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At least 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
NASA NTRS1990

Ground-based lidar measurements of stratospheric ozone. The NASA/GSFC stratospheric ozone lidar trailer experiment STROZ LITE

The major research objective is the measurement of high precision vertical profiles of ozone between 20-40 kilometers. The precision is such that the instrument should be capable of detecting a small trend (on the order of less that 1 percent per year) over a 5-10 year period. Temperature was measured between 30 and 365 km. The Goddard Space Flight Center (GSFC) mobile lidar was installed at Table Mountain and a comparison between it and the permanent Jet Propulsion Laboratory (JPL) lidar was made over the course of about 3 weeks. The lidars agreed very well between 20 and 40 km, and under certain conditions up to 45-47 km. There were several anomalies that both lidars followed very well. Agreement with Rocket Ozonesonde (ROCOZ) and electrochemical concentration cell (ECC) sondes was also very good.

Mcgee, Thomas J.↗
NASA NTRS1994

Counting Particles Emitted by Stratospheric Aircraft and Measuring Size of Particles Emitted by Stratospheric Aircraft

There were two principal objectives of the cooperative agreement between NASA and the University of Denver. The first goal was to modify the design of the ER-2 condensation nuclei counter (CNC) so that the effective lower detection limit would be improved at high altitudes. This improvement was sought because, in the instrument used prior to 1993, diffusion losses prevented the smallest detectable particles from reaching the detection volume of the instrument during operation at low pressure. Therefore, in spite of the sensor's ability to detect particles as small as 0.008 microns in diameter, many of these particles were lost in transport to the sensing region and were not counted. Most of the particles emitted by aircraft are smaller than 0.1 micron in diameter. At the start date of this work, May 1990, continuous sizing techniques available on the ER-2 were only capable of detecting particles larger than 0.17 micron. Thus, the second objective of this work was to evaluate candidate sizing techniques in an effort to gain additional information concerning the size of particles emitted by aircraft.

Wilson, James Charles↗
NASA NTRS2000

A Simulation of Bromoform's Contribution to Stratospheric Bromine

Many chlorinated and brominated compounds that are inert in the troposphere are destroyed in the stratosphere and act as an in-situ source of stratospheric reactive chlorine and bromine. Other halogenated compounds that are reactive in the troposphere might contribute to the stratosphere's halogen budget in two ways. First, like their unreactive companions, rapid convective transport might carry them to the upper troposphere and make them available for subsequent advection by the mean circulation into the stratosphere before they are oxidized or photolyzed. Second, it is more likely that they are destroyed in the troposphere, and the chlorine and bromine that is released might then be transported to the stratosphere. We evaluate the relative influence of these processes on stratospheric bromine in a three-dimensional chemistry and transport model which simulates the distribution of bromoform (CHBr3). CHBr3 is parameterized as a short-lived, ocean-surface source gas whose destruction by photolysis and reaction with hydroxyl (OH) in the troposphere and stratosphere yields inorganic bromine (Br(sub y)). Many of the observed features of CHBr3 are simulated well, and comparisons with observations are used to show that the model represents aspects of transport in the upper troposphere and lower stratosphere that are critical to the evaluation. In particular, the model maintains the observed troposphere-stratosphere distinctness in transport pathways and reproduces the observed seasonal dependence of the mixture of air in the middle- and high-latitude lowermost stratosphere. We estimate that adding CHBr3 to models which already include the long-lived organic brominated compounds (halons and methyl bromide) will increase the simulated stratospheric mass of Br(sub y) by about 15 percent. In-situ stratospheric destruction of CHBr3 produces Br(sub y) in amounts which are comparable to that transported into the stratosphere after photolysis and oxidation of CHBr3 in the troposphere. In our simulations the mass of Br(sub y) produced from the destruction of CHBr3 does not exceed the mass of Br(sub y) produced from the destruction of the long-lived compounds at any level in the stratosphere. However, Br(sub y) from the loss of CHBr3 accounts for approximately one-third of the total Br(sub y) in the lowest kilometer of the stratosphere.

