol have been suggested as a possible mechanism for the Cretaceous-Tertiary extinctions. In this paper, we investigated two shock-induced devolatization reactions of calcium sulfate up to 42 GPa in the laboratory: CaSO4 + SiO2 yields CaSiO3 + SO3(degassed) and CaSO4 yields CaO + SO2(degassed) + 1/2 O2(degassed). We found both to proceed to a much less extent than calculated by equilibrium thermodynamic calculations. Reaction products are found to be 10(exp -2) times those calculated for equilibrium. Consequently our estimate of the amount of sulfur oxides degassed into the atmosphere from shock devolatization of CaS04 in the Chicxulub lithographic section (6x10(exp 15)-2x10(exp 16)g in sulfur mass) is lower by a factor of 70 to 400 than previous estimates; the related environmental stress arising from the resultant global cooling of approximately 4 K and fallout of acid rain does not appear to suffice to explain the widespread K-T extinctions.

Chen, Guangqing↗

Aerosol Measurements by the Globally Distributed Micro Pulse Lidar Network

Full time measurements of the vertical distribution of aerosol are now being acquired at a number of globally distributed MP (micro pulse) lidar sites. The MP lidar systems provide full time profiling of all significant cloud and aerosol to the limit of signal attenuation from compact, eye safe instruments. There are currently eight sites in operation and over a dozen planned. At all sited there are also passive aerosol and radiation measurements supporting the lidar data. Four of the installations are at Atmospheric Radiation Measurement program sites. The network operation includes instrument operation and calibration and the processing of aerosol measurements with standard retrievals and data products from the network sites. Data products include optical thickness and extinction cross section profiles. Application of data is to supplement satellite aerosol measurements and to provide a climatology of the height distribution of aerosol. The height distribution of aerosol is important for aerosol transport and the direct scattering and absorption of shortwave radiation in the atmosphere. Current satellite and other data already provide a great amount of information on aerosol distribution, but no passive technique can adequately resolve the height profile of aerosol. The Geoscience Laser Altimeter System (GLAS) is an orbital lidar to be launched in early 2002. GLAS will provide global measurements of the height distribution of aerosol. The MP lidar network will provide ground truth and analysis support for GLAS and other NASA Earth Observing System data. The instruments, sites, calibration procedures and standard data product algorithms for the MPL network will be described.

Spinhirne, James↗

MPL-Net Measurements of Aerosol and Cloud Vertical Distributions at Co-Located AERONET Sites

In the early 1990s, the first small, eye-safe, and autonomous lidar system was developed, the Micropulse Lidar (MPL). The MPL acquires signal profiles of backscattered laser light from aerosols and clouds. The signals are analyzed to yield multiple layer heights, optical depths of each layer, average extinction-to-backscatter ratios for each layer, and profiles of extinction in each layer. In 2000, several MPL sites were organized into a coordinated network, called MPL-Net, by the Cloud and Aerosol Lidar Group at NASA Goddard Space Flight Center (GSFC) using funding provided by the NASA Earth Observing System. tn addition to the funding provided by NASA EOS, the NASA CERES Ground Validation Group supplied four MPL systems to the project, and the NASA TOMS group contributed their MPL for work at GSFC. The Atmospheric Radiation Measurement Program (ARM) also agreed to make their data available to the MPL-Net project for processing. In addition to the initial NASA and ARM operated sites, several other independent research groups have also expressed interest in joining the network using their own instruments. Finally, a limited amount of EOS funding was set aside to participate in various field experiments each year. The NASA Sensor Intercomparison and Merger for Biological and Interdisciplinary Oceanic Studies (SIMBIOS) project also provides funds to deploy their MPL during ocean research cruises. All together, the MPL-Net project has participated in four major field experiments since 2000. Most MPL-Net sites and field experiment locations are also co-located with sunphotometers in the NASA Aerosol Robotic Network. (AERONET). Therefore, at these locations data is collected on both aerosol and cloud vertical structure as well as column optical depth and sky radiance. Real-time data products are now available from most MPL-Net sites. Our real-time products are generated at times of AERONET aerosol optical depth (AOD) measurements. The AERONET AOD is used as input to our processing routines, which calculate the aerosol layer top height and extinction profile, and our MPL calibration value. A variety of other data products are available or under development. We present an overview of the MPL-Net project and discuss data products useful to the AERONET community. Results from several sites and field experiments will be presented.

