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Douglass, A. R.

Publications and source records attributed to Douglass, A. R..

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Seasonal Variability of Middle Latitude Ozone in the Lowermost Stratosphere Derived from Probability Distribution Functions

We present a study of the distribution of ozone in the lowermost stratosphere with the goal of understanding the relative contribution to the observations of air of either distinctly tropospheric or stratospheric origin. The air in the lowermost stratosphere is divided into two population groups based on Ertel's potential vorticity at 300 hPa. High [low] potential vorticity at 300 hPa suggests that the tropopause is low [high], and the identification of the two groups helps to account for dynamic variability. Conditional probability distribution functions are used to define the statistics of the mix from both observations and model simulations. Two data sources are chosen. First, several years of ozonesonde observations are used to exploit the high vertical resolution. Second, observations made by the Halogen Occultation Experiment [HALOE] on the Upper Atmosphere Research Satellite [UARS] are used to understand the impact on the results of the spatial limitations of the ozonesonde network. The conditional probability distribution functions are calculated at a series of potential temperature surfaces spanning the domain from the midlatitude tropopause to surfaces higher than the mean tropical tropopause [about 380K]. Despite the differences in spatial and temporal sampling, the probability distribution functions are similar for the two data sources. Comparisons with the model demonstrate that the model maintains a mix of air in the lowermost stratosphere similar to the observations. The model also simulates a realistic annual cycle. By using the model, possible mechanisms for the maintenance of mix of air in the lowermost stratosphere are revealed. The relevance of the results to the assessment of the environmental impact of aircraft effluence is discussed.

Cerniglia, M. C.↗

A Composite View of Lower Stratospheric Ozone Developed Using a Chemistry Transport Model and Observations from Airborne Lidar and Satellite

An ozone simulation from the Goddard three-dimensional chemistry and transport model for the 1995-96 northern hemisphere winter is compared with ozone observations from airborne Differential Absorption Lidar (DIAL), from the Polar Ozone and Aerosol Measurement (POAM), from the Microwave Limb Sounder (MLS), and from the Halogen Occultation Experiment (HALOE). The 3D model uses winds from the Goddard Data Assimilation System. The 3D model reproduces the latitude dependence of the horizontal and vertical ozone gradients of the subtropical DIAL observations. Comparisons with subtropical satellite observations, which lack the spatial resolution of DIAL but provide near continuous coverage throughout the subtropics, show that the model also reproduces longitude and temporal dependence in the tropical-midlatitude boundary. At polar latitudes, observations from DIAL flights on December 9 and January 30, and POAM and MLS between late December and late January are compared with the 3D model. Data from the three platforms consistently show that the observed ozone has a negative trend relative to the modeled ozone, and that the trend is uniform in time between early and mid winter, with no obvious dependence on proximity to the vortex edge.

Douglass, A. R.↗

Seasonal Variability of Middle Latitude Ozone in the Lowermost Stratosphere Derived from Probability Distribution Functions

We present a study of the distribution of ozone in the lowermost stratosphere with the goal of understanding the relative contribution to the observations of air of either distinctly tropospheric or stratospheric origin. The air in the lowermost stratosphere is divided into two population groups based on Ertel's potential vorticity at 300 hPa. High [low] potential vorticity at 300 hPa suggests that the tropopause is low [high], and the identification of the two groups helps to account for dynamic variability. Conditional probability distribution functions are used to define the statistics of the mix from both observations and model simulations. Two data sources are chosen. First, several years of ozonesonde observations are used to exploit the high vertical resolution. Second, observations made by the Halogen Occultation Experiment [HALOE) on the Upper Atmosphere Research Satellite [UARS] are used to understand the impact on the results of the spatial limitations of the ozonesonde network. The conditional probability distribution functions are calculated at a series of potential temperature surfaces spanning the domain from the midlatitude tropopause to surfaces higher than the mean tropical tropopause [approximately 380K]. Despite the differences in spatial and temporal sampling, the probability distribution functions are similar for the two data sources. Comparisons with the model demonstrate that the model maintains a mix of air in the lowermost stratosphere similar to the observations. The model also simulates a realistic annual cycle. By using the model, possible mechanisms for the maintenance of mix of air in the lowermost stratosphere are revealed. The relevance of the results to the assessment of the environmental impact of aircraft effluence is discussed.

