Patrick Hamill

Polar Stratospheric Cloud Sightings by SAM II

Abstract Sightings of polar stratospheric clouds (PSCs) by the SAM II satellite system during the northern and southern winters of 1979 are reported. PSCs were observed in the Arctic stratosphere at altitudes between about 17 and 25 km during January 1979, with a single sighting in November 1978, and in the Antarctic stratosphere from June to October 1979 at altitudes from the tropopause up to about 23 km. The measured extinction coefficients at 1 μm wavelength were as much as two orders of magnitude greater than that of the background stratospheric aerosol. with peak extinctions up to 10−2 km−1. The PSCs were observed when stratospheric temperatures were very low with a high probability of observation when temperatures were colder than 190 K and a low probability when temperatures were warmer than 198 K. In the Antarctic, clouds were observed in more than 90% of the events in which the minimum temperature was 185 K or less, and were observed in fewer than 10% of the occasions when the temperature was ...

Satellite Studies of the Stratospheric Aerosol

Abstract The potential climatological and environmental importance of the stratospheric aerosol layer has prompted great interest in measuring the properties of this aerosol. In this paper we report on two recently deployed NASA satellite systems (SAM II and SAGE) that are monitoring the stratospheric aerosol. The satellite orbits are such that nearly global coverage is obtained. The instruments mounted in the space-craft 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. The data obtained are “inverted” to yield vertical aerosol and gaseous (primarily ozone) extinction profiles with 1 km vertical resolution. Thus, latitudinal, longitudinal, and temporal variations in the aerosol layer can be evaluated. The satellite systems are being validated by a series of ground truth experiments using airborne and ground lidar, balloon-borne dustsondes, aircraft-mounted impactor...

The Formation of Polar Stratospheric Clouds

Abstract Measurements of the stratospheric aerosol by SAM II during the northern and southern winters of 1979 showed a pronounced increase in extinction on occasions when the temperature fell to a low value (below 200 K). In this paper we evaluate, from thermodynamic considerations, the correlation between extinction and temperature. As the temperature fails, the hygroscopic aerosols absorb water vapor from the atmosphere, growing as they do so. The effect of the temperature on the size distribution and composition of the aerosol is determined, and the optical extinction at 1 μm wavelength is calculated using Mie scattering theory. The theoretical predictions of the change in extinction with temperature and humidity am compared with the SAM II results at 100 mb, and the water vapor mixing ratio and aerosol number density are inferred from these results. A best fit of the theoretical curves to the SAM II data gives a water vapor content of 5–6 ppmv, and a total particle number density of 6–7 particles cm−3.

Microphysical Processes Affecting Stratospheric Aerosol Particles

Abstract Physical processes which affect stratospheric aerosol particles include nucleation, condensation, evaporation, coagulation and sedimentation. We carry out quantitative studies of these mechanisms to determine if they can account for some of the observed properties of the aerosol. We show that the altitude range in which nucleation of H2SO4-H2O solution droplets can take place corresponds to that region of the stratosphere where the aerosol is generally found. Since heterogeneous nucleation is the dominant nucleation mechanism, the stratospheric solution droplets are mainly formed on particles which have been mixed up from the troposphere or injected into the stratosphere by volcanoes or meteorites. Particle growth by heteromolecular condensation can account for the observed increase in mixing ratio of large particles in the stratosphere. Coagulation is important in reducing the number of particles smaller than 0.05 µm radius. Growth by condensation, applied to the mixed nature of the particles, s...

The life cycle of stratospheric aerosol particles

This paper describes the life cycle of the background (nonvolcanic) stratospheric sulfate aerosol. The authors assume the particles are formed by homogeneous nucleation near the tropical tropopause and are carried aloft into the stratosphere. The particles remain in the Tropics for most of their life, and during this period of time a size distribution is developed by a combination of coagulation, growth by heteromolecular condensation, and mixing with air parcels containing preexisting sulfate particles. The aerosol eventually migrates to higher latitudes and descends across isentropic surfaces to the lower stratosphere. The aerosol is removed from the stratosphere primarily at mid- and high latitudes through various processes, mainly by isentropic transport across the tropopause from the stratosphere into the troposphere.

A new parameterization of H2SO4/H2O aerosol composition: Atmospheric implications

Recent results from a thermodynamic model of aqueous sulfuric acid are used to derive a new parameterization for the variation of sulfuric acid aerosol composition with temperature and relative humidity. This formulation is valid for relative humidities above 1% in the temperature range of 185 to 260 K. An expression for calculating the vapor pressure of supercooled liquid water, consistent with the sulfuric acid model, is also presented. We show that the Steele and Hamill [1981] formulation underestimates the water partial pressure over aqueous H2SO4 solutions by up to 12% at low temperatures. This difference results in a corresponding underestimate of the H2SO4 concentration in the aerosol by about 6% of the weight percent at approximately 190 K. In addition, the relation commonly used for estimating the vapor pressure of H2O over supercooled liquid water differs by up to 10% from our derived expression. The combined error can result in a 20% underestimation of water activity over a H2SO4 solution droplet in the stratosphere, which has implications for the parameterization of heterogeneous reaction rates in stratospheric sulfuric acid aerosols. The influence of aerosol composition on the rate of homogeneous ice nucleation from a H2SO4 solution droplet is also discussed. This parameterization can also be used for homogeneous gas phase nucleation calculations of H2SO4 solution droplets under various environmental conditions such as in aircraft exhaust or in volcanic plumes.