Welton, Ellsworth J.↗

Measurements

To interpret the effects of aerosols and gases on the atmosphere, information on the vertical and horizontal distribution of aerosol particles, their size distributions and concentration of precursor gases is required. Measurements of aerosols and gases at frequent intervals and over vast areas of atmosphere generally involve remote sensing techniques. These techniques depend on the optical properties of the species studied. Optical properties can vary greatly with aerosol size and refractive index. Remote sensing instruments look at light scattering, extinction, depolarization, and reflection. The chemical composition, phase equilibria, surface properties, and photochemical behavior of stratospheric aerosols are not clearly understood or adequately measured by current technologies. Areas are listed which need technology development.

Source record↗

Mapping Aerosol Lidar Ratios Over Ocean Using Constrained Retrievals and A Global Aerosol Model

The current NASA Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) algorithms assign one lidar ratio (i.e., extinction-to-backscatter ratio; LR) value globally for each of the seven tropospheric aerosol types. In a future data products release, the CALIPSO project aims to improve these algorithms through the development of regional and seasonal LR climatologies. In this work, aerosol LRs are inferred through Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) backscatter profiles constrained by collocated aerosol optical depth (AOD) from Aqua Moderate Resolution Imaging Spectroradiometer (MODIS) data. This analysis is subsampled for those profiles that are cloud-free and contain only one CALIOP-classified aerosol type (e.g., marine). The CALIOP profiles are then collocated with aerosol volume fractions obtained through Goddard Chemistry Aerosol Radiation and Transport (GOCART) model simulations. In this presentation, we show that the twelve-year (June 2006-August 2018) mean spatial distributions of inferred aerosol LRs for CALIOP-classified marine aerosols correspond inversely with patterns of GOCART sea salt volume fraction (SSVF). For example, smaller SSVFs (< 65%) and larger LRs (> 55 sr), are found near land masses. This is indicative of the influence of over-land aerosols (e.g., pollution and biomass burning smoke). In the remote oceans (i.e., regions likely less impacted by non-sea salt aerosols), larger SSVFs (> 95%) and smaller LRs (< 25 sr) are found. The developed relationship between the GOCART SSVFs and MODIS AOD constrained LRs (polynomial fit intersect values of ~56 sr for SSVF of 0% and ~21 sr for SSVF of 100%) is used to produce model-assisted climatological LR maps on seasonal scales. Additionally, we show maps of inferred LRs from constrained retrievals using the CALIPSO Ocean Derived Column Optical Depth (ODCOD) product and comparisons with those from the MODIS analyses. The technique demonstrated in this study not only benefits CALIPSO in the near-term, but similar methods can be applied to future spaceborne elastic backscatter lidars with collocated passive sensors, such as those associated with the upcoming NASA Atmosphere Observing System (AOS).

Travis Toth↗

Simultaneous measurement of stratospheric O3, H2O, CH4, and N2O profiles from infrared limb thermal emissions

Thermal emission measurements of the earth's stratospheric limb were made with a cryogenically cooled high-resolution Michelson interferometer on a balloon flight launched from Palestine, TX, on Nov. 6, 1984. Infrared spectra for complete limb sequences were obtained over portions of the 700-1940/cm range with an unapodized spectral resolution of 0.03/cm for tangent heights varying from 13 to 39 km. The observed data from 1125 to 1425/cm have been analyzed for simultaneous measurement of O3, H2O, CH4, and N2O profiles. The analysis employs line-by-line and layer-by-layer radiative-transfer calculations, including curvature and refraction effects. The optimum use of geometric and spectral effects is made to obtain sharply peaked weighting functions. Contributions from stratospheric aerosol are included by measuring the light extinction within the window regions of the observed spectra. The retrieved constituent profiles are compared with measurements made with a variety of techniques by other groups. The comparison shows good agreement with the published data for all gases, indicating the capability of retrieving trace gas profiles from high-resolution thermal emission limb measurements.

