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Stratospheric aerosols - Observation and theory

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.

Turco, R. P.↗

Banded structures in stratospheric aerosol distributions

Zonal bands of stratospheric aerosol optical depth are observed by various sensors under both volcanic and non-volcanic conditions. Maximum optical depths occur within the tropics and at high latitudes, while minima are found between latitudes of approximately 15 deg and 45 deg. This structure is shown to result from a reservoir of aerosol over the tropics, poleward transport, and the departure of the tropopause from isentropic surfaces.

Trepte, Charles R.↗

Volcanic eruptions and the increases in the stratospheric aerosol content: Lidar measurements from 1982 to 1986

The results of the observation for stratospheric aerosols which were carried out since the autumn of 1982 by using the NIES large lidar are described. Specifications of the lidar system are shown. The lidar has two wavelenghts of 1.06 and 0.53 micrometers. The 0.53 micrometer is mainly used for the stratospheric aerosols, because the PMT for 0.53 micrometers has higher sensitivity that that for 1.06 micrometers and the total efficiency is higher in the former. A switching circuit is used to control the PMT gain for avoiding signal induced noise in PMT. For the last four years, the stratospheric aerosol layer which was significantly perturbed by the El Chichon volcanic eruption was observed. The scattering ratio profiles observed from 1982 through 1983 are given.

Hayashida, S.↗

Satellite studies of the stratospheric aerosol

The potential climatological and environmental importance of the stratospheric aerosol layer has prompted interest in measuring the properties of this aerosol. This paper reports on two recently deployed NASA satellite systems (SAM II and SAGE) that are monitoring the stratospheric aerosol. The satellite orbits obtain nearly global coverage. The instruments mounted in the spacecraft are sun photometers that measure solar intensity at specific wavelengths as it is moderated by atmospheric particulates and gases during each sunrise and sunset encountered by the satellites. Latitudinal, longitudinal, and temporal variations in the aerosol layer are evaluated. The satellite systems are being validated by a series of ground truth experiments using airborne and ground lidar, balloon-borne dustsondes, aircraft-mounted impactors, and other correlative sensors. The SAM II and SAGE satellite systems, instrument characteristics, and mode of operation are described; the methodology of the experiments is outlined; and the ground truth experiments are discussed. Preliminary results from these measurements are presented.

Mccormick, M. P.↗

Comparison of Stratospheric Aerosol and Gas Experiment II and balloon-borne stratospheric water vapor measurements

The Stratospheric Aerosol and Gas Experiment II has one channel at 940 nm related to water vapor. Two inversion procedures were developed independently in order to obtain the water vapor profile: the Chahine method by the Langley Research Center, and the Mill method by the Laboratoire d'Optique Atmospherique. Comparisons were made between these two algorithms and some results are presented at midlatitudes (about 45 deg N) and tropical latitudes (12-25 deg S). They are compared with in situ frost point hygrometer data provided by balloon experiments from the Laboratoire de Meteorologie Dynamique. At +/- 0.5 ppmv, agreement between the inversion results and the experimental results was obtained in the altitude range from 18-19 to 26-27 km. Below 18-19 km and above 26-27 km the error is larger (sometimes 1 ppmv and more).

Pruvost, P.↗

The modeling of CO2 lidar backscatter from stratospheric aerosols

Factors that affect modeling for the scattering properties of stratospheric aerosols at CO2 laser wavelengths are discussed. Particular attention is given to the relevant stratospheric aerosol measurements, both in situ and remote, and of the techniques for modeling optical properties at wavelengths close to 10.6 microns. The results obtained by such modeling are compared with published CO2 lidar data.

Kent, G. S.↗

Stratospheric aerosol injection can weaken the carbon dioxide greenhouse effect

Abstract Stratospheric aerosol injection is a proposed method for offsetting greenhouse gas-induced warming by introducing scattering aerosols into the lower stratosphere to reflect sunlight. Here we explore a potentially more efficient alternative: weakening the Earth’s greenhouse effect by deploying absorptive aerosols in the upper stratosphere (~10 hPa). These aerosols warm the carbon dioxide emission level—where outgoing longwave radiation is most sensitive to temperature—thereby enhancing top-of-atmosphere infrared emission without altering atmospheric carbon dioxide concentrations. Idealized climate model simulations indicate that this approach can reduce global temperatures an order of magnitude more efficiently per unit aerosol mass than conventional scattering-based interventions. Although based on simplified model experiments lacking interactive aerosol processes and operational constraints, our results identify a distinct physical mechanism for climate intervention, arguing for further research into the impacts—especially potential unintended side effects—of injecting absorptive aerosols into the upper stratosphere as an alternative solar radiation management strategy.

