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Tabazadeh, Azadeh

Publications and source records attributed to Tabazadeh, Azadeh.

Observational Evidence Against Mountain-Wave Generation of Ice Nuclei as a Prerequisite for the Formation of Three Solid Nitric Acid Polar Stratospheric Clouds Observed in the Arctic in Early December 1999

A number of recently published papers suggest that mountain-wave activity in the stratosphere, producing ice particles when temperatures drop below the ice frost point, may be the primary source of large NAT particles. In this paper we use measurements from the Advanced Very High Resolution Radiometer (AVHRR) instruments on board the National Oceanic and Atmospheric Administration (NOAA) polar-orbiting satellites to map out regions of ice clouds produced by stratospheric mountain-wave activity inside the Arctic vortex. Lidar observations from three DC-8 flights in early December 1999 show the presence of solid nitric acid (Type Ia or NAT) polar stratospheric clouds (PSCs). By using back trajectories and superimposing the position maps on the AVHRR cloud imagery products, we show that these observed NAT clouds could not have originated at locations of high-amplitude mountain-wave activity. We also show that mountain-wave PSC climatology data and Mountain Wave Forecast Model 2.0 (MWFM-2) raw hemispheric ray and grid box averaged hemispheric wave temperature amplitude hindcast data from the same time period are in agreement with the AVHRR data. Our results show that ice cloud formation in mountain waves cannot explain how at least three large scale NAT clouds were formed in the stratosphere in early December 1999.

MOUNTAIN WAVES↗

Interesting Scientific Questions Regarding Interactions in the Gas-aerosol-cloud System

The growth of human population and their use of land, food and energy resources affect the Earth's atmosphere, biosphere and oceans in a complex manner. Many important questions in earth sciences today deal with issues regarding the impact of human activities on our immediate and future environment, ranging in scope from local (i.e. air pollution) to global (i.e. global warming) scale problems. Because the mass of the Earth's atmosphere is negligible compare to that found in the oceans and the biosphere, the atmosphere can respond quickly to natural and/or manmade perturbations. For example, seasonal 'ozone hole' formation in the Antarctic is a result of manmade CFC emissions in just the last 40 years. Also, the observed rise in global temperatures (known as global warming) is linked to a rapid increase in carbon dioxide and other greenhouse gas concentrations (emitted primarily by combustion processes) over the last century. The Earth's atmosphere is composed of a mixture of gases, aerosol and cloud particles. Natural and anthropogenic emissions of gases and aerosols affect the composition of the Earth's atmosphere. Changes in the chemical and physical makeup of the atmosphere can influence how the Earth will interact with the incoming solar radiation and the outgoing infrared radiation and vise versa. While, some perturbations are short-lived, others are long-lived and can affect the Earth's global climate and chemistry in many decades to come, In order to be able to separate the natural effects from anthropogenic ones, it is essential that we understand the basic physics and chemistry of interactions in the gas-aerosol-cloud system in the Earth's atmosphere. The important physics and chemistry that takes place in the coupled gas-aerosol-cloud system as it relates to aircraft observations are discussed.

Tabazadeh, Azadeh↗

Surface Crystallization of Supercooled Water in Clouds

The process by which liquid cloud droplets homogeneously crystallize into ice is still not well-understood. The ice nucleation process based on the standard and classical theory of homogeneous freezing, initiates within the interior volume of a cloud droplet. Current experimental data on homogeneous freezing rates of ice in droplets of supercooled water, both in air and emulsion oil samples, show considerable scatter. For example, at -33 C, the reported volume-based freezing rates of ice in supercooled water vary by as much as 5 orders of magnitude, which is well outside the range of measurement uncertainties. Here, we show that the process of ice nucleus formation at the air (or oil)-liquid water interface may help to explain why experimental results on ice nucleation rates yield different results in different ambient phases. Our results also suggest that surface crystallization of ice in cloud droplets can explain why low amounts of supercooled water have been observed in the atmosphere near -40 C.

Tabazadeh, Azadeh↗

Volcanoes, Polar Clouds and Arctic Ozone

Satellite observations and model calculations show 5 to 10% local column ozone loss in some tropical and mid latitude locations, following El Chichon and Mount Pinatubo eruptions. The rapid deepening of the Antarctic ozone hole in the early 1980s has also been partially attributed to chemistry on volcanic aerosols from a number of large eruptions. Here the effects of volcanoes on Arctic polar processes are explored. Large polar stratospheric cloud particles that cause denitrification cannot form in a volcanically perturbed environment. Denitrification can increase Arctic ozone loss by up to 30% in a future colder climate. However, we show that enhanced chemical processing on volcanic aerosols can increase Arctic ozone loss in a cold year by about 60% independent of denitrification. A coupled chemistry-microphysics model is used to show that widespread distribution of volcanic aerosols in 2000 could have caused severe springtime ozone depletion in the Arctic stratosphere. While, volcanic aerosols can strongly affect the current Arctic column ozone abundance in a cold year, denitrification effects on ozone can only become important in a much colder lower stratosphere.

