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Stolarski, R. S.

Publications and source records attributed to Stolarski, R. S..

At least 37 records · Page 2

Variations in Stratospheric Inorganic Chlorine Between 1991 and 2006

So how quickly will the ozone hole recover? This depends on how quickly the chlorine content (Cl2) of the atmosphere will decline. The ozone hole forms over the Antarctic each southern spring (September and October). The extremely small ozone amounts in the ozone hole are there because of chemical reactions of ozone with chlorine. This chlorine originates largely from industrially produced chlorofluorocarbon (CFC) compounds. An international agreement, the Montreal Protocol, is drastically reducing the amount of chlorine-containing compounds that we are releasing into the atmosphere. To be able to attribute changes in stratospheric ozone to changes in chlorine we need to know the distribution of atmospheric chlorine. However, due to a lack of continuous observations of all the key chlorine gases, producing a continuous time series of stratospheric chlorine has not been achieved to date. We have for the first time devised a technique to make a 17-year time series for stratospheric chlorine that uses the long time series of HCl observations made from several space borne instruments and a neural network. The neural networks allow us to both inter-calibrate the various HCl instruments and to infer the total amount of atmospheric chlorine from HCl. These new estimates of Cl, provide a much needed critical test for current global models that currently predict significant differences in both Cl(sub y) and ozone recovery. These models exhibit differences in their projection of the recovery time and our chlorine content time series will help separate the good from the bad in these projections.

Lary, D. J.↗

The Relationship of Loss, Mean Age of Air and the Distribution of CFCs to Stratospheric Circulation and Implications for Atmospheric Lifetimes

Man-made molecules called chlorofluorcarbons (CFCs) are broken apart in the stratosphere by high energy light, and the reactive chlorine gases that come from them cause the ozone hole. Since the ozone layer stops high energy light from reaching low altitudes, CFCs must be transported to high altitudes to be broken apart. The number of molecules per volume (the density) is much smaller at high altitudes than near the surface, and CFC molecules have a very small chance of reaching that altitude in any particular year. Many tons of CFCs were put into the atmosphere during the end of the last century, and it will take many years for all of them to be destroyed. Each CFC has an atmospheric lifetime that depends on the amount of energy required to break them apart. Two of the gases that were made the most are CFC13 and CF2C12. It takes more energy to break apart CF2C12 than CFC13, and its lifetime is about 100 years, nearly twice as long as the lifetime for CFC13. It is hard to figure out the lifetimes from surface measurements because we don't know exactly how much was released into the air each year. Atmospheric models are used to predict what will happen to ozone and other gases as the CFCs decrease and other gases like C02 continue to increase during the next century. CFC lifetimes are used to predict future concentrations and all assessment models use the predicted future concentrations. The models have different circulations and the amount of CFC lost according to the model may not match the loss that is expected according to the lifetime. In models the amount destroyed per year depends on how fast the model pushes air into the stratosphere and how much goes to high altitudes each year. This paper looks at the way the model circulation changes the lifetimes, and looks at measurements that tell us which model is more realistic. Some models do a good job reproducing the age-of-air, which tells us that these models are circulating the stratospheric air at the right speed. These same models also do a good job reproducing the amount of CFCs in the lower atmosphere where they were measured by instruments on NASA's ER-2, a research plane that flies in the lower stratosphere. The lifetime for CFC13 that is calculated using the models that do the best job matching the data is about 25% longer than most people thought. This paper shows that using these measurements to decide which models are more realistic helps us understand why their predictions are different from each other and also to decide which predictions are more likely.

Douglass, A. R.↗

Long-term Evolution of Upper Stratospheric Ozone at Selected Stations of the Network for the Detection of Stratospheric Change (NDSC)

