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Trends in aerosol abundances and distributions

The properties of aerosols that reside in the upper atmosphere are described. Special emphasis is given to the influence these aerosols have on ozone observation systems, mainly through radiative effects, and on ambient ozone concentrations, mainly through chemical effects. It has long been appreciated that stratospheric particles can interfere with the remote sensing of ozone distribution. The mechanism and magnitude of this interference are evaluated. Separate sections deal with the optical properties of upper atmospheric aerosols, long-term trends in stratospheric aerosols, perturbations of the stratospheric aerosol layer by volcanic eruptions, and estimates of the impacts that such particles have on remotely measured ozone concentrations. Another section is devoted to a discussion of the polar stratospheric clouds (PSC's). These unique clouds, recently discovered by satellite observation, are now thought to be intimately connected with the Antarctic ozone hole. Accordingly, interest in PSC's has grown considerably in recent years. This chapter describes what we know about the morphology, physical chemistry, and microphysics of PSC's.

Turco, R. P.↗

A New Raman DIAL Technique for Measuring Stratospheric Ozone in the Presence of Volcanic Aerosols

This paper describes a new lidar scheme to measure stratospheric ozone in the presence of heavy volcanic aerosol loading. The eruptions of the Philippine volcano Pinatubo during June 1991 ejected large amounts of sulfur dioxide into the atmosphere to altitudes of at least 30 km. The resulting aerosols have severely affected the measurements of stratospheric ozone when using traditional Rayleigh differential absorption lidar (DIAL) technique, in which the scattering mechanism is almost entirely Rayleigh and which assumes a small amount or no aerosols. In order to extract an ozone profile in the regions below about 30 km where the Rayleigh lidar returns are contaminated by aerosol scattering from Mt. Pinatubo cloud, we have used a Raman lidar technique, where the scattering mechanism depends solely on molecular nitrogen. In this scheme there is no aerosol scattering component to the backscattered lidar return. Using this technique in conjunction with the Rayleigh DIAL measurement, the GSFC stratospheric ozone lidar has measured ozone profiles between 15 and 50 km during the recently held UARS correlative measurement campaign (February-March 1992) at JPL's Table Mountain Facility in California.

Upendra N. Singh↗

Global Backscatter Experiment (GLOBE) Results: Aerosol Backscatter Global Distribution and Wavelength Dependence

The GLObal Backscatter Experiment (GLOBE) was initiated by NASA in 1986 as an interagency and international research effort to characterize tropospheric backscatter properties. The primary objective of the program is to develop realistic aerosol backscatter inputs for design and simulation studies for NASA's prospective Laser Atmospheric Wind Sounder (LAWS). To achieve this, GLOBE incorporates several different types of aerosol sensors, which operate from a variety of sensor platforms, covering a wide range of spatial and temporal scales, and measure a diverse set of aerosol physical, chemical, and optical properties. The results of this analysis have provided important new information on the life cycles and physicochemical properties of global scale tropospheric aerosol systems. In addition, GLOBE analytical methods will be useful for the Earth Observing System (EOS) and other studies that involve the assimilation of large, complex atmospheric aerosol databases.

Bowdle, David A.↗

Lidar Investigation of Aerosol Pollution Distribution near a Coal Power Plant

Using aerosol lidars with high spatial and temporal resolution with the possibility of real-time data interpretation can solve a large number of ecological problems related to the aerosol-field distribution and variation and the structure of convective flows. Significantly less expensive specialized lidars are used in studying anthropogenic aerosols in the planetary boundary layer. Here, we present results of lidar measurements of the mass-concentration field around a coal-fired power plant with intensive local aerosol sources. We studied the pollution evolution as a function of the emission dynamics and the presence of retaining layers. The technique used incorporates complex analysis of three types of lidar mapping: horizontal map of the aerosol field, vertical cross-section map, and a series of profiles along a selected path. The lidar-sounding cycle was performed for the time of atmosphere's quasi-stationarity.

Mitsev, TS.↗

Simulation of the Pinatubo aerosol cloud in general circulation model

The global transport and dispersion of the Pinatubo aerosol cloud are simulated by means of a high-resolution stratospheric version of the NCAR Community Climate Model (CCM2) with an annual cycle. A passive tracer was injected into the model stratosphere over the Philippine Islands on June 15, and the transport was simulated for 180 d using an accurate semi-Lagrangian advection scheme. The simulated volcanic aerosol cloud initially drifted westward and expanded in longitude and latitude. The bulk of the aerosol cloud dispersed zonally to form a continuous belt in longitude, and remained confined to the tropics, centered near the 20-mb level for the entire 180-d model run, although a small amount was transported episodically into the upper troposphere in association with convective disturbances. Aerosol transported to the troposphere was dispersed within a few weeks into the Northern Hemisphere extratropics. In the Southern Hemisphere, the aerosol was mixed into the region equatorward of the core of the polar night jet during the first 50 d, but penetration into southern polar latitudes was delayed until the final warming in November.