Nielsen, J. Eric↗
NASA NTRS1997

On the Relation between Stratospheric Chlorine/Bromine Loading and Short-Lived Tropospheric Source Gases

Current methods for estimating the concentrations of inorganic chlorine/bromine species Cl(y)/Br(y) in the stratosphere due to decomposition of tropospheric source gases assume that the Cl(y)/Br(y) concentration in the stratosphere is determined mainly by the balance between production from in situ oxidation of the source gases in the stratosphere and removal by transport of Cl(y)/Br(y) out of the stratosphere. The rationale being that for source gases whose lifetimes are of the order of several months or longer the concentration of Cl(y)/Br(y) in the troposphere is small because they are produced at a relatively slow rate and also removed efficiently by washout processes. As a result of the small concentration, the rate at which Cl(y)/Br(y) is transported to the stratosphere is expected to be small compared to the in situ stratospheric production. Thus the transport of Cl(y)/Br(y) from the troposphere contributes little to the stratospheric concentration. In contrast, the origin of stratospheric Cl(y)/Br(y) from reactive source gases with tropospheric lifetimes comparable to the washout lifetime of Cl(y)/Br(y) (of the order of 10-30 days) in the troposphere is distinctly different. The in situ source in the stratosphere is expected to be significantly smaller because only a small portion of the source gas is expected to survive the troposphere to be transported into this region. At the same time these short-lived source gases produce appreciable amounts of Cl(y)/Br(y) in the troposphere such that transport to the stratosphere offers a larger source for stratospheric Cl(y)/Br(y) than in situ production. Thus, for reactive source species, simple methods of estimating the concentration of stratospheric Cl(y)/Br(y) that ignore the tropospheric contribution will seriously underestimate the loading. Therefore estimation of the stratospheric Cl(y)/Br(y) loading requires not only measurements of tropospheric source gases but also measurements of Cl(y)/Br(y) at the tropopause. This paper illustrates the mechanism by using results from a two-dimensional chemistry-transport model. However, in view of the importance of tropospheric transport on stratospheric loading the detailed values should be further evaluated using a three-dimensional model with appropriate treatment of convective transport.

Ko, Malcolm K. W.↗
NASA NTRS2017

Stratospheric Instrusion Catalog: A 10-Year Compilation of Events Identified by using TRACK with NASA's MERRA-2 Reanalysis

Stratospheric intrusions "the introduction of ozone-rich stratospheric air into the troposphere" have been linked with surface ozone air quality exceedances, especially at the high elevations in the western USA in springtime. However, the impact of stratospheric intrusions in the remaining seasons and over the rest of the USA is less clear. A new approach to the study of stratospheric intrusions uses NASA's Goddard Earth Observing System Model (GEOS) model and assimilation products with an objective feature tracking algorithm to investigate the atmospheric dynamics that generate stratospheric intrusions and the different mechanisms through which stratospheric intrusions may influence tropospheric chemistry and surface air quality seasonally over both the western and the eastern USA. A catalog of stratospheric intrusions identified in the MERRA-2 reanalysis was produced for the period 2004-2015 and validated against surface ozone observations (focusing on those which exceed the national air quality standard) and a recent data set of stratospheric intrusion-influenced air quality exceedance flags from the US Environmental Protection Agency (EPA). Considering not all ozone exceedances have been flagged by the EPA, a collection of stratospheric intrusions can support air quality agencies for more rapid identification of the impact of stratospheric air on surface ozone and demonstrates that future operational analyses may aid in forecasting such events. An analysis of the spatiotemporal variability of stratospheric intrusions over the continental US was performed, and while the spring over the western USA does exhibit the largest number of stratospheric intrusions affecting the lower troposphere, the number of intrusions in the remaining seasons and over the eastern USA is sizable. By focusing on the major modes of variability that influence weather in the USA, such as the Pacific North American (PNA) teleconnection index, predicative meteorological patterns associated with stratospheric intrusions and their regional effects on tropospheric ozone were identified. Improved understanding of the connections between large-scale climate variability and local-scale dynamically-driven air quality events may support improved seasonal prediction of such events.

PN↗
NASA NTRS2022

Prescribing Stratospheric Chemistry Overestimates Southern Hemisphere Climate Change During Austral Spring in Response to Quadrupled CO2