Environmental Sciences & Ecology↗

Analysis and interpretation of lidar observations of the stratospheric aerosol

Data obtained with a 48 in. telescope lidar system are compared with results obtained using a one-dimensional stratospheric aerosol model to analyze various microphysical processes influencing the formation of this aerosol. Special attention is given to the following problems: (1) how lidar data can help determine the composition of the aerosol particles and (2) how the layer corresponds to temperature profile variations. The lidar record during the period 1974 to 1979 shows a considerable decrease of the peak value of the backscatter ratio. Seasonal variations in the aerosol layer and a gradual decrease in stratospheric loading are observed. The aerosol model simulates a background stratospheric aerosol layer, and it predicts stratospheric aerosol concentrations and compositions. Numerical experiments are carried out by using the model and by comparing the theoretical results with the experimentally obtained lidar record. Comparisons show that the backscatter profile is consistent with the composition when the particles are sulfuric acid and water; it is not consistent with an ammonium sulfate composition. It is shown that the backscatter ratio is not sensitive to the composition or stratospheric loading of condensation nuclei such as meteoritic debris.

Hamill, P.↗

Retrieval of stratospheric aerosol size distribution from atmospheric extinction of solar radiation at two wavelengths

A parametric study is presented of the effects of the size distribution and composition of stratospheric aerosols on the value R, the ratio of the extinction of solar radiation at wavelength 0.45 micron to the extinction at wavelength 1.0 micron. The aerosol size distributions under study comprise nine analytical expressions, including most of the stratospheric aerosol models used by investigators. The aerosol compositions considered are the supercooled sulfuric-acid droplets, with different weight percentages of H2SO4 in the aerosol. It is found that whereas R is not very sensitive to either the composition or the radii limits of the stratospheric aerosols under consideration, it is quite sensitive to the value of the variable parameter governing the mode radius of the size distribution of aerosol particles. The results of the parametric study underlie the method proposed here of retrieving the size distribution of aerosol particles in the stratosphere from the experimental results of the extinction of solar radiation at two wavelengths.

Yue, G. K.↗

Stratospheric aerosol measurement experiment MA-007

The Apollo Soyuz Test Project Stratospheric Aerosol Measurement Experiment was flown to demonstrate that direct solar occultation measurements by photometers and photographs can be used for defining stratospheric aerosol concentrations. Supporting ground truth data were provided by laser radar and balloon borne dustsonde. Initial results show a significant difference in aerosol concentrations between the Northern and Southern Hemispheres.

Pepin, T. J.↗

The change of depolarization of backscattering light from the polar stratospheric aerosol layer

The change of polarization properties of scattered light strongly depends on the non-spherisity of target particles. It should be helpful information for the study of stratospheric aerosols to know the non-spherisity of stratospheric aerosol particles. The change of the total backscatter depolarization ratio of the stratospheric aerosol layer measured at Syowa Station (69.00 deg S, 39.35 deg E), Antarctica is described.

Iwasaka, Y.↗

Stratospheric aerosols - Undissolved granules and physical state

The physical state of stratospheric aerosol particles was studied along with the nature of included undissolved granules. It was found that: (1) undissolved granules are present in only a third of the aerosol particles and are not always associated with a slurry matrix, (2) those undissolved particles usually contain only sulfur and sodium or undetectable light elements, (3) all stratospheric aerosols have a similar appearance: a volatile slurry mixture of crystalline-like material in a liquid matrix, and (4) variations in the relative amounts of liquid and crystalline materials at different times cause variations in particle spreading.

Farlow, N. H.↗

Post-volcanic stratospheric aerosol decay as measured by lidar

The paper summarizes and discusses results of lidar observations, at Hampton (Virginia), of the stratospheric aerosol vertical distribution for a period of 22 months (October 1974 to July 1976) after the volcanic eruption of the Volcan de Fuego in Guatemala. Data are presented in terms of lidar scattering ratio, vertically integrated aerosol backscattering, layer structure and location, and rawinsonde temperature profiles as a function of time. The results reveal a sudden increase in the stratospheric aerosol content after the volcanic eruption as well as its subsequent decline. There exists a high degree of correlation between the integrated aerosol backscattering and the tropopause height such that as one decreases the other increases and vice versa. Rapid decay of the stratospheric aerosol is found to occur over the late winter to early spring period.