Abbas, M. M.↗

Improving the Performance of the OMPS Limb Profiling Instrument in Monitoring Aerosols in the Post-Pinatubo Stratosphere

The OMPS Limb Profiling (LP) instrument was launched on NOAA's Suomi NPP (SNPP) weather satellite in October 2011. The instrument measures limb-scattered radiation in the ultraviolet, visible and NIR wavelengths with high vertical resolution (~2 km) and relatively dense spatial and temporal sampling (several thousand measurements/day covering the entire sunlit globe). These measurements have very high sensitivity to stratospheric aerosols due to long path of the incoming solar photons through the aerosol layer. However, unlike the recently launched ISS/SAGE III that directly measures extinction of solar/lunar radiation by gases and particles along the line of sight (LOS) of the instrument, information content of OMPS LP measurements is complex. It consists of solar radiation singly scattered and attenuated by aerosols, air, and trace gases along the LOS of the instrument, as well as diffuse upwelling radiation from the lower atmosphere that also gets scattered and attenuated into the LOS. To unscramble this complex signal one needs to have good knowledge of aerosol size distribution (ASD) and their complex refractive index. We will describe our recent efforts in constraining the ASD parameters by analyzing in-situ balloon data from Laramie, Wyoming; aerosol microphysical model data from CARMA; and spectral information provided by OMPS LP. We will also discuss our proposed methodology to refine this information by adjusting the microphysical properties of the aerosols to make data from various occultation and scattering instruments internally consistent. This is a generalized version of the technique employed by AERONET in which solar extinction data are combined with scattered radiation measured by the almucantar technique to determine aerosol particle shape, complex refractive index and size distribution. We suggest that such closure studies are essential to develop confidence in space-based data to validate aerosol microphysical models, such as CARMA, and aerosol chemistry- transport models, such as GOCART, and for estimating radiative forcing due to stratospheric aerosols in both volcanic and quiescent time periods.

Bhartia, P. K.↗

Latitude survey of aerosol optical thickness of the El Chichon eruption cloud in May 1983

The results of measurements of the latitudinal distribution of the El Chichon eruption cloud in May 1983 for the latitude range between 71 deg N and 56 deg S are presented. Aerosol optical thicknesses are calculated from solar spectral extinction measurements made with a sunphotometer on board the NASA Convair 990 aircraft. It is shown that the thicknesses vary in the range between 0.12 and 0.01, that a maximum of about 0.12 is found at middle latitudes, and that distinct minima of 0.01-0.02 are observed at 25-deg latitude in both hemispheres. The median radius of particles is found to be between 0.16 micron and 0.18 micron in the northern hemisphere and between 0.11 micron and 0.15 micron in the southern hemisphere. Rough estimates of aerosol mass indicate that about 1.5 megatonnes of aerosol still persisted in the stratosphere between the equator and 25-deg N one year after the eruption.

Shah, G. M.↗

Creating Seasonal Climatologies of Aerosol Lidar Ratios Over Ocean Using MODIS AOD Constrained Retrievals and GOCART Model Simulations

