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Fleming, E. L.

Publications and source records attributed to Fleming, E. L..

At least 19 records

Multimodel Estimates of Atmospheric Lifetimes of Long-lived Ozone-Depleting Substances: Present and Future

We have diagnosed the lifetimes of long-lived source gases emitted at the surface and removed in the stratosphere using six three-dimensional chemistry-climate models and a two-dimensional model. The models all used the same standard photochemical data. We investigate the effect of different definitions of lifetimes, including running the models with both mixing ratio (MBC) and flux (FBC) boundary conditions. Within the same model, the lifetimes diagnosed by different methods agree very well. Using FBCs versus MBCs leads to a different tracer burden as the implied lifetime contained in the MBC value does not necessarily match a model's own calculated lifetime. In general, there are much larger differences in the lifetimes calculated by different models, the main causes of which are variations in the modeled rates of ascent and horizontal mixing in the tropical midlower stratosphere. The model runs have been used to compute instantaneous and steady state lifetimes. For chlorofluorocarbons (CFCs) their atmospheric distribution was far from steady state in their growth phase through to the 1980s, and the diagnosed instantaneous lifetime is accordingly much longer. Following the cessation of emissions, the resulting decay of CFCs is much closer to steady state. For 2100 conditions the model circulation speeds generally increase, but a thicker ozone layer due to recovery and climate change reduces photolysis rates. These effects compensate so the net impact on modeled lifetimes is small. For future assessments of stratospheric ozone, use of FBCs would allow a consistent balance between rate of CFC removal and model circulation rate

CFC↗

Multimodel Estimates of Atmospheric Lifetimes of Long-Lived Ozone-Depleting Substances: Present and Future

We have diagnosed the lifetimes of long-lived source gases emitted at the surface and removed in the stratosphere using six three-dimensional chemistry-climate models and a two-dimensional model. The models all used the same standard photochemical data. We investigate the effect of different definitions of lifetimes, including running the models with both mixing ratio (MBC) and flux (FBC) boundary conditions. Within the same model, the lifetimes diagnosed by different methods agree very well. Using FBCs versus MBCs leads to a different tracer burden as the implied lifetime contained in theMBC value does not necessarilymatch a model's own calculated lifetime. In general, there are much larger differences in the lifetimes calculated by different models, the main causes of which are variations in the modeled rates of ascent and horizontal mixing in the tropical midlower stratosphere. The model runs have been used to compute instantaneous and steady state lifetimes. For chlorofluorocarbons (CFCs) their atmospheric distribution was far from steady state in their growth phase through to the 1980s, and the diagnosed instantaneous lifetime is accordingly much longer. Following the cessation of emissions, the resulting decay of CFCs is much closer to steady state. For 2100 conditions the model circulation speeds generally increase, but a thicker ozone layer due to recovery and climate change reduces photolysis rates. These effects compensate so the net impact on modeled lifetimes is small. For future assessments of stratospheric ozone, use of FBCs would allow a consistent balance between rate of CFC removal and model circulation rate.

CH3CCl3↗

Middle Atmospheric Changes Caused by the January and March 2012 Solar Proton Events

The recent 23-30 January and 7-11 March 2012 solar proton event (SPE) periods were substantial and caused significant impacts on the middle atmosphere. These were the two largest SPE periods of solar cycle 24 so far. The highly energetic solar protons produced considerable ionization of the neutral atmosphere as well as HOx (H, OH, HO2) and NOx (N, NO, NO2). We compute a NOx production of 1.9 and 2.1 Gigamoles due to these SPE periods in January and March 2012, respectively, which places these SPE periods among the 12 largest in the past 50 years. Aura Microwave Limb Sounder (MLS) observations of the peroxy radical, HO2, show significant enhancements of 0.9 ppbv in the northern polar mesosphere as a result of these SPE periods. Both MLS measurements and Goddard Space Flight Center (GSFC) two-dimensional (2D) model predictions indicated middle mesospheric ozone decreases of 20 percent for several days in the northern polar region with maximum depletions 60 percent as a result of the HOx produced in both the January and March 2012 SPE periods. The SCISAT-1 Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE) and the Envisat Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instruments measured NO and NO2 (NOx), which indicated enhancements of over 20 ppbv in most of the northern polar mesosphere for several days as a result of these SPE periods. The GSFC 2D model was used to predict the medium-term (months) influence and found that the polar Southern Hemisphere middle atmosphere ozone was most affected by these solar events due to the increased downward motion in the fall and early winter. The downward transport moved the SPE-produced NOy to lower altitudes and led to predicted modest destruction of ozone (5-9 percent) in the upper stratosphere days to weeks after the March 2012 event. Total ozone reductions were predicted to be a maximum of 1 percent in 2012 due to these SPEs.

