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At least 307 records · Page 17

Effect of lightning on the concentration of odd nitrogen species in the lower stratosphere: An update

Revised model estimates of the effect of lightning on the lower stratospheric NOy are presented. Several changes in the Atmospheric and Environmental Research Incorporated model were made since the last evaluation of the impact of lightning. Improvements were made in the model circulation and location of tropopause in the tropics, which is now calculated from the National Meteorological Center temperature data. Changes in model circulation reduced the mass flux from the troposphere to the tropical stratosphere. The calculated mass fluxes are found to agree better with some recent estimates. The circulation changes also reduced the advective mass flux from the tropical lower stratosphere to the midlatitudes. The change in circulation and the change in the tropopause height lead to increases in the calculated concentration of N2O, O3 and NOy in the tropical lower stratosphere. The effect of lightning is to increase the calculated concentration of NOy around 64 mbar by a factor of 2, compared to a factor of 10 enhancement in the previous calculations. Comparison with the Stratosphere Troposphere Exchange Project 1987 data indicates that the inclusion of a lightning source brings the model results in closer agreement with the observations.

Kotamarthi, V. R.↗

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.↗

Evolution of the stratosphere during northern winter 1991/92 as diagnosed from U.K. Meteorological Office analyses

Meteorological analyses, produced at the U.K. Meteorological Office by data assimilation, are used to study the circulation of the stratosphere in the Northern Hemisphere during winter 1991/92. The analyses are supplemented by Lagrangian visualizations of the circulation. The main features discussed are (1) the changes in vertical structure of the circulation, (2) the merger of anticyclones that precipitated a strong stratospheric warming, (3) vortex roll up in the upper stratosphere, (4) the entrainment of air into the polar vortex in the middle and upper stratosphere, and (5) the influence of tropospheric blocking on the lower stratosphere. The study provides a meteorological basis for the interpretation of data from the Upper Atmosphere Research Satellite (UARS).

O'Neill, Alan↗

Simulation of stratospheric N2O in the NCAR CCM2: Comparison with CLAES data and global budget analyses

Global variability and budgets of stratospheric nitrous oxide (N2O) are studied using output from a stratospheric version of the National Center for Atmospheric Research Climate Model (CCM2). The model extends over 0-80 km, incorporating an N2O-like tracer with tropospheric source and upper-stratospheric photochemical sink, the latter parameterized using linear damping rates obtained from detailed two-dimensional model calculations. Results from the model over several seasonal cycles are compared with observations of N2O from the Cryogenic Limb Array Etalon Spectrometer (CLAES) instrument on the Upper Atmosphere Research Satellite (UARS). The model produces N2O structure and variability that is in reasonable agreement with the observations. Global budgets of stratospheric N2O are furthermore analyzed using model output, based on the transformed Eulerian-mean, zonal-mean framework. These budgets are used to quantify the importance of planetary wave constituent transport in the stratosphere, for both slow seasonal variations and fast planetary wave events. These results demonstrate that such wave fluxes act to form and sharpen the strong subtropical N2O gradients observed in satellite measurements.

Randel, William J.↗

Altitude dependence of stratospheric ozone trends based on Nimbus 7 SBUV data

A multiple regression statistical model is applied to estimate the altitude, latitude, and seasonal dependences of stratospheric ozone trends using 11.5 years of Nimbus 7 SBUV data for the period November 1978 to June 1990. In the upper stratosphere, the derived trends agree in both latitude dependence and approximate amplitude with published predictions from stratospheric models that consider gas-phase chemical processes together with the observed approx. 0.1 ppbV per year increase in tropospheric chlorine. The dominant contribution to column ozone trends occurs in the lower stratosphere where significant negative trends are present at latitudes greater than 20 deg in both hemispheres. The observed latitude dependence is qualitatively consistent with model predictions that include the effects of heterogeneous chemical ozone losses on lower stratospheric aerosols.