The current CALIPSO algorithms assign one lidar ratio (i.e., extinction-to-backscatter ratio; LR) value globally for each of the seven tropospheric aerosol types. In a future data products release, the CALIPSO project aims to improve these algorithms through the development of regional and seasonal LR climatologies. In this work, aerosol LRs are inferred through CALIOP backscatter profiles constrained by collocated aerosol optical depth (AOD) from Aqua Moderate Resolution Imaging Spectroradiometer (MODIS) data. This analysis is subsampled for those profiles that are cloud-free and contain only one CALIOP-classified aerosol type (e.g., marine). The CALIOP profiles are then collocated with aerosol volume fractions obtained through Goddard Chemistry Aerosol Radiation and Transport (GOCART) model simulations. In this poster, we show twelve-year (June 2006-August 2018) mean spatial distributions of inferred aerosol LRs for CALIOP-classified marine aerosols and how they correspond inversely with patterns of GOCART sea salt volume fraction (SSVF). Near land masses, smaller SSVFs and larger LRs are found (due to the influence of over-land aerosols). In the remote ocean regions (likely less impacted by over-land aerosols), larger SSVFs and smaller LRs are found. The developed relationship between the GOCART model SSVFs and MODIS AOD constrained LRs is used to create model-assisted seasonal LR maps. Additionally, we show maps of inferred LRs from constrained retrievals using the CALIPSO Ocean Derived Column Optical Depth (ODCOD) product and comparisons with those from the MODIS analyses. The technique demonstrated here benefits CALIPSO in the near-term, but similar methods can also be applied to the next generation space-based elastic backscatter lidars with collocated passive sensors, such as those of the upcoming NASA Atmosphere Observing System (AOS).

Travis Toth↗

Influence of Aerosol Embedded in Shallow Cumulus Cloud Fields on the Surface Solar Irradiance

Ubiquitous shallow cumulus clouds are associated with complex variability in surface solar irradiance (SSI). Aerosol embedded in the cloud field typically has a much smaller overall radiative effect, but can significantly perturb the shape of the SSI probability density function (PDF). These perturbations have important implications for several applications that utilize SSI, but are poorly quantified and are the subject of this study. Multiple cases of shallow cumulus cloud fields with embedded aerosol are simulated at the Southern Great Plains Atmospheric Observatory using large eddy simulation (LES). The LES-derived cloud and aerosol fields are then ingested into Monte Carlo three-dimensional (3D) radiative transfer to simulate SSI. We find a variety of perturbations to the SSI PDF that depend on aerosol presence and optical properties. The processes leading to these perturbations include extinction of the direct beam that often increases from the clear-sky region toward cloud edge due to aerosol hygroscopic growth, and scattering of radiation by aerosol into cloud shadows. The ability to predict the SSI PDF in the presence of aerosol is assessed by adding three representative aerosol optical properties into an existing machine learning framework. We show that machine learning accurately predicts the SSI PDF across a wide range of conditions with negligible computational expense. Importance metrics reveal the relatively high influence of aerosol optical properties in making the predictions. These new findings highlight the important role that aerosol plays in SSI variability for highly 3D cloud-aerosol environments and provides a computationally efficient route forward for its simulation.

3D radiative transfer↗

Modeling of growth, evaporation and sedimentation effects on transmission of visible and IR laser beams in artificial fogs

The dense polydisperse aerosol particles in a quiet chamber may spontaneously go through different microphysical processes including gravitational sedimentation, thermal coagulation, and growth or evaporation. In an earlier paper, we presented the results of a parametric study of the combined and separate effects of thermal coagulation and sedimentation on the time dependence of extinction of four visible and IR laser beams traversing an aerosol medium. As a continuation of this series of studies, the separate and combined effects of growth or evaporation and gravitational sedimentation on the time dependence of extinction of the same four visible and IR laser beams traversing in artificial fogs will be reported in this paper. The method of numerically modeling the change of water droplet size distribution with time due to growth/evaporation and the cutoff of larger aerosols due to gravitational sedimentation is described in detail. Factors governing the relative importance of these two processes are discussed. Results of this study show that the relative humidity or ambient temperature is a crucial parameter in determining the optical depth of the water droplet and aerosol media undergoing microphysical processes.

