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Microwave Limb Sounder measurement of stratospheric SO2 from the Mt. Pinatubo volcano

The Microwave Limb Sounder (MLS) experiment on the Upper Atmosphere Research Satellite (UARS) began atmospheric measurements on September 19, 1991. Residual SO2 from the Pinatubo eruption was detected immediately after instrument activation. The SO2 was 1ocated in a tropical band with peak mixing ratios of about 15 ppbv near 26 km altitude. The observed decay of SO2 has provided an estimate of the OH concentration in the plume.

Read, W. G.↗

In situ observations of aerosol and chlorine monoxide after the 1991 eruption of Mount Pinatubo - Effect of reactions on sulfate aerosol

Highly resolved aerosol size distributions measured from high-altitude aircraft can be used to describe the effect of the 1991 eruption of Mount Pinatubo on the stratospheric aerosol. In some air masses, aerosol mass mixing ratios increased by factors exceeding 100 and aerosol surface area concentrations increased by factors of 30 or more. Increases in aerosol surface area concentration were accompanied by increases in chlorine monoxide at mid-latitudes when confounding factors were controlled. This observation supports the assertion that reactions occurring on the aerosol can increase the fraction of stratospheric chlorine that occurs in ozone-destroying forms.

Wilson, J. C.↗

The atmospheric SO2 budget for Pinatubo derived from NOAA-11 SBUV/2 spectral data

Spectral scan data from the NOAA-11 SBUV/2 instrument were used to derive SO2 for three days following the eruption of Mt. Pinatubo - June 19, July 1, and July 17, 1991. Band structure between 300 and 310 nm observed in the backscattered albedo uniquely identifies the presence of SO2. Band ratios are used to infer SO2 amounts to better accuracy (10-20 percent) and sensitivity (about 0.5 milli-atm-cm of SO2) than the TOMS retrieval, but with relatively poor spatial coverage because the measurement is nadir only. Only 7 scans showed detectable SO2 on June 19 when the cloud was still very localized. On July 1 there were 29 scans between 35N and 12S with SO2, with the highest concentration detected over the Atlantic, and on July 17 SO2 was detected in 30 scans around the world, but in decreased concentration. Estimates of the total SO2 budget made after the cloud had spread sufficiently for the sparse SBUV/2 sampling to be adequate indicated that there were 8.4 million metric tons (MMT) of SO2 in the stratosphere on July 1, 1991, and 4.1 MMT remaining on July 17. This corresponds to an e-folding time of about 24 days for the conversion of SO2 to aerosol, and is consistent with an initial injection into the stratosphere of 12-15 MMT of SO2.

Mcpeters, Richard D.↗

Effects of the Mount Pinatubo eruption on the radiative and chemical processes in the troposphere and stratosphere

The Lawrence Livermore National Laboratory two-dimensional zonally-averaged chemical-radiative-transport model of the global atmosphere was used to study the effects of the 15 June 1991 eruption of the Mt. Pinatubo volcano on stratospheric processes. SAGE 2 time-dependent aerosol surface area density and optical extinction data were used as input into the model. By 22 December 1991, a maximum equatorial change of -1.8 percent in column ozone was derived from heterogeneous chemical processes that convert NO(x) into HNO3 on sulfuric acid aerosols. Radiative feedbacks from increased aerosol optical thickness independently changes column ozone by approximately -3.5 percent for the same period. This occurs from increasing the net heating of the lower stratosphere, which indirectly increases chemical reaction rates via their temperature dependence and from changes in actinic fluxes, which directly modify photodissociation rates. Including both heterogeneous and radiative effects changes column ozone by -5.5 percent. The model-derived change overestimates the decrease in column ozone relative to the TOMS instrument on the Nimbus 7 satellite. Maximum local ozone decreases of 12 percent were derived in the equatorial region, at 25 km. Model-derived column NO2 peaked (-14 percent) at 30 deg S in October 1991. The timing of the NO2 peak is consistent with observation, but the model underestimates the magnitude of the decrease. Local concentrations of NO(x) (NO + NO2), ClO(x) (Cl + ClO), and HO(x) (OH + HO2), in the lower stratosphere between 30 deg S and 30 deg N, were calculated to have changed by -40 percent, +100 to +160 percent, and +120 to +140 percent respectively.