The long-term evolution of upper stratospheric ozone has been recorded by lidars and microwave radiometers within the ground-based Network for the Detection of Stratospheric Change (NDSC), and by the space-borne Solar Backscatter Ultra-Violet instruments (SBUV), Stratospheric Aerosol and Gas Experiment (SAGE), and Halogen Occultation Experiment (HALOE). Climatological mean differences between these instruments are typically smaller than 5% between 25 and 50 km. Ozone anomaly time series from all instruments, averaged from 35 to 45 km altitude, track each other very well and typically agree within 3 to 5%. SBUV seems to have a slight positive drift against the other instruments. The corresponding 1979 to 1999 period from a transient simulation by the fully coupled MAECHAM4-CHEM chemistry climate model reproduces many features of the observed anomalies. However, in the upper stratosphere the model shows too low ozone values and too negative ozone trends, probably due to an underestimation of methane and a consequent overestimation of ClO. The combination of all observational data sets provides a very consistent picture, with a long-term stability of 2% or better. Upper stratospheric ozone shows three main features: (1) a decline by 10 to 15% since 1980, due to chemical destruction by chlorine; (2) two to three year fluctuations by 5 to 10%, due to the Quasi-Biennial Oscillation (QBO); (3) an 11-year oscillation by about 5%, due to the 11-year solar cycle. The 1979 to 1997 ozone trends are larger at the southern mid-latitude station Lauder (45 S), reaching 8%/decade, compared to only about 6%/decade at Table Mountain (35 N), Haute Provence/Bordeaux (approximately equal to 45 N), and Hohenpeissenberg/Bern(approximately equal to 47 N). At Lauder, Hawaii (20 N), Table Mountain, and Haute Provence, ozone residuals after subtraction of QBO- and solar cycle effects have levelled off in recent years, or are even increasing. Assuming a turning point in January 1997, the change of trend is largest at southern mid-latitude Lauder, +11%/decade, compared to +7%/decade at northern mid-latitudes. This points to a beginning recovery of upper stratospheric ozone. However, chlorine levels are still very high and ozone will remain vulnerable. At this point the most northerly mid-latitude station, Hohenpeissenberg/Bern differs from the other stations, and shows much less clear evidence for a beginning recovery, with a change of trend in 1997 by only +3%/decade. In fact, record low upper stratospheric ozone values were observed at Hohenpeissenberg/Bern, and to a lesser degree at Table Mountain and Haute Provence, in the winters 2003/2004 and 2004/2005.

Steinbrecht, W.↗

On detecting a trend in the residual circulation from observations of column HCl

The troposphere is the part of the atmosphere where people live. The troposphere goes up to about 12 km above the earth over places at middle latitudes like Washington, D.C. The next layer of air up in the atmosphere is called the stratosphere. The tropopause separates the troposphere and stratosphere. Most of the ozone in the atmosphere is in the stratosphere where it protects people from the harmful rays in sunlight. Near the earth s surface, ozone is a pollutant. In general, air travels from the troposphere to the stratosphere through upward motion in the tropics. Most of the air comes back down to the troposphere at middle latitudes. The so-called "stratospheric residual circulation" moves the air in the stratosphere from the tropics to the middle latitudes. In this way, the amount of air that moves out of the stratosphere into the troposphere at middle latitudes depends on the strength of the residual circulation. This overturning of the atmosphere is important as it brings chemicals produced by the activities of people into the stratosphere. Most notable are chlorofluorocarbons (CFCs) that destroy stratospheric ozone. The transport of air out of the stratosphere removes ozone-destroying chemicals, but also brings ozone into the troposphere.

Olsen, M. A.↗

The Sensitivity of Arctic Ozone Loss to Polar Stratospheric Cloud Volume and Chlorine and Bromine Loading in a Chemistry and Transport Model

The sensitivity of Arctic ozone loss to polar stratospheric cloud volume (V(sub PSC)) and chlorine and bromine loading is explored using chemistry and transport models (CTMs). A simulation using multi-decadal output from a general circulation model (GCM) in the Goddard Space Flight Center (GSFC) CTM complements one recycling a single year s GCM output in the Global Modeling Initiative (GMI) CTM. Winter polar ozone loss in the GSFC CTM depends on equivalent effective stratospheric chlorine (EESC) and polar vortex characteristics (temperatures, descent, isolation, polar stratospheric cloud amount). Polar ozone loss in the GMI CTM depends only on changes in EESC as the dynamics repeat annually. The GSFC CTM simulation reproduces a linear relationship between ozone loss and Vpsc derived from observations for 1992 - 2003 which holds for EESC within approx.85% of its maximum (approx.1990 - 2020). The GMI simulation shows that ozone loss varies linearly with EESC for constant, high V(sub PSC).