Hood, Lon L.↗

Global variations of zonal mean ozone during stratospheric warming events

Eight years of Solar Backscatter Ultraviolet (SBUV) ozone data are examined to study zonal mean variations associated with stratospheric planetary wave (warming) events. These fluctuations are found to be nearly global in extent, with relatively large variations in the tropics, and coherent signatures reaching up to 50 deg in the opposite (summer) hemisphere. These ozone variations are a manifestation of the global circulation cells associated with stratospheric warming events; the ozone responds dynamically in the lower stratosphere to transport, and photochemically in the upper stratosphere to the circulation-induced temperature changes. The observed ozone variations in the tropics are of particular interest because transport is dominated by zonal-mean vertical motions (eddy flux divergences and mean meridional transports are negligible), and hence, substantial simplifications to the governing equations occur. The response of the atmosphere to these impulsive circulation changes provides a situation for robust estimates of the ozone-temperature sensitivity in the upper stratosphere.

Randel, William J.↗

Relationship between ozone and temperature trends in the lower stratosphere: Latitude and seasonal dependences

A one-dimensional radiative transfer model with fixed dynamical heating is used to calculate the approximate latitude and seasonal dependences of lower stratospheric temperature changes associated with observed ozone trends. The spatial and temporal distribution of ozone profile trends in the lower stratosphere is estimated from a combination of Nimbus 7 Solar Backscattered Ultraviolet (SBUV) global measurements of the ozone column below 32 mbar for the period 1979-1990 and balloon ozonesonde profile trends at northern middle latitudes. The calculated temperature trends near 100 mbar compare favorably with those recently derived by Randel and Cobb (1994) using data from Channel 4 of the Microwave Sounding Unit (MSU) on the NOAA operational satellites, although a number of quantitative differences are found. An independent analysis reported here of 100 mbar temperatures derived from northern hemisphere radiosonde data at the Free University of Berlin (FUB) supports the validity of the satellite-derived lower stratospheric temperature trends. These results are therefore generally consistent with the hypothesis that observed lower stratospheric cooling trends are predominantly determined by reductions in radiative heating associated with stratospheric ozone depletion.

Mccormack, John P.↗

Towards a theory of tropical/midlatitude mass exchange from the earth's surface through the stratosphere

The main focus of this work is to understand the dynamics of mass exchange between the tropics and the midlatitudes and to determine any links between tropospheric exchange and that in the stratosphere. We have approached this problem from two different perspectives. The first is aimed towards understanding the troposphere's role in inducing lower stratospheric tropical/midlatitude exchange. For this project we focus on observational analysis of the lower stratosphere to assess the key regions of transport in/out of the tropics and to what extent this transport is driven by tropospheric processes. The second approach is to determine the extent to which stratospheric processes influence the troposphere. In this project we are performing potential vorticity (PV) inversions to assess the winds induced near the tropopause when the stratospheric polar vortex is displaced equatorward. These are each discussed in more detail in the subsections below. Also, we have organized a session on Tropical/Midlatitude Interaction and Transport at the Fall AGU where we will be showing our latest results.

Hartley, Dana↗

Interhemispheric differences in polar stratospheric HNO3, H2O, ClO, and O3

Simultaneous global measurements of nitric acid (HNO3), water (H2O), chlorine monoxide (ClO), and ozone (O3) in the stratosphere have been obtained over complete annual cycles in both hemispheres by the Microwave Limb Sounder on the Upper Atmosphere Research Satellite. A sizeable decrease in gas-phase HNO3 was evident in the lower stratospheric vortex over Antarctica by early June 1992, followed by a significant reduction in gas-phase H2O after mid-July. By mid-August, near the time of peak ClO, abundances of gas-phase HNO3 and H2O were extremely low. The concentrations of HNO3 and H2O over Antarctica remained depressed into November, well after temperatures in the lower stratosphere had risen above the evaporation threshold for polar stratospheric clouds, implying that denitrification and dehydration had occurred. No large decreases in either gas-phase HNO3 or H2O were observed in the 1992-1993 Arctic winter vortex. Although ClO was enhanced over the Arctic as it was over the Antarctic, Arctic O3 depletion was substantially smaller than that over Antarctica. A major factor currently limiting the formation of an Arctic ozone 'hole' is the lack of denitrification in the northern polar vortex, but future cooling of the lower stratosphere could lead to more intense denitrification and consequently larger losses of Arctic ozone.