ozone↗

Middle Atmosphere Response to Different Descriptions of the 11-Year Solar Cycle in Spectral Irradiance in a Chemistry-Climate Model

The 11-year solar cycle in solar spectral irradiance (SSI) inferred from measurements by the SOlar Radiation & Climate Experiment (SORCE) suggests a much larger variation in the ultraviolet than previously accepted. We present middle atmosphere ozone and temperature responses to the solar cycles in SORCE SSI and the ubiquitous Naval Research Laboratory (NRL) SSI reconstruction using the Goddard Earth Observing System chemistry-climate model (GEOS CCM). The results are largely consistent with other recent modeling studies. The modeled ozone response is positive throughout the stratosphere and lower mesosphere using the NRL SSI, while the SORCE SSI produces a response that is larger in the lower stratosphere but out of phase with respect to total solar irradiance above 45 km. The modeled responses in total ozone are similar to those derived from satellite and ground-based measurements, 3-6 Dobson Units per 100 units of 10.7-cm radio flux (F10.7) in the tropics. The peak zonal mean tropical temperature response 50 using the SORCE SSI is nearly 2 K per 100 units 3 times larger than the simulation using the NRL SSI. The GEOS CCM and the Goddard Space Flight Center (GSFC) 2-D coupled model are used to examine how the SSI solar cycle affects the atmosphere through direct solar heating and photolysis processes individually. Middle atmosphere ozone is affected almost entirely through photolysis, whereas the solar cycle in temperature is caused both through direct heating and photolysis feedbacks, processes that are mostly linearly separable. Further, the net ozone response results from the balance of ozone production at wavelengths less than 242 nm and destruction at longer wavelengths, coincidentally corresponding to the wavelength regimes of the SOLar STellar Irradiance Comparison Experiment (SOLSTICE) and Spectral Irradiance Monitor (SIM) on SORCE, respectively. A higher wavelength-resolution analysis of the spectral response could allow for a better prediction of the atmospheric response to arbitrary SSI variations.

Swartz, W. H.↗

A Model Study of the Impact of Source Gas Changes on the Stratosphere for 1850-2100

The long term stratospheric impacts due to emissions of CO2, CH4, N2O, and ozone depleting substances (ODSs) are investigated using an updated version of the Goddard two-dimensional (2D) model. Perturbation simulations with the ODSs, CO2, CH4, and N2O varied individually are performed to isolate the relative roles of these gases in driving stratospheric changes over the 1850-2100 time period. We also show comparisons with observations and the God- 40 dard Earth Observing System chemistry-climate model simulations for the time period 1970-2100 to illustrate that the 2D model captures the basic processes responsible for longterm stratospheric change. The 2D simulations indicate that prior to 1940, the 45 ozone increases due to CO2 and CH4 loading outpace the ozone losses due to increasing N2O and carbon tetrachloride (CCl4) emissions, so that ozone reaches a broad maximum during the 1920s-1930s. This preceeds the significant ozone depletion during approx. 1960-2050 driven by the ODS loading. During the latter half of the 21st century as ODS emissions diminish, CO2, N2O, and CH4 loading will all have significant impacts on global total ozone based on the IPCC AIB (medium) scenario, with CO2 having the largest individual effect. Sensitivity tests illustrate that due to the strong chemical interaction between methane and chlorine, the CH4 impact on total ozone becomes significantly more positive with larger ODS loading. The model simulations also show that changes in stratospheric temperature, Brewer-Dobson circulation (BDC), and age of air during 1850-2100 are controlled mainly by the CO2 and ODS loading. The simulated acceleration of the BDC causes the age of air to decrease by approx. 1 year from 1860-2100. The corresponding photochemical lifetimes of N2O, CFCl3, CF2Cl2, and CCl4 decrease by 11-13% during 1960-2100 due to the acceleration of the BDC, with much smaller lifetime changes 4%) caused by changes in the photochemical loss rates.

