ALBERT

Description: 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.

Description: 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.

Description: Ozone observations from ozonesondes, the DIAL and AROTEL lidars aboard the DC-8, in situ ozone measurements from the ER-2 and satellite ozone measurements from POAM were used to assess ozone loss during the SOLVE 1999-2000 campaign. We compare three different methods of computing the ozone loss. The first method simply compares the time sequence of ozonesondes taken at the same station inside the vortex from December through the end of March. In the second method, ozonesondes from a variety of stations are compared using a variant on the Match technique. This method uses short (approx. 5-10 day) forward diabatic trajectories to connect various sonde launches. In the third method, the measurements are simply injected into a diabatic trajectory model and carried forward in time from December 1 to March 16. Over 60,000 individual measurements were used in the last calculation. Again, ozone loss is estimated by comparing vortex interior measurements made early in the campaign with those made later in the campaign. The diabatic nature of the second and third methods calculation presumably corrects for the normal increase in ozone within the vortex due to downward advection. The three methods agree that the largest ozone loss occurs between 400 and 460 K potential temperatures (approx. 16-20 km) with slightly over 1.5 ppmv lost over the winter period. Between 460 K and 500 K (approx. 22 km) net ozone loss is less than 0.8 ppmv. From 500K to 600K (26 km) net loss is less than 0.5 ppmv.

Description: The existence of the multi-year HALOE CH4 data set, together with some comparisons of forward with back trajectory calculations which we have carried out, has motivated us to reexamine the question of polar vortex descent. Three-dimensional diabatic trajectory calculations have been carried out for the seven month fall to spring period in both the northern hemisphere (NH) and southern hemisphere (SH) polar stratosphere for the years 1992-1999. These computations are compared to fixed descent computations where the parcels were fixed at their latitude-longitude locations and allowed to descend without circulating. The forward trajectory computed descent is always less than the fixed descent due to horizontal parcel motions and variations in heating rates with latitude and longitude. Although the forward calculations estimate the maximum amount of descent that can occur, they do not necessarily indicate the actual origin of springtime vortex air. This is because more equator-ward air can be entrained within the vortex during its formation. To examine the origin of the springtime vortex air, the trajectory model was run backward for seven months from spring to fall. The back trajectories show a complex distribution of parcels in which one population originates in the upper stratosphere and mesosphere and experiences considerable descent in the polar regions, while the remaining parcels originate at lower altitudes of the middle and lower stratosphere and are mixed into the polar regions during vortex formation without experiencing as much vertical transport. The amount of descent experienced by the first population shows little variability from year to year, while the computed descent and mixing of the remaining parcels show considerable interannual variability due to the varying polar meteorology. Because of this complex parcel distribution it is not meaningful to speak of a net amount of descent experienced over the entire winter period. Since the back trajectories indicate that much of the air can come from lower altitudes than would be implied by the forward calculations, using a comparison between pre-winter and post-winter tracer profiles to estimate the amount of descent over this period will give erroneous descent amounts. In order to evaluate the computed descent, spring methane amounts were computed by mapping HALOE fall observations onto the final latitude-altitude locations of the back trajectories. These locations indicate the origin of the spring vortex air. The agreement between the computed means and the spring HALOE means is generally within 0.1-0.2 ppmv in the NH and 0.1-0.4 ppmv in the SH.

Description: Hemispherical dispersion of the SO2 cloud from the August 2008 Kasatochi eruption is analyzed using satellite data from the Ozone Monitoring Instrument (OMI) and the Goddard Trajectory Model (GTM). The operational OMI retrievals underestimate the total SO2 mass by 20-30% on 8-11 August, as compared with more accurate offline Extended Iterative Spectral Fit (EISF) retrievals, but the error decreases with time due to plume dispersion and a drop in peak SO2 column densities. The GTM runs were initialized with and compared to the operational OMI SO2 data during early plume dispersion to constrain SO2 plume heights and eruption times. The most probable SO2 heights during initial dispersion are estimated to be 10-12 km, in agreement with direct height retrievals using EISF algorithm and IR measurements. Using these height constraints a forward GTM run was initialized on 11 August to compare with the month-long Kasatochi SO2 cloud dispersion patterns. Predicted volcanic cloud locations generally agree with OMI observations, although some discrepancies were observed. Operational OMI SO2 burdens were refined using GTM-predicted mass-weighted probability density height distributions. The total refined SO2 mass was integrated over the Northern Hemisphere to place empirical constraints on the SO2 chemical decay rate. The resulting lower limit of the Kasatochi SO2 e-folding time is approx.8-9 days. Extrapolation of the exponential decay back in time yields an initial erupted SO2 mass of approx.2.2 Tg on 8 August, twice as much as the measured mass on that day.