Kinnison, Douglas E.↗

UV spectral irradiance measurements in New Zealand: Effects of Pinatubo volcanic aerosol

Since late 1989, regular UV spectral irradiance measurements have been made at Lauder, New Zealand (45 deg S, 170 deg E), whenever weather permits. Here, the instrumentation and measurement strategy are outlined, and early results are discussed. Following the eruption of Mt Pinatubo in June 1991, large amounts of volcanic aerosol were injected into the stratosphere and were subsequently transported to New Zealand's latitudes in the latter half of 1991. This provides an opportunity to investigate the effects of volcanic aerosols on UV irradiances measured at this clean-air site. Although changes in global (sum of diffuse plus direct) irradiances were below the detection threshold, there were significant changes in the partitioning of radiation between the direct beam and diffuse skylight. Decreases by nearly a factor of two in the direct/diffuse ratio were observed at longer wavelengths, and at smaller solar zenith angles (sza's). The aerosol optical depth due to volcanic aerosol over Lauder in December 1991 was 0.15 plus or minus 0.02 at 450 nm, with lower values at shorter wavelengths. Although effects were relatively small in the UVB region, an implication of the changes is that the contrast between shade and direct sun is reduced, so that shaded areas received relatively more radiation in the summer of 1991/92 in New Zealand.

Mckenzie, Richard L.↗

Volcanic-aerosol-induced changes in stratospheric ozone following the eruption of Mount Pinatubo

Measurements of lower stratospheric ozone in the Tropics using electrochemical concentrations cell (ECC) sondes and the airborne UV Differential Absorption Lidar (DIAL) system after the eruption of Mt. Pinatubo are compared with the Stratospheric Aerosol and Gas Experiment 2 (SAGE 2) and ECC sonde measurements from below the eruption to determine what changes have occurred as a result. Aerosol data from the Advanced Very High Resolution Radiometer (AVHRR) and the visible and IR wavelengths of the lidar system are used to examine the relationship between aerosols and ozone changes. Ozone decreases of 30 percent at altitudes between 19 and 26 km, partial column (16-28 km) decreases of about 27 D.U., and slight increases (5.4 D.U.) between 28 and 31 km are found in comparison with SAGE 2 climatological values.

Grant, W. B.↗

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↗

Radiatively forced dispersion of the Mt. Pinatubo volcanic cloud and induced temperature perturbations in the stratosphere during the first few months following the eruption

A combined 3-dimensional circulation model and aerosol microphysical/transport model is used to simulate the dispersion of the Mt. Pinatubo volcanic cloud in the stratosphere for the first few months following the eruption. Radiative heating of the cloud due to upwelling infrared radiation from the troposphere is shown to be an important factor affecting the transport. Without cloud heating, cloud material stays mostly north of the equator, whereas with cloud heating, the cloud is transported southward across the equator within the first two weeks following the eruption. Generally the simulations agree with Total Ozone Mapping Spectrometer (TOMS), Advanced Very High Resolution Radiometer (AVHRR), and Stratospheric Aerosol and Gas Experiment (SAGE) satellite observations showing the latitude distribution of cloud material to be between about 20 deg S and 30 deg N within the first few months. Temperature perturbations in the stratosphere induced by the aerosol heating are generally 1-4 K, in the range of those observed.