Douglass, A. R.↗

Interannual Variability of Ozone in the Polar Vortex during the Fall Season

Previous analysis has shown that the distribution of O3 at high northern latitudes in the lower-to-middle stratosphere at the beginning of the winter season has a characteristic distribution, which is consistent between in situ and satellite measurements. Initial O3 profiles in the vortex are similar to each other and are quite different from outside the vortex at the same latitude and also from a zonal mean climatology. In the vortex, O3 is nearly constant from 500 to above 800 K with a value near 3 ppmv. Values outside the vortex are up to a factor of 2 higher and increase significantly with potential temperature. Model analysis indicates that the characteristic vortex O3 profiles arise from a combination of seasonally accelerated photochemical loss at high latitudes and minimal transport of air from lower latitudes. Analysis of the relatively high-resolution POAM data shows that these characteristic O3 distributions are consistent from year to year and between the hemispheres. Here we emphasize analysis of the 24-year time series of O3 data from SBUV in the lower-to-middle stratosphere at high latitudes in the fall vortex. We find that the variability of O3 from SBUV is relatively small in this regime and no significant trend is detectable. The implications of the findings for stratospheric O3 chemistry and transport will be explored.

Bhartia, P. K.↗

A Monte Carlo Uncertainty Analysis of Ozone Trend Predictions in a Two Dimensional Model

We use Monte Carlo analysis to estimate the uncertainty in predictions of total O3 trends between 1979 and 1995 made by the Goddard Space Flight Center (GSFC) two-dimensional (2D) model of stratospheric photochemistry and dynamics. The uncertainty is caused by gas-phase chemical reaction rates, photolysis coefficients, and heterogeneous reaction parameters which are model inputs. The uncertainty represents a lower bound to the total model uncertainty assuming the input parameter uncertainties are characterized correctly. Each of the Monte Carlo runs was initialized in 1970 and integrated for 26 model years through the end of 1995. This was repeated 419 times using input parameter sets generated by Latin Hypercube Sampling. The standard deviation (a) of the Monte Carlo ensemble of total 03 trend predictions is used to quantify the model uncertainty. The 34% difference between the model trend in globally and annually averaged total O3 using nominal inputs and atmospheric trends calculated from Nimbus 7 and Meteor 3 total ozone mapping spectrometer (TOMS) version 7 data is less than the 46% calculated 1 (sigma), model uncertainty, so there is no significant difference between the modeled and observed trends. In the northern hemisphere midlatitude spring the modeled and observed total 03 trends differ by more than 1(sigma) but less than 2(sigma), which we refer to as marginal significance. We perform a multiple linear regression analysis of the runs which suggests that only a few of the model reactions contribute significantly to the variance in the model predictions. The lack of significance in these comparisons suggests that they are of questionable use as guides for continuing model development. Large model/measurement differences which are many multiples of the input parameter uncertainty are seen in the meridional gradients of the trend and the peak-to-peak variations in the trends over an annual cycle. These discrepancies unambiguously indicate model formulation problems and provide a measure of model performance which can be used in attempts to improve such models.

Considine, D. B.↗

Simulation of Long Lived Tracers Using an Improved Empirically Based Two-Dimensional Model Transport Algorithm

We have developed a new empirically-based transport algorithm for use in our GSFC two-dimensional transport and chemistry model. The new algorithm contains planetary wave statistics, and parameterizations to account for the effects due to gravity waves and equatorial Kelvin waves. As such, this scheme utilizes significantly more information compared to our previous algorithm which was based only on zonal mean temperatures and heating rates. The new model transport captures much of the qualitative structure and seasonal variability observed in long lived tracers, such as: isolation of the tropics and the southern hemisphere winter polar vortex; the well mixed surf-zone region of the winter sub-tropics and mid-latitudes; the latitudinal and seasonal variations of total ozone; and the seasonal variations of mesospheric H2O. The model also indicates a double peaked structure in methane associated with the semiannual oscillation in the tropical upper stratosphere. This feature is similar in phase but is significantly weaker in amplitude compared to the observations. The model simulations of carbon-14 and strontium-90 are in good agreement with observations, both in simulating the peak in mixing ratio at 20-25 km, and the decrease with altitude in mixing ratio above 25 km. We also find mostly good agreement between modeled and observed age of air determined from SF6 outside of the northern hemisphere polar vortex. However, observations inside the vortex reveal significantly older air compared to the model. This is consistent with the model deficiencies in simulating CH4 in the northern hemisphere winter high latitudes and illustrates the limitations of the current climatological zonal mean model formulation. The propagation of seasonal signals in water vapor and CO2 in the lower stratosphere showed general agreement in phase, and the model qualitatively captured the observed amplitude decrease in CO2 from the tropics to midlatitudes. However, the simulated seasonal amplitudes were attenuated too rapidly with altitude in the tropics. Overall, the simulations with the new transport formulation are in substantially better agreement with observations compared with our previous model transport.