The interaction of stratospheric chemistry with a changing climate from an abrupt CO2 quadrupling is assessed using the coupled atmosphere–ocean Goddard Earth Observing System Chemistry-Climate Model (GEOSCCM). Two abrupt 4 × CO2 experiments were performed, one with interactive stratospheric chemistry and the other with a prescribed stratospheric chemistry that does not simulate stratospheric ozone response to 4 × CO2. The interactive and prescribed chemistry experiments simulate similar global mean surface temperature change. Nevertheless, interactive chemistry is critical to capture the Southern Hemisphere tropospheric midlatitude jet response to 4 × CO2. When stratospheric ozone response to 4 × CO2 is neglected, GEOSCCM overestimates Southern Hemisphere tropospheric circulation change. This stratospheric chemistry-induced climate impact has large seasonal variability. During the austral spring season September–October–November (SON), prescribed chemistry yields a stronger poleward shift and intensification of the Southern Hemisphere midlatitude tropospheric jet, surface wind stress, and the Southern Ocean meridional overturning circulation than occurs with interactive chemistry. In other seasons interactive and prescribed chemistry have similar effects on the Southern Hemisphere circulation. The seasonality of stratospheric chemistry-induced climate impact is related to the seasonality of Antarctic lower stratospheric ozone response to 4 × CO2. In contrast to this stratospheric ozone response to 4 × CO2, stratospheric ozone recovery from decline of the ozone depleting substances has its largest impact on the Southern Hemisphere tropospheric circulation in austral summer (December–January–February), but no effects in SON. It is found that the different seasonality for these two stratospheric ozone layer change scenarios is related to the different seasonality of tropopause meridional temperature gradient response.

Stratospheric ozone feedback↗
NASA NTRS2024

Stratospheric Temperature and Ozone Impacts of the Hunga Tonga-Hunga Ha'apai Water Vapor Injection

The January 2022 eruption of the Hunga Tonga-Hunga Ha'apai underwater volcano injected a large amount of water vapor into the mid-stratosphere. This study uses model simulations to investigate the resulting stratospheric impacts out to 2031. Maximum radiatively-driven model temperature changes occur in the Southern Hemisphere (SH) subtropics in April–May 2022, with warming of ∼1 K in the lower stratosphere and cooling of 3 K in the mid-stratosphere. The radiative cooling combined with adiabatic cooling driven by the quasi-biennial oscillation meridional circulation explains the near-record cold anomaly observed in the SH subtropical mid-stratosphere. Projected ozone responses maximize in 2023–2024 as the water vapor plume is transported globally throughout the stratosphere and mesosphere. The excess H2O increases the OH radical, causing a negative global ozone response (2%–10%) in the upper stratosphere and mesosphere due to increased odd hydrogen-ozone loss, and a small positive ozone response (0.5%–1%) in the mid-stratosphere due to interference of the NOx catalytic loss cycle by the additional OH. In the lower stratosphere, the excess H2O is projected to increase polar stratospheric clouds and springtime halogen-ozone loss, enhancing the Antarctic ozone hole by 25–30 DU in 2023. Arctic impact is small, with maximum additional ozone loss of 4–5 DU projected in spring 2024. These responses diminish after 2024 to be quite small by 2031, as the excess H2O is removed from the stratosphere with a 2.5-year e-folding time. Given the year-to-year variability of the stratosphere, the magnitudes of these ozone responses may be below the threshold of detectability in observations.

stratosphere↗
NASA NTRS1998

Towards a Theory of Tropical/Midlatitude Mass Exchange from the Earth's Surface through the Stratosphere

The main findings of this research project have been the following: (1) there is a significant feedback from the stratosphere on tropospheric dynamics, and (2) a detailed analysis of the interaction between tropical and polar wave breaking in controlling stratospheric mixing. Two papers are were written and are included. The first paper is titled, "A New Perspective on the Dynamical Link Between the Stratosphere and Troposphere." Atmospheric processes of tropospheric origin can perturb the stratosphere, but direct feedback in the opposite direction is usually assumed to be negligible, despite the troposphere's sensitivity to changes in the release of wave activity into the stratosphere. Here, however, we present evidence that such a feedback exists and can be significant. We find that if the wintertime Arctic polar stratospheric vortex is distorted, either by waves propagating upward from the troposphere or by eastward-travelling stratospheric waves, then there is a concomitant redistribution of stratospheric potential vorticity that induces perturbations in key meteorological fields in the upper troposphere. The feedback is large despite the much greater mass of the troposphere: it can account for up to half of the geopotential height anomaly at the tropopause. Although the relative strength of the feedback is partly due to a cancellation between contributions to these anomalies from lower altitudes, our results imply that stratospheric dynamics and its feedback on the troposphere are more significant for climate modelling and data assimilation than was previously assumed. The second article is titled "Diagnosing the Polar Excitation of Subtropical Waves in the Stratosphere". The poleward migration of planetary scale tongues of subtropical air has often been associated with intense polar vortex disturbances in the stratosphere. This question of vortex influence is reexamined from a potential vorticity (PV) perspective. Anomalous geopotential height and wind fields associated solely with vortex PV anomalies are derived and their impact on the stratospheric subtropical circulation is evaluated. Combined PV inversion and Contour Advection (CA) calculations indicate that transient large scale disturbances of the polar vortex do have a far reaching impact that extends beyond the midlatitude surf zone all the way to the subtropics. This vortex influence is clearly non-local so that even simple wave 2 distortions that leave the vortex well confined within the midlatitudes are observed to excite subtropical waves. Treating subtropical PV as active tracers also showed that upon entrainment, these large scale tongues of low PV air also influenced the dynamics of their own poleward migration.