Boville, Byron A.↗

A diagnostic stratospheric aerosol size distribution inferred from SAGE II measurements

An aerosol size distribution model for the stratosphere is inferred based on 5 years of Stratospheric Aerosol and Gas Experiment (SAGE) II measurements of multispectral aerosol and water vapor extinction. The SAGE II aerosol and water vapor extinction data strongly suggest that there is a critical particle radius below which there is a relatively weak dependence of particle number density with size and above which there are few, if any, particles. A segmented power law model, as a simple representation of this dependence, is used in theoretical calculations and intercomparisons with a variety of aerosol measurements including dustsondes, longwave lidar, and wire impactors and shows a consistently good agreement.

Thomason, Larry W.↗

Aerosol characterization in smoke plumes from a wetlands fire

Results are presented from airborne measurements of aerosol mass loading, size distribution, and elemental composition obtained in a smoke plume from a fire at a Florida wildlife refuge. It is found that there was a high concentration of carbon-containing aerosols and salt crystals in the 0.1-0.2 micron size range; the composition and morphology of the aerosols differed with size. Aerosol mass concentrations are used in conjunction with those obtained for CO2 in order to calculate ratios of aerosol and CO2. The ratios are noted to be higher for the smoldering phase of the fire than for its flaming phase.

Woods, David C.↗

The potential effects of volcanic aerosols on cirrus cloud microphysics

The potential impact of volcanic aerosols on nucleation of ice crystals in upper tropospheric cirrus clouds is examined from a microphysical perspective. The sulfuric acid aerosols which form in the stratosphere are presumably transported into the troposphere by sedimentation and tropopause folding. The tropospheric volcanic aerosol size distribution is estimated from 10-micron lidar backscatter and in situ measurements. Microphysical simulations suggest that at temperatures below about -50 C the concentration of ice crystals which nucleate may be as much as a factor of 5 larger when volcanic aerosols are present. The simulations suggest that the presence of volcanic aerosols may increase the net radiative forcing (surface warming) of certain types of cirrus near the tropopause by as much as 8 W/sq m. Further observations are required to determine whether these effects actually occur, and their global impact.

Jensen, Eric J.↗

Aerosol chemistry in GLOBE

This task addresses the measurement and understanding of the physical and chemical properties of aerosol in remote regions that are responsible for aerosol backscatter at infrared wavelengths. Because it is representative of other clean areas, the remote Pacific is of extreme interest. Emphasis is on the determination size dependent aerosol properties that are required for modeling backscatter at various wavelengths and upon those features that may be used to help understand the nature, origin, cycling and climatology of these aerosols in the remote troposphere. Empirical relationships will be established between lidar measurements and backscatter derived from the aerosol microphysics as required by the NASA Doppler Lidar Program. This will include the analysis of results from the NASA GLOBE Survey Mission Flight Program. Additional instrument development and deployment will be carried out in order to extend and refine this data base. Identified activities include participation in groundbased and airborne experiments. Progress to date includes participation in, analysis of, and publication of results from Mauna Loa Backscatter Intercomparison Experiment (MABIE) and Global Backscatter Experiment (GLOBE).

Clarke, Antony D.↗

Remote sensing of aerosols with the Earth Observing Scanning Polarimeter

Tropospheric aerosols have potential climate forcing roles through both the direct effect on solar radiation scattered and absorbed and the indirect effect as condensation nuclei for cloud particles. Present capabilities for characterizing the global aerosol climatology are limited by the existing satellite remote sensing measurements, making a quantitative determination of the climate forcing effects of aerosols rather difficult and uncertain. The Earth Observing Scanning Polarimeter (EOSP) instrument under consideration for Earth Observing System (EOS) mission platforms and for a proposed Climsat Earth Probe mission is intended to provide global mapping with multispectral photopolarimetry, which can be exploited for the more pronounced aerosol signature in the polarization of the scattered light as compared to the radiance. We describe the essential features and performance specifications of the EOSP instrument and discuss approaches for retrieving tropospheric aerosol properties from multispectral photopolarimetry.