Fleming, E. L.↗

Northern Hemisphere Atmospheric Influence of the Solar Proton Events and Ground Level Enhancement in January 2005

Solar eruptions in early 2005 led substantial barrage of charged particles on the Earth's atmosphere during the January 16-21 period. Proton fluxes were greatly increased during these several days and led to the production ofHO(x)(H, OH, BO2)and NO(x)(N, NO, NO2), which then caused the destruction of ozone. We focus on the Northern polar region, where satellite measurements and simulations with the Whole Atmosphere Community Climate Model (WACCM3) showed large enhancements in mesospheric HO(x) and NO(x) constituents, and associated ozone reductions, due 10 these solar proton events (SPEs). The WACCM3 simulations show enhanced short-lived OH throughout the mesosphere in the 60-82.5degN latitude band due to the SPEs for most days in the Jan.16-2l,2005 period, in reasonable agreement with the Aura Microwave Limb Sounder (MLS) measurements. Mesospheric HO2 is also predicted to be increased by the SPEs, however, the modeled HO2 results are somewhat larger than the MLS measurements. These HO(x) enhancements led to huge predicted and MLS-measured ozone decreases of greater than 40% throughout most of the Northern polar mesosphere during the SPE period. Envisat Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) measurements of hydrogen peroxide (H2O2) show increases throughout the stratosphere with highest enhancements of about 60 ppt y in the lowermost mesosphere over the Jan. 16-18, 2005 period due to the solar protons. WACCM3 predictions indicate H2O2 enhancements over the same time period of more than twice that amount. Measurements of nitric acid (HNO3) by both MLS and MIPAS show an increase of about 1 ppbv above background levels in the upper stratosphere during January 16-29, 2005. WACCM3 simulations show only minuscule HNO3 changes in the upper stratosphere during this time period. However due to the small loss rates during winter, polar mesospheric enhancements of NO(x) are computed to be greater than 50 ppbv during the SPE period. Computed NO(x)increases, which were statistically significant at the 95% level, lasted about a month past the SPEs. The SCISAT-I Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) NO(x) measurements and MIPAS NO, measurements for the polar Northern Hemisphere are in reasonable agreement with these predictions. An extremely large ground level enhancement (GLE) occurred during the SPE period on January 20, 2005. We find that protons of energies 300 to 20,000 MeV, not normally included in our computations, led to enhanced lower stratospheric odd nitrogen concentrations of less than 0.1% as a result of this GLE.

Jackman, C. H.↗

Options to Accelerate Ozone Recovery: Ozone and Climate Benefits

The humankind or anthropogenic influence on ozone primarily originated from the chlorofluorocarbons and halons (chlorine and bromine). Representatives from governments have met periodically over the years to establish international regulations starting with the Montreal Protocol in 1987, which greatly limited the release of these ozone-depleting substances (DDSs). Two global models have been used to investigate the impact of hypothetical reductions in future emissions of ODSs on total column ozone. The investigations primarily focused on chlorine- and bromine-containing gases, but some computations also included nitrous oxide (N2O). The Montreal Protocol with ODS controls have been so successful that further regulations of chlorine- and bromine-containing gases could have only a fraction of the impact that regulations already in force have had. if all anthropogenic ODS emissions were halted beginning in 2011, ozone is calculated to be higher by about 1-2% during the period 2030-2100 compared to a case of no additional ODS restrictions. Chlorine- and bromine-containing gases and nitrous oxide are also greenhouse gases and lead to warming of the troposphere. Elimination of N 20 emissions would result in a reduction of radiative forcing of 0.23 W/sq m in 2100 than presently computed and destruction of the CFC bank would produce a reduction in radiative forcing of 0.005 W/sq m in 2100. This paper provides a quantitative way to consider future regulations of the CFC bank and N 20 emissions

Fleming, E. L.↗

What Would Have Happened to the Ozone Layer if Chlorofluorocarbons (CFCs) had not been Regulated?