Tabazadeh, Azadeh↗

Simulations of Polar Stratospheric Clouds and Denitrification Using Laboratory Freezing Rates

During the 1999-2000 Arctic winter, the SAGE (Stratospheric Aerosol and Gas Experiment) III Ozone Loss and Validation Experiment (SOLVE) provided evidence of widespread solid-phase polar stratospheric clouds (PSCs) accompanied by severe nitrification. Previous simulations have shown that a freezing process occurring at temperatures above the ice frost point is necessary to explain these observations. In this work, the nitric acid freezing rates measured by Salcedo et al. and discussed by Tabazadeh et al. have been examined. These freezing rates have been tested in winter-long microphysical simulations of the 1999-2000 Arctic vortex evolution in order to determine whether they can explain the observations. A range of cases have been explored, including whether the PSC particles are composed of nitric acid dihydrate or trihydrate, whether the freezing process is a bulk process or occurs only on the particle surfaces, and uncertainties in the derived freezing rates. Finally, the possibility that meteoritic debris enhances the freezing rate has also been examined. The results of these simulations have been compared with key PSC and denitrification measurements made by the SOLVE campaign. The cases that best reproduce the measurements will he highlighted, with a discussion of the implications for our understanding of PSCs.

Drdla, Katja↗

Simulations of the Vertical Redistribution of HNO3 by NAT or NAD PSCs: The Sensitivity to the Number of Cloud Particles Formed and the Cloud Lifetime

Recent satellite and in situ measurements have indicated that limited denitrification can occur in the Arctic stratosphere. In situ measurements from the SOLVE campaign indicate polar stratospheric clouds (PSCs) composed of small numbers (about 3 x 10^ -4 cm^-3) of 10-20 micron particles (probably NAT or NAD). These observations raise the issue of whether low number density NAT PSCs can substantially denitrify the air with reasonable cloud lifetimes. In this study, we use a one dimensional cloud model to investigate the verticle redistribution of HNO3 by NAT/NAD PSCs. The cloud formation is driven by a temperature oscillation which drops the temperature below the NAT/NAD formation threshold (about 195 K) for a few days. We assume that a small fraction of the available aerosols act as NAT nuclei when the saturation ratio of HNO3 over NAT(NAD) exceeds 10(l.5). The result is a cloud between about 16 and 20 km in the model, with NAT/NAD particle effective radii as large as about 10 microns (in agreement with the SOLVE data). We find that for typical cloud lifetimes of 2-3 days or less, the net depletion of HNO3 is no more than 1-2 ppbv, regardless of the NAT or NAD particle number density. Repeated passes of the air column through the cold pool build up the denitrification to 3-4 ppbv, and the cloud altitude steadily decreases due to the downward transport of nitric acid. Increasing the cloud lifetime results in considerably more effective denitrification, even with very low cloud particle number densities. As expected, the degree of denitrification by NAT clouds is much larger than that by NAD Clouds. Significant denitrification by NAD Clouds is only possible if the cloud lifetime is several days or more. The clouds also cause a local maximum HNO3 mixing ratio at cloud base where the cloud particles sublimate.

Jensen, Eric J.↗

Stratospheric Cooling and Arctic Ozone Recovery

We present sensitivity studies using the AER box model for an idealized parcel in the lower stratosphere at 70 deg N during winter/spring with different assumed stratospheric cooling and chlorine loadings. Our calculations show that stratospheric cooling could further deplete ozone via increased polar stratospheric cloud (PSC) formation and retard its expected recovery even with the projected chlorine loading decrease. We introduce the concept of chlorine-cooling equivalent and show that a 1 K cooling could provide the same local ozone depletion as an increase of chlorine by 0.4 - 0.7 ppbv for the scenarios considered. Thus, sustained stratospheric cooling could further reduce Arctic ozone content and delay the anticipated ozone recovery in the Northern Hemisphere even with the realization of the Montreal Protocol and its Amendments.

Danilin, Michael Y.↗

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 H2SOI 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.

Tabazadeh, Azadeh↗

A model for studying the composition and chemical effects of stratospheric aerosols

We developed polynomial expressions for the temperature dependence of the mean binary and water activity coefficients for H2SO4 and HNO3 solutions. These activities were used in an equilibrium model to predict the composition of stratospheric aerosols under a wide range of environmental conditions. For typical concentrations of H2O, H2SO4, HNO3, HCl, HBr, HF, and HOCl in the lower stratosphere, the aerosol composition is estimated as a function of the local temperature and the ambient relative humidity. For temperatures below 200 K, our results indicate that (1) HNO3 contributes a significant mass fraction to stratospheric aerosols, and (2) HCl solubility is considerably affected by HNO3 dissolution into sulfate aerosols. We also show that, in volcanically disturbed periods, changes in stratospheric aerosol composition can significantly alter the microphysics that leads to the formation of polar stratospheric clouds. The effects caused by HNO3 dissolution on the physical and chemical properties of stratospheric aerosols are discussed.

Tabazadeh, Azadeh↗

A model for heterogeneous chemical processes on the surfaces of ice and nitric acid trihydrate particles

The study presents a model that incorporates the physics and physical chemistry of ice surfaces relevant to polar stratospheric clouds. Surface concentrations of H2O, HCl, HOCl, ClONO2, and N2O5 on ice and nitric acid trihydrate (NAT) crystals are computed, and surface reaction rates and reaction probabilities (sticking coefficients) are determined. For gas pressures of about 10 exp -7 torr and temperatures in the range of 180-200 K, HCl completely coats ice and water-rich NAT surfaces, while HOCl, ClOHO2, and N2O5 may cover 0.01-1 percent of these surfaces. The energy parameters are used to calculate surface temperatures such as adsorption and desorption constants, surface coverages, reaction rate coefficients, surface diffusion coefficients, and reaction probabilities for various species and chemical interactions on ice and NAT surfaces. Implications for chemical processing on polar stratospheric clouds are discussed.

Tabazadeh, Azadeh↗