Yue, G. K.↗

Soot Aerosol from Aircraft: Is there Enough to Cause Middle-Latitude Lower Stratospheric Ozone

Soot aerosol from aircraft has been implicated to cause long-term ozone depletion at mid-latitudes in the lower stratosphere at a rate of approx. equals 5%,per decade. During the 1996 SUCCESS field campaign, we sampling aerosols in the exhaust wake of a Boeing 757 aircraft and determined emission indices for sulfuric acid (EIH2SO4=4.8E-2 and 5.7E- 1. g/kgFUEL for 75 and 675 ppm fuel-sulfur, respectively) and soot (EIsoot=7.5E-4 g/kgFUEL). The corresponding fuel-sulfur to H2SO4 conversion efficiency was 25 % and 30%,respctively. Applying the H2SO4 emission index to the 1990 fuel by the world's commercial fleets of 1.3E11 kg, a conversion efficiency of 30% would have led to an annual contribution to the atmospheric sulfur budget by aircraft of 2.E7 kg H2SO4, if the fuels averaged 500 ppmm.The soot emission index given above yielded a 1990 injection of soot aerosol by aircraft of 1.E5 kg. Thus, soot amounts to only one half of one percent of the aerosol generated by aircraft. The fractal nature of soot may increase its actual surface area by about a factor of 10. The findings, however, of (1) 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; and (2) a trend in stratospheric soot loading of approx.6% per year since 1981, similar to the annual increase of aircraft operations since that time, 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 extinction, against the "noise" due to volcanic eruptions, The current single scatter albedo of the stratospheric aerosol is omega = 0.993+/-0.004.

Pueschel, R. F.↗

Near-IR extinction and backscatter coefficient measurements in low- and mid-altitude clouds

Knowledge of the attenuation and backscattering properties of clouds is required to high resolution for several types of optical sensing systems. Such data was obtained in about 15 hours of flights through clouds in the vicinity of Washington, D.C. The flights were mainly through stratocumulus, altocumulus, stratus, and stratus fractus clouds and covered an altitude and temperature range of 300 to 3200 m and -13 to 17 C. Two instruments were flown, each of which measured the backscatter from close range in two range bins to independently determine both the extinction and backscatter coefficients. The extinction and backscatter coefficients can be obtained from the signals in the two channels of each instrument, provided that the aerosol is uniform over the measurement region. When this assumptions holds, the extinction coefficient is derived basically from the ratio of the signal in the two channels; the backscatter coefficient can then be obtained from the signal in either channel.

Sztankay, Z. G.↗

Raman Lidar Measurements of Pinatubo Aerosols over Southeastern Kansas During November-december 1991

The eruptions of the Philippine volcano Pinatubo during June 1991 produced large amounts of stratospheric aerosols that could significantly affect earth's climate as well as trigger stratospheric ozone depletion through heterogeneous chemical reactions. Information regarding the physical and optical properties of these aerosols is required to quantify those effects. By measuring both the elastically backscattered signal and the inelastic signal produced by Raman scattering from nitrogen molecules, Raman lidar can provide some of this information. In this presentation we discuss Raman lidar measurements of the scattering ratio, backscattering, extinction, extinction/backscattering ratio, and optical thickness of the Pinatubo aerosols over southeastern Kansas made on 10 nights during November and December, 1991. The Raman lidar developed at GSFC is a trailer-based system which uses an XeF excimer laser to transmit light at 351 nm. The light backscattered by molecules and aerosols at this wavelength is detected as well as Raman scattered light from water vapor, nitrogen, and oxygen molecules. Since background skylights interfere with the detection of the Raman signals the data discussed in this paper were acquired only at night.