Ozone depletion by chlorofluorocarbons (CFCs) was first proposed by Molina and Rowland in their 1974 Nature paper. Since that time, the sci entific connection between ozone losses and CFCs and other ozone depl eting substances (ODSs) has been firmly established with laboratory m easurements, atmospheric observations, and modeling research. This science research led to the implementation of international agreements t hat largely stopped the production of ODSs. In this study we use a fu lly-coupled radiation-chemical-dynamical model to simulate a future world where ODSs were never regulated and ODS production grew at an ann ual rate of 3%. In this "world avoided" simulation 1.7 % of the globa lly-average column ozone is destroyed by 2020, and 67% is destroyed b y 2065 in comparison to 1980. Large ozone depletions in the polar region become year-round rather than just seasonal as is currently observ ed in the Antarctic ozone hole. Very large temperature decreases are observed in response to circulation changes and decreased shortwave radiation absorption by ozone. Ozone levels in the tropical lower strat osphere remain constant until about 2053 and then collapse to near ze ro by 2058 as a result of heterogeneous chemical processes (as curren tly observed in the Antarctic ozone hole). The tropical cooling that triggers the ozone collapse is caused by an increase of the tropical upwelling. In response to ozone changes, ultraviolet radiation increa ses, more than doubling the erythemal radiation in the northern summer midlatitudes by 2060.

Newman, Paul A.↗

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

Model-derived estimates of the annually integrated destruction and lifetime for various ozone depleting substances (ODSs) depend on the simulated stratospheric transport and mixing in the global model used to produce the estimate. Observations in the middle and high latitude lower stratosphere show that the mean age of an air parcel (i.e., the time since its stratospheric entry) is related to the fractional release for the ODs (i.e., the amount of the ODS that has been destroyed relative to the amount at the time of stratospheric entry). We use back trajectory calculations to produce an age spectrum, and explain the relationship between the mean age and the fractional release by showing that older elements in the age spectrum have experienced higher altitudes and greater ODs destruction than younger elements. In our study, models with faster circulations produce distributions for the age-of-air that are 'young' compared to a distribution derived from observations. These models also fail to reproduce the observed relationship between the mean age of air and the fractional release. Models with slower circulations produce both realistic distributions for mean age and a realistic relationship between mean age and fractional release. These models also produce a CFCl3 lifetime of approximately 56 years, longer than the 45 year lifetime used to project future mixing ratios. We find that the use of flux boundary conditions in assessment models would have several advantages, including consistency between ODS evolution and simulated loss even if the simulated residual circulation changes due to climate change.

Douglas, A. R.↗

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.↗

Comparison of Recent Modeled and Observed Trends in Total Column Ozone

We present a comparison of trends in total column ozone from 10 two-dimensional and 4 three-dimensional models and solar backscatter ultraviolet-2 (SBUV/2) satellite observations from the period 1979-2003. Trends for the past (1979-2000), the recent 7 years (1996-2003), and the future (2000-2050) are compared. We have analyzed the data using both simple linear trends and linear trends derived with a hockey stick method including a turnaround point in 1996. If the last 7 years, 1996-2003, are analyzed in isolation, the SBUV/2 observations show no increase in ozone, and most of the models predict continued depletion, although at a lesser rate. In sharp contrast to this, the recent data show positive trends for the Northern and the Southern Hemispheres if the hockey stick method with a turnaround point in 1996 is employed for the models and observations. The analysis shows that the observed positive trends in both hemispheres in the recent 7-year period are much larger than what is predicted by the models. The trends derived with the hockey stick method are very dependent on the values just before the turnaround point. The analysis of the recent data therefore depends greatly on these years being representative of the overall trend. Most models underestimate the past trends at middle and high latitudes. This is particularly pronounced in the Northern Hemisphere. Quantitatively, there is much disagreement among the models concerning future trends. However, the models agree that future trends are expected to be positive and less than half the magnitude of the past downward trends. Examination of the model projections shows that there is virtually no correlation between the past and future trends from the individual models.

Andersen, S. B.↗

Neutral Middle Atmospheric Influences by the Extremely Large October 2003 Solar Proton Event

The huge coronal mass ejection (CME) on October 28,2003 caused an extremely large solar proton event (SPE) at the Earth, which impacted the middle atmospheric polar cap regions. The highly energetic protons produce ionizations, excitations, dissociations, and dissociative ionizations of the background constituents, which lead to the production of HOx (H, OH, HO2) and NOy (N, NO, NO2, NO3, N2O5, HNO3, HO2NO2, ClONO2, BrONO2). The total production of middle atmospheric NOy molecules by individual SPEs can be used to compare their sizes. Using this scale, the extremely large October 2003 SPE was the fourth largest in the past 40 years and the second largest of solar cycle 23. Only the October 1989, August 1972, and July 2000 SPEs were larger. The Goddard Space Flight Center (GSFC) Two-dimensional (2D) Model was used in computing the influence of this gigantic SPE. The NOy amount was increased by over two orders of magnitude in the mesosphere in both the GSFC 2D Model computations and Upper Atmosphere Research Satellite (UARS) Halogen Occultation Experiment (HALOE) measurements as a result of this noteworthy SPE. The model also calculated polar middle mesospheric ozone decreases of over 70% during the SPE. Other atmospheric impacts from both model predictions and measurements as a result of this major SPE will be discussed in this paper.

