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Schoeberl, M. R.

Publications and source records attributed to Schoeberl, M. R..

At least 37 records · Page 2

Nighttime OClO in the Winter Arctic Vortex

We show that a nighttime profile of OClO in the Arctic vortex during the winter of 2000 is overestimated, by nearly a factor of 2, using an isentropic trajectory model constrained by observed profiles of ClOx (ClO + 2 X ClOOCl) and BrO. Calculated abundances of nighttime OClO are shown to be sensitive to the abundance of BrOx (BrO + BrCl), details of the air parcel history during the most recent sunrise/sunset transitions, and the BrCl yield from the reaction BrO + ClO. Many uncertainties are considered, and the discrepancy between measured and modeled nighttime OClO appears to be robust. This discrepancy suggests that production of OClO occurs more slowly than implied by standard photochemistry. If the yield of BrCl from the reaction of BrO + ClO is increased from 7% (JPL 2002 value) to 11% (near the upper limit of the uncertainty), good agreement is found between measured and modeled nighttime OClO. This study highlights the importance of accurate knowledge of BrO + ClO reaction kinetics as well as air parcel trajectories for proper interpretation of nighttime OClO. These factors have a considerably smaller impact on the interpretation of OClO observations obtained during twilight (90(deg) <=SZA <= 92(deg)), when photolytic processes are still active.

chlorine activation↗

Non-coincident Inter-instrument Comparisons of Ozone Measurements Using Quasi-conservative Coordinates

Ozone measurements from ozonesondes, AROTAL, DIAL, and POAM III instruments during the SOLVE-2/VINTERSOL period are composited in a time-varying, flow-following quasi-conservative (PV-6) coordinate space; the resulting composites from each instrument are mapped onto the other instruments locations and times. The mapped data are then used to intercompare data from the different instruments. Overall, the four data sets are found to be in good agreement. AROTAL shows somewhat lower values below 16 km, and DIAL has a positive bias at the upper limits of its altitude range. These intercomparisons are consistent with those obtained from more conventional near-coincident profiles, where available. Although the PV-theta mapping technique entails larger uncertainties of individual profile differences compared to direct near-coincident comparisons, the ability to include much larger numbers of comparisons can make this technique advantageous.

Lait, L. R.↗

Entrainment and Optical Properties of an Elevated Forest Fire Plume Transported into the Planetary Boundary Layer near Washington, D.C.

Smoke and pollutants from Canadian forest fires were transported over the northeastern United States in July 2002. Lidar observations at the NASA Goddard Space Flight Center show the smoke from these fires arriving in an elevated plume that was subsequently transported to the surface. Trajectory and three-dimensional model calculations confirm the origin of the smoke and show that it mixed to the surface after it was intercepted by the turbulent planetary boundary layer. Modeled smoke optical properties agreed well with aircraft and remote sensing observations provided coagulation of smoke particles was accounted for in the model. Our results have important implications for the long-range transport of pollutants and their subsequent entrainment to the surface, as well as the evolving optical properties of smoke from boreal forest fires.

Colarco, P. R.↗

Entrainment and Optical Properties of an Elevated Canadian Forest Fire Plume Transported into the Planetary Boundary Layer near Washington, D.C.

Smoke and pollutants from Canadian forest fires were transported over the northeastern United States in July 2002. Lidar observations at the NASA Goddard Space Flight Center show the smoke from these fires arriving in an elevated plume that was subsequently mixed to the surface. Trajectory and three-dimensional model calculations confirm the origin of the smoke and show that it mixed to the surface after it was intercepted by the turbulent planetary boundary layer. Modeled smoke optical properties agreed well with aircraft and remote sensing observations provided coagulation of smoke particles was accounted for in the model. Our results have important implications for the long-range transport of pollutants and their subsequent entrainment to the surface, as well as the evolving optical properties of smoke from boreal forest fires.

Colarco, P. R.↗

Impacts of PSC Microphysics on Modelled Ozone Loss

Winter-long simulations of the 1999-2000 winter using a coupled microphysical/chemical model have been carried out to explore how PSC microphysics affects ozone loss. Although many models assures that water ice formation leads to denitrification, these simulations show that observed characteristics of the 1999-2000 winter can not be reproduced by such a denitrification mechanism. Instead, denitrification observations are best reproduced by a small number of particles freezing at temperatures near the nitric acid trihydration condensation point. Implications of such a mechanism for assessments of future ozone loss will be discussed. The simulations have also revealed that ozone loss during the 1999-2000 winter was sensitive to chlorine reactivation that occurred during February. Uncertainties in PSC microphysics and heterogeneous reaction rates both influence the modelled chlorine reactivation. For the 1999-2000 winter, these uncertainties have a larger effect on model ozone loss than denitrification. The role of denitrification would have increased if the Arctic vortex had persisted for a longer period.