Mccormick, M. P.↗

Evaluation of SAGE II and Balloon-Borne Stratospheric Aerosol Measurements: Evaluation of Aerosol Measurements from SAGE II, HALOE, and Balloonborne Optical Particle Counters

Stratospheric aerosol measurements from the University of Wyoming balloonborne optical particle counters (OPCs), the Stratospheric Aerosol and Gas Experiment (SAGE) II, and the Halogen Occultation Experiment (HALOE) were compared in the period 1982-2000, when measurements were available. The OPCs measure aerosol size distributions, and HALOE multiwavelength (2.45-5.26 micrometers) extinction measurements can be used to retrieve aerosol size distributions. Aerosol extinctions at the SAGE II wavelengths (0.386-1.02 micrometers) were computed from these size distributions and compared to SAGE II measurements. In addition, surface areas derived from all three experiments were compared. While the overall impression from these results is encouraging, the agreement can change with latitude, altitude, time, and parameter. In the broadest sense, these comparisons fall into two categories: high aerosol loading (volcanic periods) and low aerosol loading (background periods and altitudes above 25 km). When the aerosol amount was low, SAGE II and HALOE extinctions were higher than the OPC estimates, while the SAGE II surface areas were lower than HALOE and the OPCS. Under high loading conditions all three instruments mutually agree to within 50%.

Hervig, Mark↗

Stratospheric aerosol acidity, density, and refractive index deduced from SAGE 2 and NMC temperature data

Water vapor concentrations obtained by the Stratospheric Aerosol and Gas Experiment 2 (SAGE 2) and collocated temperatures provided by the National Meteorological Center (NMC) from 1986 to 1990 are used to deduce seasonally and zonally averaged acidity, density, and refractive index of stratospheric aerosols. It is found that the weight percentage of sulfuric acid in the aerosols increases from about 60 just above the tropopause to about 86 at 35 km. The density increases from about 1.55 to 1.85 g/cu cm between the same altitude limits. Some seasonal variations of composition and density are evident at high latitudes. The refractive indices at 1.02, 0.694, and 0.532 micrometers increase, respectively, from about 1.425, 1.430, and 1.435 just above the tropopause to about 1.445, 1.455, and 1.458 at altitudes above 27 km, depending on the season and latitude. The aerosol properties presented can be used in models to study the effectiveness of heterogeneous chemistry, the mass loading of stratospheric aerosols, and the extinction and backscatter of aerosols at different wavelengths. Computed aerosol surface areas, rate coefficients for the heterogeneous reaction ClONO2 + H2O yields HOCl + HNO3 and aerosol mass concentrations before and after the Pinatubo eruption in June 1991 are shown as sample applications.

Yue, G. K.↗

Applying Orbital Multi-Angle Photopolarimetric Observations to Study Properties of Aerosols in the Earth's Atmosphere: Implications of Measurements in the 1.378 µm Spectral Channel to Retrieve Microphysical Characteristics and Composition of Stratospheric Aerosols

We analyze the possibilities of orbital photopolarimetric measurements to study properties of aerosols in the Earth's atmosphere. As an example, we consider the case when such measurements are performed within a narrow spectral channel centered at 1.378 µm that allows to retrieve microphysical characteristics of stratospheric aerosols separately from those of tropospheric aerosols. We consider the case of stratospheric aerosols caused by volcanic eruption, and adopt the model of the stratosphere in the form of a homogeneous plane-parallel layer composed of polydisperse spherical particles. We use numerically exact solutions of the vector radiative transfer equation to theoretically simulate measurements carried out at various numbers of scattering angles, including: (i) radiance measurements alone; (ii) polarization measurements alone; and (iii) radiance and polarization measurements together. The results of computations show that the simultaneous use of radiance and polarization measurements at a sufficiently large number of scattering angles enables one to retrieve the optical thickness, effective radius, and refractive index of aerosols with adequate accuracy. We demonstrate how the accuracy of the derived values of the optical parameters of aerosols depends on the accuracy of measurements of the intensity and polarization of the reflected light, optical thickness of aerosol layer itself, effective radius of aerosols, width of the particle size distribution, and number of viewing angles.

Aerosols↗

Inference of stratospheric aerosol composition and size distribution from SAGE II satellite measurements

A method for inferring stratospheric aerosol composition and size distribution from the water vapor concentration and aerosol extinction measurements obtained in the Stratospheric Aerosol and Gas Experiment (SAGE) II and the associated temperature from the NMC. The aerosols are assumed to be sulfuric acid-water droplets. A modified Levenberg-Marquardt algorithm is used to determine model size distribution parameters based on the SAGE II multiwavelength aerosol extinctions. It is found that the best aerosol size information is contained in the aerosol radius range between about 0.25 and 0.80 micron.

Wang, Pi-Huan↗