Young, Richard E.↗

Ozone response to enhanced heterogeneous processing after the eruption of Mt. Pinatubo

Increases in aerosol loading after the Pinatubo eruption are expected to cause additional ozone depletion. Even though aerosol loadings were highest in the winter of 1991-1992, recent analyses of satellite and ground-based ozone measurements indicate that ozone levels in the winter of 1992-1993 are the lowest recorded in recent years, raising the question of the mechanisms responsible for such behavior. We have incorporated aerosol surface areas derived from the Stratospheric Aerosol and Gas Experiment II (SAGE-II) measurements into our two-dimensional model. Inclusion of heterogeneous chemsitry on these enhanced aerosol surfaces yields maximum ozone reductions during the winter of 1992-1993 in the Northern Hemisphere, consistent with those derived from observations. This delayed behavior is due to the combination of the non-linear nature of the impact of heterogeneous reactions as a function of aerosol surface area, and the long time constants for ozone in the lower stratosphere. If heterogeneous mechanisms are primarily responsible for the low 1992-1993 ozone levels, we expect ozone concentrations to start recovering in 1994.

Rodriguez, Jose M.↗

The effect of the Mt. Pinatubo aerosol on the NHO3 column over Mauna Loa, Hawaii

A very high resolution infrared solar spectrometer system for the Network for Detection of Stratospheric Change has been routinely operated at the Mauna Loa Observatory in Hawaii since November, 1991. Solar absorption spectra are normally taken one day a week at sunrise. We report the analysis of these spectra for the vertical column amount of nitric acid (HNO3) vapor. The observations began four months after the arrival of volcanic aerosols from Mt. Pinatubo over the site. Although quite variable, total HNO3 columns were initially about 7 x 10(exp 15) molecules/sq cm and have decreased about 30% in the following two years.

David, Shelle J.↗

Effects of Pinatubo aerosol on stratospheric ozone at mid-latitudes

Mid-latitude ozone data from ER-2 aircraft measurements in 1989, 1991, and 1992 were examined to determine how sulfate aerosols from the eruption of Mt. Pinatubo had affected ozone at about 18 km. N2O was used as a tracer to help distinguish between chemical and dynamical aerosol effects. At 20-45 deg N in February 1992, ozone was about 10-20% lower than February 1989 and 1991, with respect to N2O. Data from Aug. 1991 - Mar. 1992 showed changes in ozone with respect to N2O, but the magnitude of those changes was not correlated with the magnitude of the changes in aerosol surface area density.

Weaver, A.↗

In situ measurements of ClO at mid-latitudes: Is there an effect from Mt. Pinatubo?

Observations of ClO from 20 to 60 deg N made before and after the eruption of Mt. Pinatubo are compared for changes which may result from increased sulfate aerosol surface area. Using ozone as a vertical coordinate and examining data at similar latitudes and seasons, elevated abundances of ClO are found at low latitudes (20 to 30 deg N), an effect which decreases with increasing latitude. For the flights compared, there appear to be no differences, within the uncertainty of the measurements, at latitudes poleward of 40 deg N. These results are consistent with the idea that the hydrolysis of N2O5 on sulfate aerosols becomes saturated at moderate aerosol loadings.

Avallone, L. M.↗

Post-Pinatubo optical depth spectra vs. latitude and vortex structure: Airborne tracking sunphotometer measurements in AASE 2

In January and March 1992, DC-8-measured stratospheric particle optical depth spectra, tau(sub P)(lambda), peaked broadly at midvisible or longer wavelenghts. At mid-to-high northern latitudes outside the vortex, tau(sub p)(526 nm) above about 11 km was as large as 0.22 in both January and March, reflecting continued Pinatubo volcanic influence. In both months, in-vortex tau(sub p)(lambda) above 11 km was smaller than outside-vortex values by a factor of two or more, and in January a strong anticorrelation was observed between tau(sub p)(lambda) and HF column content (an indicator of vortex penetration). In late January at 18-20S, near the edge of the southern subtropical jet, tau(sub p)(526 nm) above 12 km was only about 0.07-0.09, with a flatter spectral shape than northern mid- to high-latitude measurements in both January and March. Occasional high-latitude vertical profiles indicate 6-11-km slab optical depths, Delta tau(sub p)(526 nm), of 0.05 to 0.1, which should be added to the above-11-km values to yield values above 6 km.