Ferrare, R. A.↗

Aerosol Absorption Retrieval at Ultraviolet Wavelengths in a Complex Environment

We have used total and diffuse UV irradiance measurements from a multi-filter rotating shadow-band radiometer (UVMFR) in order to investigate aerosol absorption in the UV range for a 5-year period in Athens, Greece. This dataset was used as input to a radiative transfer model and the single scattering albedo (SSA) at 368 and 332 nm was calculated. Retrievals from a collocated CIMEL sun photometer were used to evaluate the products and study the absorption spectral behavior of retrieved SSA values. The UVMFR SSA, together with synchronous, CIMEL-derived retrievals of SSA at 440 nm, had a mean of 0.90, 0.87 and 0.83, with lowest values (higher absorption) encountered at the shorter wavelengths. In addition, noticeable diurnal variation of the SSA in all wavelengths is shown, with amplitudes up to 0.05. Strong SSA wavelength dependence is revealed for cases of low Angstrom exponents, accompanied by a SSA decrease with decreasing extinction optical depth, suggesting varying influence under different aerosol composition. However, part of this dependence for low aerosol optical depths is masked by the enhanced SSA retrieval uncertainty. Dust and brown carbon UV absorbing properties were also investigated to explain seasonal patterns.

Kazadzis, Stelios↗

Aerosol Radiative Forcing in Asian Continental Outflow

Aerosols in elevated layers were sampled with FSSP-probes and wire impactors over the Pacific ocean aboard the NASA DC-8 aircraft. Analyses of particle size and morphology identifies two distinctly different aerosol types for cases when the mid-visible extinctions exceed 0.2/km. Smaller sizes (effective radii of 0.2 um) and moderate absorption (mid-visible single scattering albedo of.935) are typical for urban-industrial pollution. Larger sizes (effective radii of 0.7 um) and weak absorption (mid-visible single scattering albedo of 0.985) identify dust. This aerosol classification is in agreement with its origin as determined by airmass back trajectory analysis. Based on lidar vertical profiling, aerosol dominated by dust and urban-industrial pollution above 3km were assigned mid-visible optical depths of 0.50 and 0.27, respectively. Radiative transfer simulations, considering a 50% cloud-cover below the aerosol layers, suggest (on a daily tP C)C> basis) small reductions (-4W/m2) to the energy budget at the top of the atmosphere for both aerosol types. For c' 0 dust, more backscattering of sunlight (weaker solar absorption) is compensated by a stronger greenhouse effect due to larger sizes. Forced reductions to the energy budget at the surface are 12W/m2 for both aerosol types. In contrast, impacts on heating rates within the aerosol layers are quite different: While urban-industrial aerosol warms the layer (at +0.6K/day as solar heating dominates), dust cools (at -0.5K/day as infrared cooling dominates). Sensitivity tests show the dependence of the aerosol climatic impact on the optical depth, particle size, absorptivity, and altitude of the layers, as well as clouds and surface properties. Climatic cooling can be eliminated (1) for the urban-industrial aerosol if absorption is increased to yield a mid-visible single scattering albedo of 0.89, or if the ocean is replaced by a land surface; (2) for the dust aerosol if the effective radius is increased from 0.7 to 1.2 um. The removal of low-level clouds doubles the cooling at the top of the atmosphere to about -8W/m2.

Pueschel, R.↗

Stratospheric aerosols

The current state of information on stratospheric aerosols is reviewed. Aerosol properties such as size, size distribution, composition, refractive index, number density, extinction, optical depth, and single scattering albedo are considered and generalized as much as possible to be representative of the global aerosol in times of volcanic and nonvolcanic (background) periods. Data are presented that show the global distribution of stratospheric aerosols as measured by the stratospheric aerosol and gas experiment (SAGE) satellite system for background and volcanic (post-Mount St. Helens) conditions. In addition, lidar and dustsonde data are presented that show the changes in stratospheric aerosol over an 8-year period.

Mccormick, M. P.↗

Cloud Physics Lidar Optical Measurements During the SAFARI-2000 Field Campaign

In this presentation, we will show new optical data processing results from the Cloud Physics War during SAFARI-2000. Retrieved products include aerosol and cloud layer location and identification, layer optical depths, vertical extinction profiles, and extinction-to-backscatter (S) ratios for 532 and 1064 nm. The retrievals will focus on the persistent and smoky planetary boundary layer and occasional elevated aerosol layers found in southern Africa during August and September 2000.

Hlavka, Dennis L.↗