Hartley, Dana↗
DOE OSTI2025

Recent Warming of the Southern Hemisphere Subtropical Lower Stratosphere and Antarctic Ozone Healing

Observed temperature changes from 2002 to 2022 reveal a pronounced warming of the Southern Hemisphere (SH) subtropical lower stratosphere, and a cooling of the Antarctic lower stratosphere. In contrast, model simulations of 21st-century stratospheric temperature changes show widespread cooling driven by increasing greenhouse gases, with local warming in the Antarctic lower stratosphere due to ozone healing. We provide evidence that these discrepancies between observed and simulated stratospheric temperature changes are linked to a slowdown of the Brewer-Dobson Circulation, particularly in the SH. These changes in the stratospheric circulation are strongest from October through December. This altered circulation warms the SH subtropical lower stratosphere while cooling the Antarctic lower stratosphere, canceling and even reversing the Antarctic ozone recovery that would have occurred in its absence during this period. When circulation changes are accounted for, the SH subtropical lower-stratospheric warming is removed, and Antarctic lower-stratospheric warming is revealed with enhanced ozone healing, highlighting the crucial role of the stratospheric circulation in shaping temperature and ozone changes.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2014

Northern Winter Climate Change: Assessment of Uncertainty in CMIP5 Projections Related to Stratosphere-Troposphere Coupling

Future changes in the stratospheric circulation could have an important impact on northern winter tropospheric climate change, given that sea level pressure (SLP) responds not only to tropospheric circulation variations but also to vertically coherent variations in troposphere-stratosphere circulation. Here we assess northern winter stratospheric change and its potential to influence surface climate change in the Coupled Model Intercomparison Project-Phase 5 (CMIP5) multimodel ensemble. In the stratosphere at high latitudes, an easterly change in zonally averaged zonal wind is found for the majority of the CMIP5 models, under the Representative Concentration Pathway 8.5 scenario. Comparable results are also found in the 1% CO2 increase per year projections, indicating that the stratospheric easterly change is common feature in future climate projections. This stratospheric wind change, however, shows a significant spread among the models. By using linear regression, we quantify the impact of tropical upper troposphere warming, polar amplification, and the stratospheric wind change on SLP. We find that the intermodel spread in stratospheric wind change contributes substantially to the intermodel spread in Arctic SLP change. The role of the stratosphere in determining part of the spread in SLP change is supported by the fact that the SLP change lags the stratospheric zonally averaged wind change. Taken together, these findings provide further support for the importance of simulating the coupling between the stratosphere and the troposphere, to narrow the uncertainty in the future projection of tropospheric circulation changes.

climate change↗
NASA NTRS2005

The Remarkable 2003--2004 Winter and Other Recent Warm Winters in the Arctic Stratosphere Since the Late 1990s

The 2003-2004 Arctic winter was remarkable in the approximately 50-year record of meteorological analyses. A major warming beginning in early January 2004 led to nearly 2 months of vortex disruption with high-latitude easterlies in the middle to lower stratosphere. The upper stratospheric vortex broke up in late December, but began to recover by early January, and in February and March was the strongest since regular observations began in 1979. The lower stratospheric vortex broke up in late January. Comparison with 2 previous years, 1984-1985 and 1986-1987, with prolonged midwinter warming periods shows unique characteristics of the 2003-2004 warming period: The length of the vortex disruption, the strong and rapid recovery in the upper stratosphere, and the slow progression of the warming from upper to lower stratosphere. January 2004 zonal mean winds in the middle and lower stratosphere were over 2 standard deviations below average. Examination of past variability shows that the recent frequency of major stratospheric warmings (7 in the past 6 years) is unprecedented. Lower stratospheric temperatures were unusually high during 6 of the past 7 years, with 5 having much lower than usual potential for polar stratospheric cloud (PSC) formation and ozone loss (nearly none in 1998-1999, 2001-2002, and 2003-2004, and very little in 1997-1998 and 2000-2001). Middle and upper stratospheric temperatures, however, were unusually low during and after February. The pattern of 5 of the last 7 years with very low PSC potential would be expected to occur randomly once every 850 years. This cluster of warm winters, immediately following a period of unusually cold winters, may have important implications for possible changes in interannual variability and for determination and attribution of trends in stratospheric temperatures and ozone.