Fleming, E. L.↗

The global distribution of ozone destruction rates obtained from 13 years of Nimbus/TOMS data (1979-1991)

Long-term ozone trends (percentage change) have been computed from 13 years of Nimbus/TOMS (Total Ozone Mapping Spectrometer) data as a function of latitude, longitude, and month for the period January 1, 1979 to December 31, 1991. In both hemispheres, the ozone column content has decreased at latitudes above 30 deg by amounts that are larger than predicted by homogeneous chemistry models for the 13-year time period. The largest rates of ozone decrease occur in the Southern Hemisphere during winter and spring, with recovery during the summer and autumn. The large winter ozone loss rates are consistent with observed low stratospheric temperatures, ice-cloud formation, and heterogeneous chemistry at middle and high latitudes. There are similar, but smaller changes observed in the Northern Hemisphere. At midlatitudes, (40 deg N to 50 deg N) there are increased zonal average ozone depletion rates that correspond to 5 geographically localized regions of increased ozone depletion rates. Only the equatorial band between plus or minus 20 deg shows little or no long-term ozone change since January, 1979. The long-term winter ozone depletion rate data for both hemispheres suggests that heterogeneous chemistry processes may operate over a wide range of latitudes during half of the year.

Herman, Jay R.↗

MLS CLO observations and arctic polar vortex temperatures

Analysis of Upper Altmosphere Research Satellite (UARS) Microwave Limb Sounder (MLS) observations in early January 1992 shows a clear relationship between predicted polar stratospheric cloud formation along the back trajectory and elevated ClO amounts. These findings are in good agreement with aircraft observations. The MLS observed variation of ClO amounts within the vortex also fits the pattern of ClO change as a result of air parcel solar exposure and nitric acid photolysis. Outside the polar vortex, the occasional highly elevated ClO appear statistically consistent with MLS measurement noise.

Schoeberl, M. R.↗

Interpretation of NO(x)/NO(y) observations from AASE-2 using a model of chemistry along trajectories

In situ measurements of NO and NO(y) are used to derive the ratio NO(x)/NO(y) along the flight track of the NASA ER-2 aircraft. Data are presented for two flights at midlatitudes in October 1991 during the Airborne Arctic Stratospheric Expedition-2 (AASE-2). Aerosol particle surface area was concurrently measured. The observations are compared with a photochemical model integrated along back trajectories from the aircraft flight track. Comparison of observations with the model run along trajectories and at a fixed position clearly and quantitatively demonstrates the importance of an air parcel's dynamic history in interpretation of local chemical observations. Comparison of the data with model runs under different assumptions regarding heterogeneous chemistry further reinforces the case for occurrence of the reaction of N2O5 + H2O on sulfate aerosol surfaces in the atmosphere. Finally, comparisons for which relative changes in the model and the data are not consistent caution that our ability to resolve all the observations is not yet complete.

Kawa, S. R.↗

The evolution of ClO and NO along air parcel trajectories

Back trajectory analysis of Arctic and Antarctic aircraft data reveals that high ClO concentrations are associated with predicted polar stratospheric cloud (PSCs) encounters. The ClO concentrations within the Arctic and Antarctic polar vortices vary widely but appear to be inversely related to parcel solar exposure since the last PSC interaction. These results imply that production of NO(x) from HNO3 photolysis and reaction with OH is the mechanism for the loss of chlorine radicals through the reformation of chlorine nitrate. Highly denitrified air parcels show no change in ClO with solar exposure. The recovery process is quantitatively duplicated using a model of chemistry along trajectories. Although PSC processing is the primary mechanism for producing elevated ClO amounts, back trajectories apparently unperturbed by PSC's also show slightly elevated ClO levels in 1992 compared to Arctic 1989 and Antarctic 1987 measurements presumably due to the presence of Pinatubo aerosol.

Schoeberl, M. R.↗

Record low global ozone in 1992

The 1992 global average total ozone, measured by the Total Ozone Mapping Spectrometer (TOMS) on the Nimbus-7 satellite, was 2 to 3 percent lower than any earlier year observed by TOMS (1979 to 1991). Ozone amounts were low in a wide range of latitudes in both the Northern and Southern Hemispheres, and the largest decreases were in the regions from 10 to 20 deg S and 10 to 60 deg N. Global ozone in 1992 is at least 1.5 percent lower than would be predicted by a statistical model that includes a linear trend and accounts for solar cycle variation and the quasi-biennial oscillation. These results are confirmed by comparisons with data from other ozone monitoring instruments: the SBUV/2 instrument on the NOAA-11 satellite, the TOMS instrument on the Russian Meteor-3 satellite, the World Standard Dobson Instrument 83, and a collection of 22 ground-based Dobson instruments.