Cerniglia, M. C.↗

Choosing Meteorological Input for the Global Modeling Initiative Assessment of High Speed Aircraft

The Global Modeling Initiative (GMI) science team is developing a three dimensional chemistry and transport model (CTM) to be used in assessment of the atmospheric effects of aviation. Requirements are that this model be documented be validated against observations, use a realistic atmospheric circulation, and contain numerical transport and photochemical modules representing atmospheric processes. The model must also retain computational efficiency to be tractable to use for multiple scenarios and sensitivity studies. To meet these requirements, a facility model concept was developed in which the different components of the CTM are evaluated separately. The first use of the GMI model will be to evaluate the impact of the exhaust of supersonic aircraft on the stratosphere. The assessment calculations will depend strongly on the wind and temperature fields used by the CTM. Three meteorological data sets for the stratosphere are available to GMI: the National Center for Atmospheric Research Community Climate Model (CCM2), the Goddard Earth Observing System Data Assimilation System (GEOS DAS), and the Goddard Institute for Space Studies general circulation model (GISS). Objective criteria were established by the GMI team to identify the data set which provides the best representation of the stratosphere. Simulations of gases with simple chemical control were chosen to test various aspects of model transport. The three meteorological data sets were evaluated and graded based on their ability to simulate these aspects of stratospheric measurements. This paper describes the criteria used in grading the meteorological fields. The meteorological data set which has the highest score and therefore was selected for GMI is CCM2. This type of objective model evaluation establishes a physical basis for interpretation of differences between models and observations. Further, the method provides a quantitative basis for defining model errors, for discriminating between different models, and for ready re-evaluation of improved models. These in turn will lead to a higher level of confidence in assessment calculations.

Douglass, A. R.↗

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.↗

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.↗

Contrast Between 1992 and 1997 High Latitude Spring Haloe Observations of Lower Stratospheric HCl

HCl measurements from HALOE in the northern hemisphere during mid-May 1997 revealed vortex fragments in which the chlorine reservoir partitioning was strongly pushed toward HCl (approx. 90% HCl, approx. 10% ClONO2), similar to partitioning previously observed in the Antarctic vortex region. In contrast, observations of ClONO2 and HCl in the northern polar spring, 1992, and in other years, show these species established the balance typical for gas phase photochemical reactions in this region (approx. 60% HCl, approx. 40% ClONO2). Annually, chlorine reservoirs in the winter lower stratosphere polar vortex are converted to chlorine radicals via heterogeneous reactions on particle surfaces at very cold temperatures (less than about 200 K). As temperatures warm in spring, the heterogeneous processes become insignificant compared with gas phase reactions, and the chlorine reservoirs are reformed. Measurements through the northern winter/spring in 1992 show rapid formation of ClONO2, followed by steady loss of ClONO2 and increasing HCl. Although ClONO2 measurements are not available for 1997, the HCl increase in 1997 is observed to be much more rapid and the eventual HCl mixing ratio is about 50% greater than that of 1992. The observations are examined through comparison with the Goddard three-dimensional chemistry and transport model. This model utilizes winds and temperatures from the Goddard Earth Observing System Data Assimilation System and a complete integration scheme for stratospheric photochemistry. Analysis of the evolution of HCl and ClONO2 shows that the observed difference in the overall rate of HCl formation is explained by the sensitivity of the gas-phase chemistry to the ozone mixing ratio and the temperature. The results show that the model accurately simulates HCl and ClONO2 evolution during these two winters. Model validity is further supported by comparisons with O3 and reactive nitrogen species NO and NO2. This analysis provides a sensitive test of the lower stratospheric chlorine photochemistry, particularly because the analysis considers constituent evolution at a time when the HCl and ClONO2 are far from a photochemical stationary state.

Douglass, A. R.↗

Ozone Budgets from a Global Chemistry/Transport Model and Comparison to Observations from POLARIS

The objective of the Photochemistry of Ozone Loss in the Arctic Region in Summer (POLARIS) field mission was to obtain data to better characterize the summertime seasonal decrease of ozone at mid to high latitudes. The decrease in ozone occurs mainly in the lower stratosphere and is expected to result from in situ chemical destruction. Instrumented balloons and aircraft were used in POLARIS, along with satellites, to measure ozone and chemical species which are involved with stratospheric ozone chemistry. In order to close the seasonal ozone budget, however, ozone transport must also be estimated. Comparison to a global chemistry and transport model (CTM) of the stratosphere indicates how well the summertime ozone loss processes are simulated and thus how well we can predict the ozone response to changing amounts of chemical source gases. Moreover, the model gives insight into the possible relative magnitude of transport contributions to the seasonal ozone decline. Initial comparison to the Goddard CTM, which uses transport winds and temperatures from meteorological data assimilation, shows a high ozone bias in the model and an attenuated summertime ozone loss cycle. Comparison of the model chemical partitioning and ozone catalytic loss rates to those derived from measurements shows fairly close agreement both at ER-2 altitudes (20 km) and higher. This suggests that the model transport is too active in resupplying ozone to the high latitude region, although chemistry failings cannot be completely ruled out. Comparison of ozone and related species will be shown along with a full diagnosis of the model ozone budget and its possible sources of error.

Kawa, S. Randolph↗

Doubled CO2 Effects on NO(y) in a Coupled 2D Model

Changes in temperature and ozone have been the main focus of studies of the stratospheric impact of doubled CO2. Increased CO2 is expected to cool the stratosphere, which will result in increases in stratospheric ozone through temperature dependent loss rates. Less attention has been paid to changes in minor constituents which affect the O3 balance and which may provide additional feedbacks. Stratospheric NO(y) fields calculated using the GSFC 2D interactive chemistry-radiation-dynamics model show significant sensitivity to the model CO2. Modeled upper stratospheric NO(y) decreases by about 15% in response to CO2 doubling, mainly due to the temperature decrease calculated to result from increased cooling. The abundance of atomic nitrogen, N, increases because the rate of the strongly temperature dependent reaction N + O2 yields NO + O decreases at lower temperatures. Increased N leads to an increase in the loss of NO(y) which is controlled by the reaction N + NO yields N2 + O. The NO(y) reduction is shown to be sensitive to the NO photolysis rate. The decrease in the O3 loss rate due to the NO(y) changes is significant when compared to the decrease in the O3 loss rate due to the temperature changes.