Drdla, K.↗

The Distribution of Ozone in the Early Stages of Polar Vortex Development

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, 1999-2000 has a characteristic distribution, which is consistent between in situ and satellite measurements [Kawa et al., The Interaction Between Dynamics and Chemistry of Ozone in the Set-up Phase of the Northern Hemisphere Polar Vortex, submitted manuscript, 2001 ]. 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 at 3 ppmv +/- approx.10%. Values outside the vortex are up to a factor of 2 higher and increase significantly with potential temperature. The seasonal time series of POAM data shows that relatively low O3 mixing ratios, which characterize the vortex in late fall, are already present at high latitudes at the end of summer in September before the vortex circulation sets up. This suggests a possible feedback role between O3 chemistry and the formation of the vortex, which is dominated by the seasonal radiation balance. Here we show that these characteristic O3 distributions are consistent from year to year and between the hemispheres. We will attempt to determine whether variations in fall vortex O3 are related in any way to O3 abundances and vortex structure later during winter and into spring.

Kawa, S. 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.↗

The Interaction Between Dynamics and Chemistry of Ozone in the Set-up Phase of the Northern Hemisphere Polar Vortex

The morphology and evolution of the stratospheric ozone (O3) distribution at high latitudes in the Northern Hemisphere (NH) are examined for the late summer and fall seasons of 1999. This time period sets the O3 initial condition for the SOLVE/THESEO field mission performed during winter 1999-2000. In situ and satellite data are used along with a three-dimensional model of chemistry and transport (CTM) to determine the key processes that control the distribution of O3 in the lower-to-middle stratosphere. O3 in the vortex at the beginning of the winter season is found to be nearly constant from 500 to above 800 K with a value at 3 ppmv +/- approx. 10%. Values outside the vortex are up to a factor of 2 higher and increase significantly with potential temperature. The seasonal time series of data from POAM shows that relatively low O3 mixing ratios, which characterize the vortex in late fall, are already present at high latitudes at the end of summer before the vortex circulation sets up. Analysis of the CTM output shows that the minimum O3 and increase in variance in late summer are the result of: 1) stirring of polar concentric O3 gradients by nascent wave-driven transport, and 2) an acceleration of net photochemical loss with decreasing solar illumination. The segregation of low O3 mixing ratios into the vortex as the circulation strengthens through the fall suggests a possible feedback role between O3 chemistry and the vortex formation dynamics. Trajectory calculations from O3 sample points early in the fall, however, show only a weak correlation between initial O3 mixing ratio and potential vorticity later in the season consistent with order-of-magnitude calculations for the relative importance of O3 in the fall radiative balance at high latitudes. The possible connection between O3 chemistry and the dynamics of vortex formation does suggest that these feedbacks and sensitivities need to be better understood in order to make confident predictions of the recovery of NH O3.

Kawa, S. R.↗

Ozone Loss From Quasi-Conservative Coordinate Mapping During the 1999-2000 SOLVE Campaign

During the winter of 1999-2000, the Sage III Ozone Loss and Validation Experiment (SOLVE) field experiment took place in Kiruna, Sweden. The purpose of SOLVE was to examine ozone depletion mechanisms in the Arctic stratosphere (from about 10 to 50 km altitude) during the winter and early spring, when a band of strong winds (the 'polar vortex') circle the pole. Measurements of stratospheric ozone were made by several different kinds of instruments in different meteorological situations. We analyzed these data using the 'quasi-conservative coordinate mapping' technique, in which the measurements are analyzed in terms of meteorological properties ('potential temperature' and 'potential vorticity') which tend not to change very much over a few days. This technique reduces or removes the changes that are associated with the polar vortex moving around. Over longer time periods, potential temperature and potential vorticity change as air cools and descends within the polar vortex. We account for these changes by calculating the trajectories of air parcels, and this enables us to extend the analysis over a ten-week period from January 10 to March 17, 2000. Using data from the NASA ER-2 aircraft, from the DIAL and AROTEL laser sounders on the NASA DC-8 aircraft, and balloon-borne ozonesondes, our analysis reveals changes in ozone which, because we have removed the effects of polar vortex motion and the descending air, indicate chemical destruction of ozone in early 2000. We find a peak decline rate of approximately 0.03 ppmv/day near 470 K of potential temperature (near 20 km) in mid-January which sinks in altitude to around 440 K (near 18 km) in mid-March.

Lait, L. R.↗

Stratospheric Polar Freezing Belt Causes Denitrification

Trajectory cloud model calculations are presented to show that homogeneous freezing of nitric acid hydrates can produce a polar freezing belt in both hemispheres that can cause denitrification. While hydrate cloud microphysical properties are similar over both poles, the shorter persistence of clouds in the Arctic prevents the depth of the denitrified layers from growing beyond a few kilometers. The 1999-2000 Arctic winter is unique in showing a distinct denitrification profile with a depth of approx. 4.5 km that is nearly half as deep as that computed for a typical Antarctic winter.

Tabazadeh, A.↗

On the Origin of Polar Vortex Air

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.