Travis, Larry D.↗

Airborne lidar measurements of ozone and aerosols in the summertime Arctic troposphere

Ozone (O3) and aerosol distributions were remotely measured from an aircraft using a differential absorption lidar (DIAL) system as part of the 1988 NASA Global Tropospheric Experiment - Arctic Boundary Layer Experiment (ABLE-3A). The airborne DIAL system made simultaneous measurements of O3 and aerosols from the surface to above the tropopause. These measurements were made in a broad range of atmospheric conditions over the tundra, ice, and ocean regions near Barrow and Bethel, Alaska, during July and August 1988. The tropospheric composition over the Arctic was found to be strongly influenced by stratospheric intrusions. Regions of low aerosol scattering and enhanced O3 mixing ratios were usually correlated with descending air from the upper troposphere or lower stratosphere. Several cases of enhanced O3 were observed during ABLE-3A in conjunction with enhanced aerosol layers in the free troposphere resulting from biomass burning. As was found in the Amazon, the products of biomass burning can significantly alter O3 concentrations in the troposphere. This paper describes the NASA airborne DIAL system and discusses the large-scale variations of O3 and aerosols observed with the airborne DIAL system during ABLE-3A.

Browell, Edward V.↗

Stratospheric Aerosol and Gas Experiment (SAGE 3)

The proposed SAGE III instrument would be the principal source of data for global changes of stratospheric aerosols, stratospheric water vapor, and ozone profiles, and a contributing source of data for upper tropospheric water vapor, aerosols, and clouds. The ability to obtain such data has been demonstrated by the predecessor instrument, SAGE II, but SAGE III will be substantially more capable, as discussed below. The capabilities for monitoring the profiles of atmospheric constituents have been verified in detail, including ground-based validations, for aerosol, ozone, and water vapor. Indeed, because of its self-calibrating characteristics, SAGE II was an essential component of the international ozone trend assessments, and SAGE II is now proving to be invaluable in tracking the aerosols from Mt. Pinatubo. Although SAGE profiles generally terminate at the height of the first tropospheric cloud layer, it has been found that the measurements extend down to 3 km altitude more than 40 percent of the time at most latitudes. Thus, useful information can also be obtained on upper tropospheric aerosols, water vapor, and ozone.

Mccormick, M. P.↗

Comparison of the impact of volcanic eruptions and aircraft emissions on the aerosol mass loading and sulfur budget in the stratosphere

Data obtained by the Stratospheric Aerosol and Gas Experiment (SAGE) 1 and 2 were used to study the temporal variation of aerosol optical properties and to assess the mass loading of stratospheric aerosols from the eruption of volcanos Ruiz and Kelut. It was found that the yearly global average of optical depth at 1.0 micron for stratospheric background aerosols in 1979 was 1.16 x 10(exp -3) and in 1989 was 1.66 x 10(exp -3). The eruptions of volcanos Ruiz and Kelut ejected at least 5.6 x 10(exp 5) and 1.8 x 10(exp 5) tons of materials into the stratosphere, respectively. The amount of sulfur emitted per year from the projected subsonic and supersonic fleet is comparable to that contained in the background aerosol particles in midlatitudes from 35 deg N to 55 deg N.

Yue, Glenn K.↗

Effects of stratospheric aerosol surface processes on the LLNL two-dimensional zonally averaged model

We have investigated the effects of incorporating representations of heterogeneous chemical processes associated with stratospheric sulfuric acid aerosol into the LLNL two-dimensional, zonally averaged, model of the troposphere and stratosphere. Using distributions of aerosol surface area and volume density derived from SAGE II satellite observations, we were primarily interested in changes in partitioning within the Cl- and N- families in the lower stratosphere, compared to a model including only gas phase photochemical reactions. We have considered the heterogeneous hydrolysis reactions N2O5 + H2O(aerosol) yields 2 HNO3 and ClONO2 + H2O(aerosol) yields HOCl + HNO3 alone and in combination with the proposed formation of nitrosyl sulfuric acid (NSA) in the aerosol and its reaction with HCl. Inclusion of these processes produces significant changes in partitioning in the NO(y) and ClO(y) families in the middle stratosphere.

Connell, Peter S.↗

Lidar measurements of ozone and aerosol distributions during the 1992 airborne Arctic stratospheric expedition

The NASA Langley airborne differential absorption lidar system was operated from the NASA Ames DC-8 aircraft during the 1992 Airborne Arctic Stratospheric Expedition to investigate the distribution of stratospheric aerosols and ozone (O3) across the Arctic vortex from January to March 1992. Aerosols from the Mt. Pinatubo eruption were found outside and inside the Arctic vortex with distinctly different scattering characteristics and spatial distributions in the two regions. The aerosol and O3 distributions clearly identified the edge of the vortex and provided additional information on vortex dynamics and transport processes. Few polar stratospheric clouds were observed during the AASE-2; however, those that were found had enhanced scattering and depolarization over the background Pinatubo aerosols. The distribution of aerosols inside the vortex exhibited relatively minor changes during the AASE-2. Ozone depletion inside the vortex as limited to less than or equal to 20 percent in the altitude region from 15-20 km.