Gleason, J. F.↗

Natural Cycles, Gases

The major gaseous components of the exhaust of stratospheric aircraft are expected to be the products of combustion (CO2 and H2O), odd nitrogen (NO, NO2 HNO3), and products indicating combustion inefficiencies (CO and total unburned hydrocarbons). The species distributions are produced by a balance of photochemical and transport processes. A necessary element in evaluating the impact of aircraft exhaust on the lower stratospheric composition is to place the aircraft emissions in perspective within the natural cycles of stratospheric species. Following are a description of mass transport in the lower stratosphere and a discussion of the natural behavior of the major gaseous components of the stratospheric aircraft exhaust.

Douglass, Anne R.↗

Recent trends in stratospheric total ozone - Implications of dynamical and El Chichon perturbations

The recently reprocessed Nimbus-7 TOMS total ozone data from 1979 to 1989 are analyzed to assess the global impact of the El Chichon volcanic eruption on stratospheric total ozone. An apparent decrease in total ozone of 5 to 6 percent is present during the winter of 1982-1983 following the eruption of El Chichon. A regression analysis of total ozone with the equatorial zonal wind at 30 mb indicates that response to the quasi-biennial oscillation can explain much of the observed ozone anomaly, and that the total ozone decrease which can be attributed to El Chichon is at most 2 to 4 percent. This study also suggests that the interannual variability caused by the quasi-biennial oscillation and planetary wave activity may introduce apparent seasonal trends in total ozone and temperature in the lower stratosphere, particularly if the length of the data record is not very long. Such trends may affect the assessment of total ozone changes caused by chemical perturbations.

Chandra, S.↗

Antarctic ozone hole - Possible implications for ozone trends in the Southern Hemisphere

Satellite-borne instruments (the Total Ozone Mapping Spectrometer and the Solar Backscattered Ultraviolet Instrument) show that, compared to 1979, total column ozone has a year-round decrease of more than 5 percent in the neighborhood of 60 deg S. The meteorological conditions (warmer temperatures, the absence of polar stratospheric clouds) at these latitudes do not seem to favor heterogeneous chemistry as the direct cause for the observed year-round ozone reduction. A mechanism involving the seasonal transport of ozone-poor air from within the polar vortex to lower latitudes (the so-called 'dilution effect') is proposed as a possible explanation for the observed year-round ozone reduction in subpolar regions. A two-dimensional model with an imposed springtime Antarctic ozone depletion is used to study the post-ozone hole impact on the spatial and temporal distributions of column ozone at latitudes north of 60 deg S. It is found that the time constant associated with the dilution effect in the latitude region 40-60 deg S is about 1 year, long enough to contribute to the observed year-round decrease of total ozone in that region.

Sze, N. D.↗

Trends in total column ozone measurements

It is important to ensure the best available data are used in any determination of possible trends in total ozone in order to have the most accurate estimates of any trends and the associated uncertainties. Accordingly, the existing total ozone records were examined in considerable detail. Once the best data set has been produced, the statistical analysis must examine the data for any effects that might indicate changes in the behavior of global total ozone. The changes at any individual measuring station could be local in nature, and herein, particular attention was paid to the seasonal and latitudinal variations of total ozone, because two dimensional photochemical models indicate that any changes in total ozone would be most pronounced at high latitudes during the winter months. The conclusions derived from this detailed examination of available total ozone can be split into two categories, one concerning the quality and the other the statistical analysis of the total ozone record.

Rowland, F. S.↗

Theory and observations: Model simulations of the period 1955-1985

The main objective of the theoretical studies presented here is to apply models of stratospheric chemistry and transport in order to understand the processes that control stratospheric ozone and that are responsible for the observed variations. The model calculations are intended to simulate the observed behavior of atmospheric ozone over the past three decades (1955-1985), for which there exists a substantial record of both ground-based and, more recently, satellite measurements. Ozone concentrations in the atmosphere vary on different time scales and for several different causes. The models described here were designed to simulate the effect on ozone of changes in the concentration of such trace gases as CFC, CH4, N2O, and CO2. Changes from year to year in ultraviolet radiation associated with the solar cycle are also included in the models. A third source of variability explicitly considered is the sporadic introduction of large amounts of NO sub x into the stratosphere during atmospheric nuclear tests.

Isaksen, Ivar S. A.↗