Important chemical and physical roles of aerosols are discussed, and properties of stratospheric aerosols as revealed by experimental data are described. In situ measurements obtained by mechanical collection and scattered-light detection yield the overall size distribution of the aerosols, and analyses of preserved aerosol precursor gases by wet chemical, cryogenic and spectroscopic techniques indicate the photochemical sources of particle mass. Aerosol chemical reactions including those of gaseous precursors, those in aqueous solution, and those on particle surfaces are discussed, in addition to aerosol microphysical processes such as nucleation, condensation/evaporation, coagulation and sedimentation. Models of aerosols incorporating such chemical and physical processes are presented, and simulations are shown to agree with measurements. Estimates are presented for the potential aerosol changes due to emission of particles and gases by aerospace operations and industrial consumption of fossil fuels, and it is demonstrated that although the climatic effects of existing levels of stratospheric aerosol pollution are negligible, potential increases in those levels might pose a future threat.

Stratospheric aerosols: Observation and theory

Data obtained from measurements of the stratospheric aerosol at Laramie, Wyoming (41°N), indicate that the background or nonvolcanic stratospheric sulfuric acid aerosol mass at northern mid-latitudes has increased by about 5 ± 2 percent per year during the past 10 years. Whether this increase is natural or anthropogenic could not be determined at this time because of inadequate information on sulfur sources, in particular, carbonyl sulfide, which is thought to be the dominant nonvolcanic source of stratospheric sulfuric acid vapor. An increase in stratospheric sulfate levels has important climatic implications as well as heterogeneous chemical effects that may alter the concentration of stratospheric ozone.

https://science.sciencemag.org/content/sci/248/4958/996.full.pdf

Increase in the stratospheric background sulfuric acid aerosol mass in the past 10 years.

The stratospheric sulfuric acid fraction and mass for the 1982 volcanic eruptions of El Chichon are investigated using data from balloon soundings at Laramie (41 deg N) and in southern Texas (27-29 deg N). The total stratospheric mass of these eruptions is estimated to be approximately 8 Tg about 6.5 months after the eruption with possibly as much as 20 Tg in the stratosphere about 45 days after the eruption. Observations of the aerosol in Texas revealed two primary layers, both highly volatile at 150 C. Aerosol in the upper layer at about 25 km was composed of an approximately 80 percent H2SO4 solution while the lower layer at approximately 18 km was composed of a 60-65 percent H2SO4 solution aerosol. It is calculated that an H2SO4 vapor concentration of at least 3 x 10 to the 7th molecules/cu cm is needed to sustain the large droplets in the upper layer. An early bi-modal nature in the size distribution indicates droplet nucleation from the gas phase during the first 3 months, while the similarity of the large particle profiles 2 months apart shows continued particle growth 6.5 months after the explosion.

Stratospheric sulfuric acid fraction and mass estimate for the 1982 volcanic eruption of El Chichon

Characterizations of meteoric dust height and size distributions are obtained using Hunten's calculations of meteor ablation and recondensation rates. The contribution of meteor residues to aerosol composition, the role of meteoric dust as condensation nuclei, and the effects of meteor debris on aerosol size distributions are quantified, and particle surface areas are estimated. The potential importance of heterogeneous chemistry for stratospheric trace gases is discussed. The interaction between H2SO4 vapor and meteor metal vapors is investigated. It is concluded that meteoric particles may dominate the natural stratospheric aerosols at small (less than .01 micron radius) and large (greater than 1 micron radius) sizes under normal conditions.

Effects of meteoric debris on stratospheric aerosols and gases

The paper examines the tropospheric aerosol record obtained over the period 1971 to 1990, during which high-altitude balloons with optical particle counters were launched at Laramie, Wyoming, in a long-term study of the stratospheric sulfate aerosol layer. All aerosol particle size ranges display pronounced seasonal variations, with the condensation nuclei concentration and the optically active component showing a summer maximum throughout the troposphere. Mass estimates, assuming spherical sulfate particles, indicate an average column mass between altitudes of 2.5 and 10 km of about 4 and 16 mg/sq m in winter and summer, respectively. Calculated optical depths vary between 0.01 and 0.04 from winter to summer; the estimated mass scattering cross section is about 3 sq m/g throughout the troposphere. There is evidence for a decreasing trend of 1.6-1.8 percent/yr in the optically active tropospheric aerosol over the past 20 yr, which may be related to a similar reduction in SO2 emission in the U.S. over this period.

Twenty years of balloon-borne tropospheric aerosol measurements at Laramie, Wyoming

A condensation nuclei (CN) counter has been developed for balloonborne use at ambient pressures in the troposphere and stratosphere. The instrument employs a thermal gradient diffusion cloud chamber to produce particle growth and a photoelectric particle counter for detection. After extensive laboratory tests, the instrument was successfully flown on several balloon soundings over Laramie. The results show a roughly constant mixing ratio in the stratosphere with a CN concentration of about 20 cm−3 at 15 km. The vertical profile of CN in the troposphere displayed concentration fluctuations ranging between 200 and 2000 cm−3 with a definite maximum in the mixing ratio just below the tropopause.

Balloonborne Measurements of Condensation Nuclei

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Balloonborne Measurements of Condensation Nuclei