ozone↗
NASA NTRS2016

Stratospheric Aerosol--Observations, Processes, and Impact on Climate

Interest in stratospheric aerosol and its role in climate have increased over the last decade due to the observed increase in stratospheric aerosol since 2000 and the potential for changes in the sulfur cycle induced by climate change. This review provides an overview about the advances in stratospheric aerosol research since the last comprehensive assessment of stratospheric aerosol was published in 2006. A crucial development since 2006 is the substantial improvement in the agreement between in situ and space-based inferences of stratospheric aerosol properties during volcanically quiescent periods. Furthermore, new measurement systems and techniques, both in situ and space based, have been developed for measuring physical aerosol properties with greater accuracy and for characterizing aerosol composition. However, these changes induce challenges to constructing a long-term stratospheric aerosol climatology. Currently, changes in stratospheric aerosol levels less than 20% cannot be confidently quantified. The volcanic signals tend to mask any nonvolcanically driven change, making them difficult to understand. While the role of carbonyl sulfide as a substantial and relatively constant source of stratospheric sulfur has been confirmed by new observations and model simulations, large uncertainties remain with respect to the contribution from anthropogenic sulfur dioxide emissions. New evidence has been provided that stratospheric aerosol can also contain small amounts of nonsulfatematter such as black carbon and organics. Chemistry-climate models have substantially increased in quantity and sophistication. In many models the implementation of stratospheric aerosol processes is coupled to radiation and/or stratospheric chemistry modules to account for relevant feedback processes.

Kresmer, Stefanie↗
NASA NTRS2012

The Origin and Evolution of Saturn's 2011-2012 Stratospheric Vortex

The planet-encircling springtime storm in Saturn's troposphere (December 2010-July 2011, Fletcher, L.N. et al. [2011]. Science 332, 1413-1414; Sánchez-Lavega, A. et al. [2011]. Nature 475, 71-74; Fischer, G. et al. [2011]. Nature 475, 75-77) produced dramatic perturbations to stratospheric temperatures, winds and composition at mbar pressures that persisted long after the tropospheric disturbance had abated. Thermal infrared (IR) spectroscopy from the Cassini Composite Infrared Spectrometer (CIRS), supported by ground-based IR imaging from the VISIR instrument on the Very Large Telescope and the MIRSI instrument on NASA's IRTF, is used to track the evolution of a large, hot stratospheric anticyclone between January 2011 and March 2012. The evolutionary sequence can be divided into three phases: (I) the formation and intensification of two distinct warm airmasses near 0.5 mbar between 25 and 35degN (B1 and B2) between January-April 2011, moving westward with different zonal velocities, B1 residing directly above the convective tropospheric storm head; (II) the merging of the warm airmasses to form the large single 'stratospheric beacon' near 40degN (B0) between April and June 2011, disassociated from the storm head and at a higher pressure (2 mbar) than the original beacons, a downward shift of 1.4 scale heights (approximately 85 km) post-merger; and (III) the mature phase characterised by slow cooling (0.11 +/- 0.01 K/day) and longitudinal shrinkage of the anticyclone since July 2011. Peak temperatures of 221.6 +/- 1.4 K at 2 mbar were measured on May 5th 2011 immediately after the merger, some 80 K warmer than the quiescent surroundings. From July 2011 to the time of writing, B0 remained as a long-lived stable stratospheric phenomenon at 2 mbar, moving west with a near-constant velocity of 2.70 +/- 0.04 deg/day (24.5 +/- 0.4 m/s at 40degN relative to System III longitudes). No perturbations to visible clouds and hazes were detected during this period. With no direct tracers of motion in the stratosphere, we use thermal windshear calculations to estimate clockwise peripheral velocities of 200-400 m/s at 2 mbar around B0. The peripheral velocities of the two original airmasses were smaller (70-140 m/s). In August 2011, the size of the vortex as defined by the peripheral collar was 65deg longitude (50,000 km in diameter) and 25deg latitude. Stratospheric acetylene (C2H2) was uniformly enhanced by a factor of three within the vortex, whereas ethane (C2H6) remained unaffected. The passage of B0 generated a new band of warm stratospheric emission at 0.5 mbar at its northern edge, and there are hints of warm stratospheric structures associated with the beacons at higher altitudes (p < 0.1 mbar) than can be reliably observed by CIRS nadir spectroscopy. Analysis of the zonal windshear suggests that Rossby wave perturbations from the convective storm could have propagated vertically into the stratosphere at this point in Saturn's seasonal cycle, one possible source of energy for the formation of these stratospheric anticyclones.