Santee, M. L.↗

The post-pinatubo evolution of stratospheric aerosol surface area density as inferred from SAGE 2

Following the eruption of Mount Pinatubo in June of 1991, the aerosol mass loading of the stratosphere increased from -1 Mt to approximately 30 Mt. This change in aerosol loading was responsible for numerous radiative and chemical changes observed within the stratosphere. As a result, the ability to quantify aerosol properties on a global basis during this period is important. Aerosol surface area density is a critical parameter in governing the rates of heterogeneous reactions, such as ClONO2 plus H2O yields HNO3 plus HOCl, which influence the stratospheric abundance of ozone. Following the eruption of Mt. Pinatubo, measurements by the Stratospheric Aerosol and Gas Experiment (SAGE 2) indicated that the stratospheric aerosol surface area density increased by as much as a factor of 100. Using SAGE 2 multi-wavelength aerosol extinction data, aerosol surface area density as well as mass are derived for the period following the eruption of Mt. Pinatubo through the present.

Poole, L. R.↗

Seasonal Variations of Water Vapor in the Lower Stratosphere Inferred from ATMOS/ATLAS-3 Measurements of H2O and CH4

Stratospheric measurements of H2O and CH4 by the Atmospheric Trace Molecule Spectroscopy (ATMOS) Fourier transform spectrometer on the ATLAS-3 shuttle flight in November 1994 have been examined to investigate the altitude and geographic variability of H2O and the quantity H = (H2O + 2CH4) in the tropics and at mid-latitudes (8 to 49 deg N) in the northern hemisphere. The measurements indicate an average value of 7.24 +/- 0.44 ppmv for H between altitudes of about 18 to 35 km, corresponding to an annual average water vapor mixing ratio of 3.85 +/- 0.29 ppmv entering the stratosphere. The H2O vertical distribution in the tropics exhibits a wave-like structure in the 16- to 25-km altitude range, suggestive of seasonal variations in the water vapor transported from the troposphere to the stratosphere. The hygropause appears to be nearly coincident with the tropopause at the time of observations. This is consistent with the phase of the seasonal cycle of H2O in the lower stratosphere, since the ATMOS observations were made in November when the H2O content of air injected into the stratosphere from the troposphere is decreasing from its seasonal peak in July-August.

Abbas, M. M.↗

Stratospheric Observations of CH3D and HDO from ATMOS Infrared Solar Spectra: Enrichments of Deuterium in Methane and Implications for HD

Stratospheric mixing ratios of CH3D from 100 mb to 17mb (approximately equals 15 to 28 km)and HDO from 100 mb to 10 mb (approximately equals 15 to 32 km) have been inferred from high resolution solar occultation infrared spectra from the Atmospheric Trace MOlecule Spectroscopy (ATMOS) Fourier-transform interferometer. The spectra, taken on board the Space Shuttle during the Spacelab 3 and ATLAS-1, -2, and -3 missions, extend in latitude from 70 deg S to 65 deg N. We find CH3D entering the stratosphere at an average mixing ratio of (9.9 +/- 0.8) x 10(exp -10) with a D/H ratio in methane (7.1 +/- 7.4)% less than that in Standard Mean Ocean Water (SMOW) (1 sigma combined precision and systematic error). In the mid to lower stratosphere, the average lifetime of CH3D is found to be (1.19 +/- 0.02) times that of CH4, resulting in an increasing D/H ratio in methane as air 'ages' and the methane mixing ratio decreases. We find an average of (1.0 +/- 0.1) molecules of stratospheric HDO are produced for each CH3D destroyed (1 sigma combined precision and systematic error), indicating that the rate of HDO production is approximately equal to the rate of CH3D destruction. Assuming negligible amounts of deuterium in species other than HDO, CH3D and HD, this limits the possible change in the stratospheric HD mixing ratio below about 10 mb to be +/- 0.1 molecules HD created per molecule CH3D destroyed.