Rosenfield, J. E.↗

Retrieval of Black Carbon Absorption from Proposed Satellite Measurements Over the Ocean Glint

Haze and air pollution includes many chemicals that together form small particles suspended in the air called aerosols. One of the main ingredients found to affect climate and human health is Black Carbon. Black particles emitted from engines that do not burn the fuel completely, e.g. old trucks. Black carbon absorption of sunlight emerges as one of the key components of man-made forcing of climate. However, global characterization of black carbon emissions, distribution and pathways in which it can affect the amount of solar radiation absorbed by the atmosphere is very uncertain. A new method is proposed to measure sunlight absorption by fine aerosol particles containing black carbon over the ocean glint from a satellite mission designed for this purpose. The satellite will scan the same spot over the ocean in the glint plane and a plane 40 degrees off-glint a minute apart, collecting measurements of the reflected light across the solar spectrum. First the dark ocean off the glint is used to derive aerosol properties. Then the black carbon absorption is derived prop the attenuation of the bright glint by the aerosol layer. Such measurements if realized in a proposed future mission - COBRA are expected to produce global monthly climatology of black carbon absorption with high accuracy (110 to 15%) that can show their effect on climate.

Kaufman, Y. J.↗

Microphysical Modelling of the 1999-2000 Arctic Winter: Chlorine Activation and Ozone Depletion - 2

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.

Drdla, K.↗

A Composite View of Ozone Evolution in the 1995-1996 Northern Winter Polar Vortex Developed from Airborne Lidar and Satellite Observations

The processes which contribute to the ozone evolution in the high latitude northern lower stratosphere are evaluated using a three dimensional model simulation and ozone observations. The model uses winds and temperatures from the Goddard Earth Observing System Data Assimilation System. The simulation results are compared with ozone observations from three platforms: the differential absorption lidar (DIAL) which was flown on the NASA DC-8 as part of the Vortex Ozone Transport Experiment; the Microwave Limb Sounder (MLS); the Polar Ozone and Aerosol Measurement (POAM II) solar occultation instrument. Time series for the different data sets are consistent with each other, and diverge from model time series during December and January. The model ozone in December and January is shown to be much less sensitive to the model photochemistry than to the model vertical transport, which depends on the model vertical motion as well as the model vertical gradient. We evaluate the dependence of model ozone evolution on the model ozone gradient by comparing simulations with different initial conditions for ozone. The modeled ozone throughout December and January most closely resembles observed ozone when the vertical profiles between 12 and 20 km within the polar vortex closely match December DIAL observations. We make a quantitative estimate of the uncertainty in the vertical advection using diabatic trajectory calculations. The net transport uncertainty is significant, and should be accounted for when comparing observations with model ozone. The observed and modeled ozone time series during December and January are consistent when these transport uncertainties are taken into account.

Douglass, A. R.↗

A Composite View of Ozone Evolution in the 1995-96 Northern Winter Polar Vortex Developed from Airborne Lidar and Satellite Observations

The processes which contribute to the ozone evolution in the high latitude lower stratosphere are evaluated using a three dimensional model simulation and ozone observations. The model uses winds and temperatures from the Goddard Earth Observing System Data Assimilation System. The simulation results are compared with ozone observations from three platforms: the differential absorption lidar (DIAL) which was flown on the NASA DC-8 as part of the Vortex Ozone Transport Experiment; the Microwave Limb Sounder (MLS) on the Upper Atmosphere Research Satellite; and the Polar Ozone and Aerosol Measurement (POAM II) solar occulation instrument, on board the French Satellite Pour I'Observations de la Terre. Comparisons of the different data sets with the model simulation are shown to provide complementary information and a consistent view of the ozone evolution. The model ozone in December and January is shown to be sensitive to the ozone vertical gradient and the model vertical transport, and only weakly sensitive to the model photochemistry. The most consistent comparison between observed and modeled ozone evolution is found for a simulation where the vertical profiles between 12 and 20 km within the polar vortex closely match December DIAL observations. Diabatic trajectory calculations are used to estimate the uncertainty due to vertical advection quantitatively. The transport uncertainty is significant, and should be accounted for when comparing observations with model ozone. The model ozone evolution during December and January is broadly consistent with the observations when these transport uncertainties are taken into account.

Douglass, Anne R.↗

Chance Encounter with a Stratospheric Kerosene Rocket Plume From Russia Over California

A high-altitude aircraft flight on April 18, 1997 detected an enormous aerosol cloud at 20 km altitude near California (37 N). Not visually observed, the cloud had high concentrations of soot and sulfate aerosol, and was over 180 km in horizontal extent. The cloud was probably a large hydrocarbon fueled vehicle, most likely from rocket motors burning liquid oxygen and kerosene. One of two Russian Soyuz rockets could have produced the cloud: a launch from the Baikonur Cosmodrome, Kazakhstan on April 6; or from Plesetsk, Russia on April 9. Parcel trajectories and long-lived trace gas concentrations suggest the Baikonur launch as the cloud source. Cloud trajectories do not trace the Soyuz plume from Asia to North America, illustrating the uncertainties of point-to-point trajectories. This cloud encounter is the only stratospheric measurement of a hydrocarbon fuel powered rocket.

Newman, P. A.↗