Jackman, C. H.↗

Neutral Middle Atmospheric Influences by the Extremely Large October 2003 Solar Proton

The huge coronal mass ejection (CME) on October 28, 2003 caused an extremely large solar proton event (SPE) 3t the Earth, which impacted the middle atmospheric polar cap regions. The highly energetic protons produce ionizations, excitations, dissociations, and dissociative ionizations of the background constituents, which lead to the production of HO(x) (H, OH, HO2) and NO(y) (N, NO, NO2, NO3, N2O5, HNO3, HO2NO2, ClONO2, BrONO2). The total production of middle atmospheric NO(y) molecules by individual SPEs can be used to compare their sizes. Using this scale, the extremely large October 2003 SPE was the fourth largest in the past 40 years and the second largest of solar cycle 23. Only the October 1989, August 1972, and July 2000 SPEs were larger. The Goddard Space Flight Center (CSFC) Two-dimensional (2D)) Model was used in computing the influence of this gigantic SPE The NO(y) amount was increased by over two orders of Atmosphere Research Satellite (UARS) Halogen Occultation Experiment (HALOE) measurements as a result of this noteworthy SPE. The model also calculated polar middle mesosphere ozone decreases of over 70% during the SPE. Other atmospheric impacts from both model predictions and measurements as a result of this major SPE will be discussed in this paper.

Jackman, C. H.↗

Aviation Fuel Tracer Simulation: Model Intercomparison and Implications

An upper limit for aircraft-produced perturbations to aerosols and gaseous exhaust products in the upper troposphere and lower stratosphere (UT/LS) is derived using the 1992 aviation fuel tracer simulation performed by eleven global atmospheric models. Key findings are that subsonic aircraft emissions: (1) have not been responsible for the observed water vapor trends at 40degN; (2) could be a significant source of soot mass near 12 km, but not at 20 km; (3) might cause a noticeable increase in the background sulfate aerosol surface area and number densities (but not mass density) near the northern mid-latitude tropopause; and (4) could provide a global, annual mean top of the atmosphere radiative forcing up to +0.006 W/sq m and -0.013 W/sq m due to emitted soot and sulfur, respectively.

Danilin, M. Y.↗

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.↗

Aviation Fuel Tracer Simulation: Model Intercomparison and Implications

An upper limit for aircraft-produced perturbations to aerosols and gaseous exhaust products in the upper troposphere and lower stratosphere (UT/LS) is derived using the 1992 aviation fuel tracer simulation performed by eleven global atmospheric models. Key Endings are that subsonic aircraft emissions: (1) have not be responsible for the observed water vapor trends at 40 deg N; (2) could be a significant source of soot mass near 12 km, but not at 20 km; (3) might cause a noticeable increase in the background sulfate aerosol surface area and number densities (but not mass density) near the northern mid-latitude tropopause; and (4) could provide a global, annual mean top of the atmosphere radiative forcing up to +0.006 W/sq m and -0.013 W/sq m due to emitted soot and sulfur, respectively.

Danilin, M. Y.↗

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.↗

A Lagrangian View of Stratospheric Trace Gas Distributions

As a result of photochemistry, some relationship between the stratospheric age-of-air and the amount of tracer contained within an air sample is expected. The existence of such a relationship allows inferences about transport history to be made from observations of chemical tracers. This paper lays down the conceptual foundations for the relationship between age and tracer amount, developed within a Lagrangian framework. In general, the photochemical loss depends not only on the age of the parcel but also on its path. We show that under the "average path approximation" that the path variations are less important than parcel age. The average path approximation then allows us to develop a formal relationship between the age spectrum and the tracer spectrum. Using the relation between the tracer and age spectra, tracer-tracer correlations can be interpreted as resulting from mixing which connects parts of the single path photochemistry curve, which is formed purely from the action of photochemistry on an irreducible parcel. This geometric interpretation of mixing gives rise to constraints on trace gas correlations, and explains why some observations are do not fall on rapid mixing curves. This effect is seen in the ATMOS observations.

Schoeberl, M. R.↗