Browell, Edward V.↗

Stratospheric aerosol increase after eruption of Pinatubo observed with lidar and aureolemeter

An increase in the amount of stratospheric aerosol due to the Pinatubo eruption (June 12-15, 1991, 15.14 deg N, 120.35 deg E) was observed from the end of June, 1991 by a lidar in NIES (National Institute for Environmental Studies), Tsukuba (36.0 deg N, 140.1 deg E). After large fluctuations in summer of 1991, the amount of the aerosols increased in mid-September as a result of enhanced transportation from the subtropical region. In autumn and winter of 1991, dense aerosol layers were continuously observed. Aureolemeter (scanning spectral radiometer) measurements were also carried out with lidar measurements and columnar size distribution of stratospheric aerosols was estimated for some cases. Collaborative measurements with the lidar and aureolemeter provided some information on height distribution of the surface area of aerosols in late 1991.

Hayashida, Sachiko↗

Aerosol-associated changes in tropical stratospheric ozone following the eruption of Mount Pinatubo

The large amount of sulfuric acid aerosol formed in the stratosphere by conversion of sulfur dioxide emitted by the eruption of Mount Pinatubo (15.14 deg N, 120.35 deg E) in the Philippines around June 15, 1991, has had a pronounced effect on lower stratospheric ozone in the tropics. Measurements of stratospheric ozone in the tropics using electrochemical concentration cell (ECC) sondes before and after the eruption and the airborne UV differential absorption lidar (DIAL) system after the eruption are compared with Stratospheric Aerosol and Gas Experiment II (SAGE II) measurements from several years before the eruption and ECC sonde measurements from the year prior to the eruption to determine the resulting changes. Ozone decreases of up to 33 % compared with SAGE II climatological values were found to be directly correlated with altitude regions of enhanced aerosol loading in the 16- to 28-km range. A maximum partial-column decrease of 29 +/- Dobson units (DU) was found over the 16- to 28-km range in September 1991 along with small increases (to 5.9 +/- 2 DU) from 28 to 31.5 km. A large decrease of ozone was also found at 4 deg to 8 deg S from May to August 1992, with a maximum decrease of 33 +/- 7 DU found above Brazzaville in July. Aerosol data form the visible channel of the advanced very high resolution radiometer (AVHRR) and the visible wavelength of the UV DIAL system were used to examine the relationship between aerosol (surface area) densities and ozone changes. The tropical stratospheric ozone changes we observed in 1991 and 1992 are likely be explained by a combination of dynamical (vertical transport) perturbations, radiative perturbations on ozone photochemistry, and heterogeneous chemistry.

Grant, William B.↗

Two-dimensional simulation of Pinatubo aerosol and its effect on stratospheric ozone

This paper presents time-dependent simulations of the response of the stratosphere to the injection into the atmosphere of massive amounts of sulfur during the eruption of Mt. Pinatubo (The Philippines) in June 1991. The study is based on a coupled two-dimensional chemical-dynamical-radiative model to which a microphysical model for sulfate aerosol formation and fate has been added. The study suggests that, during the first year (July 1991 to June 1992) following the volcanic eruption, the observed changes in the ozone amount integrated between 65 deg S and 65 deg N were caused primarily by changes in the meridional circulation (associated with heating by the volcanic cloud in the tropics) and in the photolysis rate of molecules such as ozone (associated with backscattering of light by the cloud). During the second year after the eruption, as the aerosol was dispersed at all latitudes and, in particular, reached the polar region, the largest contribution to ozone reduction resulted from the heterogeneous chemical conversion of N2O5 and ClONO2 on the surface of the aerosol particles. The conversion of the latter compound, and hence the magnitude of the calculated ozone depletion, is highly dependent on the temperature in the lower stratosphere. Despite the fact that the surface area provided by aerosol particles decreased during the second year following the eruption, the calculated ozone depletion remained significant because the conversion of N2O5 is insensitive to the aerosol surface area density for values larger than 1-10 sq microns/cu cm (depending on latitude). The predicted reduction in ozone at 20 km in March during the third year (July 1993 to June 1994) of the model integration is smaller by a factor of 2 than it was during the second year.

Tie, Xuexi↗