evolution↗
NASA NTRS2022

NASA GEOS Composition Forecast Modeling System GEOS-CF v1.0: Stratospheric Composition

The NASA Goddard Earth Observing System (GEOS) Composition Forecast (GEOS-29CF) provides recent estimates and five-day forecasts of atmospheric composition to the public in near-real time. To do this, the GEOS Earth system model is coupled with the GEOS-Chem tropospheric-stratospheric unified chemistry extension (UCX) to represent composition from the surface to the top of the GEOS atmosphere (0.01 hPa). The GEOS-CF system is described, including updates made to the GEOS-Chem UCX mechanism within GEOS-CF for improved representation of stratospheric chemistry. Comparisons are made against balloon, lidar and satellite observations for stratospheric composition, including measurements of ozone (O3) and important nitrogen and chlorine species related to stratospheric O3recovery. The GEOS-CF nudges the stratospheric O3towards the GEOS Forward Processing (GEOS FP) assimilated O3product; as a result the stratospheric O3in the GEOS-CF historical estimate agrees well with observations. During abnormal dynamical and chemical environments such as the 2020 polar vortexes, the GEOS-CF O3forecasts are more realistic than GEOS FP O3forecasts because of the inclusion of the complex GEOS-Chem UCX stratospheric chemistry. Overall, the spatial patterns of the GEOS-CF simulated concentrations of stratospheric composition agree well with satellite observations. However, there are notable biases – such as low NOx and HNO3 in the polar regions and generally low HCl throughout the stratosphere – and future improvements to the chemistry mechanism and emissions are discussed. GEOS-CF is a new tool for the research community and instrument teams observing trace gases in the stratosphere and troposphere, providing near-real-time three-dimensional gridded information on atmospheric composition.

GEOS-CF↗
NASA NTRS1995

The fate of atmospheric phosgene and the stratospheric chlorine loadings of its parent compounds: CCl4, C2Cl4, C2HCL3, CH3CCl3, and CHCl3

A study of the tropospheric and stratospheric cycles of phosgene is carried out to determine its fate and ultimate role in controlling the ozone depletion potentials of its parent compounds. Tropospheric phosgene is produced from the OH-initiated oxidation of C2Cl4, CH3CCl3, CHCl3, and C2HCl3. Simulations using a two-dimensional model indicate that these processes produce about 90 pptv/yr of tropospheric phosgene with an average concentration of about 18 pptv, in reasonable agreement with observations. We estimate a residence time of about 70 days for tropospheric phosgene, with the vast majority being removed by hydrolysis in cloudwater. Only about 0.4% of the phosgene produced in the troposphere avoids wet removal and is transported to the stratosphere, where its chlorine can be released to participate in the catalytic destruction of ozone. Stratospheric phosgene is produced from the photochemical degradation of CCl4, C2Cl4, CHCl3, and CH3CCl3 and is removed by photolysis and downward transport to the troposphere. Model calculations, in good agreement with observations, indicate that these processes produce a peak stratospheric concentration of about 25-30 pptv at an altitude of about 25 km. In contrast to tropospheric phosgene, stratospheric phosgene is found to have a lifetime against photochemical removal of the order of years. As a result, a significant portion of the phosgene that is produced in the stratosphere is ultimately returned to the troposphere, where it is rapidly removed by clouds. This phenomenon effectively decreases the amount of reactive chlorine injected into the stratosphere and available for ozone depletion from phosgene's parent compounds. A similar phenomenon due to the downward transport of stratospheric COFCl produced from CFC-11 is estimated to cause a 7% decrease in the amount of reactive chlorine injected into the stratosphere from this compound. Our results are potentially sensitive to a variety of parameters, most notably the rate of reaction of phosgene with sulfate aerosols. However, on the basis of the observed vertical distribution of COCl2, we estimate that the reaction of COCl2 with sulfate aerosol most likely has a gamma less than 5 x 10(exp -5) and, as a result, has a negligible impact on the stratospheric chlorine loadings of the phosgene parent compounds.

Kindler, T. P.↗