Irion, F. W.↗

Seasonal Variations of Water Vapor in the Lower Stratosphere Inferred from ATMOS/ATLAS-3 Measurements of H2O and CH4

Stratospheric measurements of H2O and CH4 by the Atmospheric Trace Molecule Spectroscopy (ATMOS) Fourier transform spectrometer on the ATLAS-3 shuttle flight in November 1994 have been examined to investigate the altitude and geographic variability of H2O and the quantity H = (H2O + 2CH4) in the tropics and at mid-latitudes (8 to 49 deg N) in the northern hemisphere. The measurements indicate an average value of 7.24 plus or minus 0.44 ppmv for H between altitudes of about 18 to 35 km, corresponding to an annual average water vapor mixing ratio of 3.85 plus or minus 0.29 ppmv entering the stratosphere. The H2O vertical distribution in the tropics exhibits a wave-like structure in the 16- to 25-km altitude range, suggestive of seasonal variations in the water vapor transported from the troposphere to the stratosphere. The hygropause appears to be nearly coincident with the tropopause at the time of observations. This is consistent with the phase of the seasonal cycle of H2O in the lower stratosphere, since the ATMOS observations were made in November when the H2O content of air injected into the stratosphere from the troposphere is decreasing from its seasonal peak in July - August.

Abbas, M. M.↗

Heterogeneous Interactions of ClONO2 and HCl with Sulfuric Acid Tetrahydrate: Implications for the Stratosphere

The reaction probabilities for ClONO2+H2O- HOCl + HNO3 and ClONO2+ HCl Cl2 +HNO3 have been investigated on sulfuric acid tetrahydrate (SAT, H2SO4-4H2O)surfaces at temperatures between 190 and 230 K and at reactant concentrations that are typical in the lower stratosphere, using a fast-flow reactor coupled to a quadrupole mass spectrometer. The results indicate that the reaction probabilities as well as HCl uptake depend strongly on the thermodynamic state of SAT surface: they decrease significantly with decreasing H2O partial pressure at a given temperature, and decrease with increasing temperature at a given H2O partial pressure, as the SAT changes from the H2O-rich form to the H2SO4-rich form. For H2O-rich SAT at 195 K gamma(sub 1) approx. = -0.01 and gamma(sub 2) greater or equal to 0.1, whereas the values for H2SO4-rich SAT decrease by more than 2 orders of magnitude. At low concentrations of HCl, close to those found in the stratosphere, the amount of HCl taken up by H2O-rich SAT films corresponds to a coverage of the order of a tenth of a monolayer (approx. = 10(exp 14) molecules/sq cm); H2SO4-rich SAT films take up 2 orders of magnitude less HCl (les than 10(exp 12) molecules/sq cm). Substantial HCl uptake at high HCl concentrations is also observed, as a result of surface melting. The data reveal that frozen stratospheric sulfate aerosols may play an important role in chlorine activation in the winter polar stratosphere via processes similar to those occurring on the surfaces of polar stratospheric cloud particles.

Zhang, Renyi↗

Prediction of Dynamical Impact of Changes in Stratospheric Ozone

Under this grant one paper by Lou et al and a second paper by Kindler et al is in journal. These papers both describe N2O simulations using UKMO and Goddard assimilated wind fields and comparisons of the results against CLAES N2O observations. The results of these studies indicate some of the difficulties of using the assimilated wind fields, and the vertical motions in particular, in simulating long term variations in trace gases in the stratosphere. On the other hand, qualitatively the results possess a number of features of the observations even on time scales longer than a month or two. More recently we have started to examine results obtained using NCAR models a 3D version of which also uses the UKMO assimilated wind fields. Calculations have already been made with their 2D model with emphasis on the seasonal cycle in ozone at high latitudes in the upper stratosphere. Simultaneously trends in stratospheric ozone have been studied in detail from SAGE and UARS observations. Moreover, observations of the trends since 1984 do not show a significant interhemispheric asymmetry in upper stratospheric ozone. Therefore any asymmetry in the trends must have occurred prior to the mid-eighties and would most likely have been related to interhemispheric differences in upper stratospheric temperature trends. Another activity has been to compile an ozone climatology from UARS and SAGE observations. This effort has been performed as part of a UARS team activity to assemble a climatology of all the UARS long-lived trace gases for 1992-1993.