Rosenfield, J. E.↗

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.↗

Satellite observation and mapping of wintertime ozone variability in the lower stratosphere

Comparison is made between 30 mbar ozone fields that are generated by a transport chemistry model utilizing the winds from the Goddard Space Flight Center stratospheric data assimilation system (STRATAN), observations from the LIMS instrument on Nimbus-7, and the ozone fields that result from 'flying' a mathematical simulation of LIMS observations through the transport chemistry model ozone fields. The modeled ozone fields were found to resemble the LIMS observations, but the model fields show much more temporal and spatial structure than do the LIMS observations. The 'satellite mapped' model results resemble the LIMS observations much more closely. These results are very consistent with the earlier discussions of satellite space-time sampling by Salby.

Geller, M. A.↗

The atmospheric effects of stratospheric aircraft: A current consensus

In the early 1970's, a fleet of supersonic aircraft flying in the lower stratosphere was proposed. A large fleet was never built for economic, political, and environmental reasons. Technological improvements may make it economically feasible to develop supersonic aircraft for current markets. Some key results of earlier scientific programs designed to assess the impact of aircraft emissions on stratospheric ozone are reviewed, and factors that must be considered to assess the environmental impact of aircraft exhaust are discussed. These include the amount of nitrogen oxides injected in the stratosphere, horizontal transport, and stratosphere/troposphere assessment models are presented. Areas in which improvements in scientific understanding and model representation must be made to reduce the uncertainty in model calculations are identified.

Douglass, A. R.↗

Stratospheric responses to solar ultraviolet variations - Comparisons with photochemical models

At latitudes and altitudes where transport effects on ozone mixing ratio can be neglected, ozone and temperature responses to short-term changes in solar ultraviolet flux can be used to calculate implied bounds on two basic photochemical parameters: the odd oxygen photochemical relaxation time and the chemical sensitivity of odd oxygen to local temperature changes. Seasonally averaged values of these parameters are derived from response measurements and are compared with model calculations between 0.7 and 4 mbar at tropical latitudes. Results are in agreement within measurement and model uncertainties at all pressure levels. Model values of mean ozone and of the response of ozone to perturbations are functions of the same photochemical data. Therefore this agreement provides a constraint which should be considered when changes are proposed in model input data for the purpose of improving agreement between measured and calculated high-altitude ozone.

Hood, L. L.↗

Sensitivity of an atmospheric photochemistry model to chlorine perturbations including consideration of uncertainty propagation

Models of stratospheric photochemistry are generally tested by comparing their predictions for the composition of the present atmosphere with measurements of species concentrations. These models are then used to make predictions of the atmospheric sensitivity to perturbations. Here the problem of the sensitivity of such a model to chlorine perturbations ranging from the present influx of chlorine-containing compounds to several times that influx is addressed. The effects of uncertainties in input parameters, including reaction rate coefficients, cross sections, solar fluxes, and boundary conditions, are evaluated using a Monte Carlo method in which the values of the input parameters are randomly selected. The results are probability distributions for present atmosheric concentrations and for calculated perturbations due to chlorine from fluorocarbons. For more than 300 Monte Carlo runs the calculated ozone perturbation for continued emission of fluorocarbons at today's rates had a mean value of -6.2 percent, with a 1-sigma width of 5.5 percent. Using the same runs but only allowing the cases in which the calculated present atmosphere values of NO, NO2, and ClO at 25 km altitude fell within the range of measurements yielded a mean ozone depletion of -3 percent, with a 1-sigma deviation of 2.2 percent. The model showed a nonlinear behavior as a function of added fluorocarbons. The mean of the Monte Carlo runs was less nonlinear than the model run using mean value of the input parameters.

Stolarski, R. S.↗

Interpretation of ozone temperature correlations. II - Analysis of SBUV ozone data

In an effort to understand the behavior of ozone in the transition region, the terms in the perturbation continuity equation have been evaluated from solar backscattered ultraviolet ozone data, National Meteorological Center temperature data, and geostrophic winds derived from the temperature data at 2 mbar, winter 1978-1979. A linear parameterization is used to estimate the chemical source term. The perturbation ozone field calculated by integrating the net forcing evaluated from the data compares well with the measured perturbation ozone field. There are occasions during the winter when the sum of the dynamic terms is small due to cancellation, and the ozone and temperature perturbations are anticorrelated. The -1 correlation between the ozone and temperature perturbations does not necessarily imply that chemical forcing is dominant.

Douglass, A. R.↗