Description: We present comparisons of simulations of upper tropospheric humidity at 215 and 146 hPa with satellite measurements. Our model uses diabatic trajectories to advect water vapor from an initial condition of 100% relative humidity to the final state. The model does not allow parcels' relative humidity to exceed 100%, and in this way crudely incorporates condensation. We find that this simple model does a good job of simulating the observations. Sensitivity studies suggest that one must have realistic wind velocities in order to accurately simulate the humidity distribution; microphysical parameterizations seem to be less important. Comparisions between simulations using UKMO and NCEP horizontal winds will be discussed.

Description: Project Loon has been launching super-pressure balloons since January 2013 to provide worldwide Internet coverage. These balloons typically fly between 18-21 km and provide measurements of winds and pressure fluctuations in the lower stratosphere. We divide 1,560 Loon flights into 3,405 two-day segments for gravity wave analysis. We derive the kinetic energy spectrum from the horizontal balloon motion and estimate the temperature perturbation spectrum (proportional to the potential energy spectrum) from the pressure variations. We fit the temperature (and kinetic energy) data to the functional form T'2=T'o 2(omega/omega())lpha where omega is the wave frequency, omega() is daily frequency, T'o is the base temperature amplitude and alpha is the slope. Both the kinetic energy and temperature spectra show -1.9 +/- 0.2 power-law dependence in the intrinsic frequency window 3 - 50 cycles/day. The temperature spectrum slope is weakly anticorrelated with the base temperature amplitude. We also find that the wave base temperature distribution is highly skewed. The average tropical modal temperature is 0.77 K. The highest amplitude waves occur over the mountainous regions, the tropics, and the high southern latitudes. Temperature amplitudes show little height variation over our 18-21 km domain. Our results are consistent with other limited super-pressure balloon analyses. The modal temperature is higher than the temperature currently used in Lagrangian model gravity wave parameterizations.

Description: The effect of a range of assumptions about polar stratospheric clouds (PSCs) on ozone depletion has been assessed using at couple microphysical/photochemical model. The composition of the PSCs was varied (ternary solutions, nitric acid trihydrate, nitric acid dehydrate, or ice), as were parameters that affected the levels of denitrification and dehydration. Ozone depletion was affected by assumptions about PSC freezing because of the variability in resultant nitrification chlorine activation in all scenarios was similar despite the range of assumed PSC compositions. Vortex-average ozone loss exceeded 40% in the lower stratosphere for simulations without nitrification an additional ozone loss of 15-20% was possible in scenarios where vortex-average nitrification reached 60%. Ozone loss intensifies non-linearly with enhanced nitrification in air parcels with 90% nitrification 40% ozone loss in mid-April can be attributed to nitrification alone. However, these effects are sensitive to the stability of the vortex in springtime: nitrification only began to influence ozone depletion in mid-March.

Description: 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.

Description: Biomass burning is an important source of chemical precursors of tropospheric ozone. In the tropics, biomass burning produces ozone enhancements over broad regions of Indonesia, Africa, and South America including Brazil. Fires are intentionally set in these regions during the dry season each year to clear cropland and to clear land for human/industrial expansion. In Indonesia enhanced burning occurs during dry El Nino conditions such as in 1997 and 2006. These burning activities cause enhancement in atmospheric particulates and trace gases which are harmful to human health. Measurements from the Aura Ozone Monitoring Instrument (OMI) and Microwave Limb Sounder (MLS) from October 2004-November 2008 are used to evaluate the effects of biomass burning on tropical tropospheric ozone. These measurements show sizeable decreases approx.15-20% in ozone in Brazil during 2008 compared to 2007 which we attribute to the reduction in biomass burning. Three broad biomass burning regions in the tropics (South America including Brazil, western Africa, and Indonesia) were analyzed in the context of OMI/MLS measurements and the Global Modeling Initiative (GMI) chemical transport model developed at Goddard Space Flight Center. The results indicate that the impact of biomass burning on ozone is significant within and near the burning regions with increases of approx.10-25% in tropospheric column ozone relative to average background concentrations. The model suggests that about half of the increases in ozone from these burning events come from altitudes below 3 km. Globally the model indicates increases of approx.4-5% in ozone, approx.7-9% in NO, (NO+NO2), and approx.30-40% in CO.