Russell, P. B.↗

Physical and optical properties of the Pinatubo volcanic aerosol: Aircraft observations with impactors and a Sun-tracking photometer

As determined in situ by impactor samplers flown on an ER-2 at 16.5- to 20.7-km pressure altitude and on a DC-8 at 9.5- to 12.6-km pressure altitudes, the 1991 Pinatubo volcanic eruption increased the particle surface area of stratospheric aerosols up to 50-fold and the particle volume up to 2 orders of magnitude. Particle composition was typical of a sulfuric acid-water mixture at ER-2 altitudes. Ash particles coated with sulfuric acid comprised a significant fraction of aerosol at DC-8 altitudes. Mie-computed light extinction increased up to 20-fold at midvisible and greater than 100-fold at near-IR wavelengths. The optical thickness measured through the aerosol layer by an autotracking Sun photometer aboard a DC-8 aircraft at 10.7- to 11.3-km pressure altitudes shows a spectral shape that is similar to the Mie-calculated spectral extinction at ER-2 altitudes. Surface area distributions calculated by inversion of spectral optical depth measurements show characteristics that are similar to the mean surface area distribution resulting from 35 in situ measurements.

Pueschel, R. F.↗

Evolution of Pinatubo aerosol near 19 km altitude over western North America

Stratospheric aerosols, collected near 19 km altitude on wire impactors over western North America from August 20, 1991 to May 11, 1993, show strong influence of the June 1991 Mt. Pinatubo eruption. Lognormal size distributions are bimodal; each of the mode radii increases and reaches maximum value at about 15 months after eruption. The second (large particle) mode becomes well developed then, and about 40% of the droplets are larger than 0.4 micron radius. The eruption of Mt. Spurr (Alaska) may also have contributed to this. Sulfate mass loading decays exponentially (e-folding 216 days), similar to El Chichon. Silicates are present in samples only immediately after eruption. Two years after eruption, sulfate mass loading is about 0.4 micrograms/cu m, about an order of magnitude higher than background pre-volcanic values. Aerosol size distributions are still bimodal with a very well-defined large droplet mode.

Goodman, Jindra↗

Mid-infrared extinction by sulfate aerosols from the Mt. Pinatubo eruption

Quantitative measurements of the wavelength dependence of aerosol extinction in the 750-3400/cm spectral region have been derived from 0.01/cm resolution stratospheric solar occultation spectra recorded by the ATMOS (Atmospheric Trace Molecule Spectroscopy) Fourier transform spectrometer about 9 1/2 months after the Mt Pinatubo volcanic eruption. Strong, broad aerosol features have been identified near 900, 1060, 1190, 1720, and 2900/cm below a tangent height of approximately 30 km. Aerosol extinction measurements derived from approximately 0.05/cm wide microwindows nearly free of telluric line absorption in the ATMOS spectra are compared with transmission calculations derived from aerosol size distribution profiles retrieved from correlative SAGE (Stratospheric Aerosol and Gas Experiment) II visible and near i.r. extinction measurements, seasonal and zonally averaged H2SO4 aerosol weight percentage profiles, and published sulfuric acid optical constants derived from room temperature laboratory measurements. The calculated shapes and positions of the aerosol features are generally consistent with the observations, thereby confirming that the aerosols are predominantly concentrated H2SO4-H2O droplets, but there are significant differences between the measured and calculated wavelength dependences of the aerosol extinction. We attribute these differences as primarily the result of errors in the calculated low temperature H2SO4-H2O optical constants. Errors in both the published room temperature optical constants and the limitations of the Lorentz-Lorenz relation are likely to be important.

Rinsland, C. P.↗