The vertical structure and thickness of Saturn's rings

Abstract We have considered the steady state vertical structure of Saturns rings with regard to whether collapse to a monolayer due to collisions between particles, the end state predicted by Jeffreys (1947a), may be prevented by any of a variety of mechanisms. Given a broad distribution of particle sizes such as a typical power law n ( R ) = n 0 R −3 , it is found that gravitational scattering of small particles by large particles maintains a true ring thickness of several times the radius of the largest particles, or many times the radius of the smallest particles. Thus the “many-particle-thick” condition which best satisfies optical observations, such as the opposition effect, may be reconciled with ongoing particle collisions. If we consider the obvious sources of energy available for such a process, we find that a ring thickness of only tens of meters may be sustained over the lifetime of the solar system. This implies a maximum particle size on the order of a few meters.

Dependence of aerosol light absorption and single‐scattering albedo on ambient relative humidity for sulfate aerosols with black carbon cores

Atmospheric aerosols frequently contain hygroscopic sulfate species and black carbon (soot) inclusions. In this paper we report results of a modeling study to determine the change in aerosol absorption due to increases in ambient relative humidity (RH), for three common sulfate species, assuming that the soot mass fraction is present as a single concentric core within each particle. Because of the lack of detailed knowledge about various input parameters to models describing internally mixed aerosol particle optics, we focus on results that were aimed at determining the maximum effect that particle humidification may have on aerosol light absorption. In the wavelength range from 450 to 700 nm, maximum absorption humidification factors (ratio of wet to “dry = 30% RH” absorption) for single aerosol particles are found to be as large as 1.75 when the RH changes from 30 to 99.5%. Upon lesser humidification from 30 to 80% RH, absorption humidification for single particles is only as much as 1.2, even for the most favorable combination of initial (“dry”) soot mass fraction and particle size. Integrated over monomodal lognormal particle size distributions, maximum absorption humidification factors range between 1.07 and 1.15 for humidification from 30 to 80% and between 1.1 and 1.35 for humidification from 30 to 95% RH for all species considered. The largest humidification factors at a wavelength of 450 nm are obtained for “dry” particle size distributions that peak at a radius of 0.05 μm, while the absorption humidification factors at 700 nm are largest for “dry” size distributions that are dominated by particles in the radius range of 0.06 to 0.08 μm. Single-scattering albedo estimates at ambient conditions are often based on absorption measurements at low RH (∼30%) and the assumption that aerosol absorption does not change upon humidification (i.e., absorption humidification equal to unity). Our modeling study suggests that this assumption alone can introduce absolute errors in estimates of the midvisible single-scattering albedo of up to 0.05 for realistic dry particle size distributions. Our study also indicates that this error increases with increasing wavelength. The potential errors in aerosol single-scattering albedo derived here are comparable in magnitude and in addition to uncertainties in single-scattering albedo estimates that are based on measurements of aerosol light absorption and scattering.

On the growth of nitric and sulfuric acid aerosol particles under stratospheric conditions

We present a theory for the formation of frozen aerosol particles in the Antarctic stratosphere, the coldest region of the Earths stratosphere. The theory is applied specifically to the formation of polar stratospheric clouds. We suggest that the condensed ices are composed primarily of nitric acid and water with small admixtures of other compounds such as H2SO4 and HCl in solid solution. Our assumed particle formation mechanism is in agreement with the magnitude and seasonal behavior of the optical extinctions observed in the winter polar stratosphere. Physical chemistry and thermodynamic considerations suggest that at temperatures between about 200 and 185 K, stratospheric particulates are composed primarily of frozen nitric acid solutions with a composition near that of the trihydrate. Available data suggest the particles are amorphous solid solutions and not in the crystalline hydrate form. At lower temperatures (i.e., below the forst point of pure water) cirrus-like ice clouds can form.

The Nucleation of H2SO4-H2O Solution Aerosol Particles in the Stratosphere

Abstract The homogeneous- and heterogeneous-heteromolecular nucleation of H2SO4-H2O solution droplets in the stratosphere is investigated and order-of-magnitude nucleation rates are evaluated. The heterogeneous processes considered are nucleation (i) onto soluble particles, (ii) onto flat insoluble surfaces, (iii) onto spherical insoluble particles and (iv) onto ions. The relative importance of the various nucleation mechanisms is determined for conditions assumed to correspond to 18 km altitude. Under the assumed conditions the heterogeneous nucleation rate onto insoluble particles is shown to be about 1069 times larger than the homogeneous nucleation rate and 1057 times larger than nucleation onto ions.