Cunnold, Derek M.↗

Bismuth Oxide Nanoparticles in the Stratosphere

Platey grains of cubic Bi2O3, alpha-Bi2O3, and Bi2O(2.75), nanograins were associated with chondritic porous interplanetary dust particles W7029C1, W7029E5, and 2011C2 that were collected in the stratosphere at 17-19 km altitude. Similar Bi oxide nanograins were present in the upper stratosphere during May 1985. These grains are linked to the plumes of several major volcanic eruptions during the early 1980s that injected material into the stratosphere. The mass of sulfur from these eruptions is a proxy for the mass of stratospheric Bi from which we derive the particle number densities (p/cu m) for "average Bi2O3 nanograins" due to this volcanic activity and those necessary to contaminate the extraterrestrial chondritic porous interplanetary dust particles via collisional sticking. The match between both values supports the idea that Bi2O3 nanograins of volcanic origin could contaminate interplanetary dust particles in the Earth's stratosphere.

Rietmeijer, Frans J. M.↗

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 N during winter/spring with different assumed stratospheric coolings 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.↗

Physical and Chemical Characterization of Particles in the Upper Troposphere and Lower Stratosphere: Microanalysis of Aerosol Impactor Samples

Herein is reported activities to support the characterization of the aerosol in the upper troposphere (UT) and lower stratosphere (LS) collected during the Airborne Southern Hemisphere Ozone Experiment/Measurements for Assessing the Effects of Stratospheric Aircraft (ASHOE/MAESA) missions in 1994. Through a companion proposal, another group was to measure the size distribution of aerosols in the 0.008 to 2 micrometer diameter range and to collect for us impactor samples of particles larger than about 0.02 gm. In the first year, we conducted laboratory studies related to particulate deposition patterns on our collection substrates, and have performed the analysis of many ASHOE/MAESA aerosol samples from 1994 using analytical electron microscopy (AEM). We have been building an "aerosol climatology" with these data that documents the types and relative abundances of particles observed at different latitudes and altitudes. The second year (and non-funded extension periods) saw continued analyses of impactor aerosol samples, including more ASHOE/MAESA samples, some northern hemisphere samples from the NASA Stratospheric Photochemistry Aerosols and Dynamics Expedition (SPADE) program for comparison, and a few aerosol samples from the NASA Stratospheric TRacers of Atmospheric Transport (STRAT) program. A high-resolution field emission microscope was used for the analysis and re-analysis of a number of samples to determine if this instrument was superior in performance to our conventional electron microscope. In addition, some basic laboratory studies were conducted to determine the minimum detectable and analyzable particle size for different types of aerosols. In all, 61 aerosol samples were analyzed, with a total of over 30,000 individual particle analyses. In all analyzed samples, sulfate particles comprised the major aerosol number fraction. It must be stressed that particles composed of more than one species, for example sulfate and organic carbon, were classified according to the major fraction. Thus, many of the particles classified as sulfate may have contained significant mass fractions of carbonaceous or other material. These particles for the most part did not show two physical phases, however. Nonsulfate particles were classified according to the physical and chemical characteristics of each particle, and were grouped into the major nonsulfate particle classes, including C-rich, crustal, metallic, and salts. Our UT and LS sample analyses indicate a maximum for crustal and C-rich particle abundance in the Northern Hemisphere upper troposphere, and a salt particle maximum in the Southern Hemisphere upper troposphere. Metallic particles are clearly more prevalent in the troposphere than in the stratosphere, but interhemispheric differences appear small.

Sheridan, Patrick J.↗