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Weisenstein, D. K.

Publications and source records attributed to Weisenstein, D. K..

15 records
All sourcesNASA NTRSDOE OSTI
NASA NTRS2006

Toward a Better Quantitative Understanding of Polar Stratospheric Ozone Loss

Previous studies have shown that observed large O3 loss rates in cold Arctic Januaries cannot be explained with current understanding of the loss processes, recommended reaction kinetics, and standard assumptions about total stratospheric chlorine and bromine. Studies based on data collected during recent field campaigns suggest faster rates of photolysis and thermal decomposition of ClOOCl and higher stratospheric bromine concentrations than previously assumed. We show that a model accounting for these kinetic changes and higher levels of BrO can largely resolve the January Arctic O3 loss problem and closely reproduces observed Arctic O3 loss while being consistent with observed levels of ClO and ClOOCl. The model also suggests that bromine catalyzed O3 loss is more important relative to chlorine catalyzed loss than previously thought.

Frieler, K.↗
NASA NTRS2006

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.↗
NASA NTRS2005

Sensitivity of Ozone to Bromine in the Lower Stratosphere

Measurements of BrO suggest that inorganic bromine (Br(sub y)) at and above the tropopause is 4 to 8 ppt greater than assumed in models used in past ozone trend assessment studies. This additional bromine is likely carried to the stratosphere by short-lived biogenic compounds and their decomposition products, including tropospheric BrO. Including this additional bromine in an ozone trend simulation increases the computed ozone depletion over the past approx.25 years, leading to better agreement between measured and modeled ozone trends. This additional Br(sub y) (assumed constant over time) causes more ozone depletion because associated BrO provides a reaction partner for ClO, which increases due to anthropogenic sources. Enhanced Br(sub y) causes photochemical loss of ozone below approx.14 km to change from being controlled by HO(sub x) catalytic cycles (primarily HO2+O3) to a situation where loss by the BrO+HO2 cycle is also important.

ozone trends↗
NASA NTRS1998

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.↗
NASA NTRS1998

Transport Between the Tropical and Midlatitude Lower Stratosphere: Implications for Ozone Response to High Speed Civil Transport Emissions

Several recent studies have quantified the air exchange rate between the tropics and midlatitudes in the lower stratosphere using airborne and satellite measurements of chemical species. It is found that the midlatitude air is mixed into the tropical lower stratosphere with a replacement timescale of 13.5 months (with 20% uncertainty) for the region from the tropopause to 21 km and at least 18 months for the region of 20-28 km. These estimates are used to adjust the horizontal eddy diffusion coefficients, K(sub yy), in a two-dimensional chemistry transport model. The value of K(sub yy) previously used to simulate the subtropical barrier, 0.03 x 10(exp 6)sq m/s, generates an exchange time of about 4 years, and the model without subtropical barrier (K(sub yy) = 0.3 x 10(exp 6)sq m/s) has an exchange time of 5 months. Adjusting the K(sub yy) to 0.13 x 10(exp 6) sq m/s from the tropopause to 21 km and 0.07 x 10(exp 6)sq m/s above 21 km produces the exchange timescales which match the estimates deduced from the measurements. The subtropical barrier prevents the engine emissions of the high-speed civil transport (HSCT) aircraft from being transported into the tropics and subsequently lifted into the upper atmosphere or mixed into the southern hemisphere. The model results show that the calculated ozone response to HSCT aircraft emissions using the K(sub yy), adjusted to observed mixing rates is substantially smaller than that simulated without the subtropical barrier.

Shia, R.-L.↗
NASA NTRS1998

Transport Between the Tropical and Midlatitude Lower Statosphere: Implications for Ozone Response to High-Speed Civil Transport Emissions

Several recent studies have quantified the air exchange rate between the tropics and midlatitudes in the lower stratosphere using airborne and satellite measurements of chemical species. It is found that the midlatitude air is mixed into the tropical lower stratosphere with a replacement timescale of 13.5 months (with 20% uncertainty) for the region from the tropopause to 21 km and at least 18 months for the region of 20-28 km. These estimates are used to adjust the horizontal eddy diffusion coefficients, K(sub yy), in a two-dimensional chemistry transport model. The value of K(sub yy) previously used to simulate the subtropical barrier, 0.03 x 10(exp 6) sq m/s, generates an exchange time of about 4 years, and the model without subtropical barrier (K(sub yy) = 0.3 x 10(exp 6) sq m/s) has an exchange time of 5 months. Adjusting the K(sub yy) to 0.13 x 10(exp 6) sq m/s from the tropopause to 21 km and 0.07 x 10(exp 6) sq m/s above 21 km produces the exchange timescales which match the estimates deduced from the measurements. The subtropical barrier prevents the engine emissions of the high-speed civil transport (HSCT) aircraft from being transported into the tropics and subsequently lifted into the upper atmosphere or mixed into the southern hemisphere. The model results show that the calculated ozone response to HSCT aircraft emissions using the K(sob yy) adjusted to observed mixing rates is substantially smaller than that simulated without the subtropical barrier.

Shia, R.-L.↗
NASA NTRS1998

Nitrogen Species in the Post-Pinatubo Stratosphere: Model Analysis Utilizing UARS Measurements

We present an analysis of the impact of heterogeneous chemistry on the partitioning of nitrogen species measured by the Upper Atmosphere Research Satellite (UARS) instruments. The UARS measurements utilized include: N2O, HNO3 and ClONO2 (Cryogen Limb Array Etalon Spectrometer (CLAES), version 7), temperature, methane, ozone, H2O, HCl, NO and NO2 (HALogen Occultation Experiment (HALOE), version 18). The analysis is carried out for the data from January 1992 to September 1994 in the 100-1 mbar (approx.17-47 km) altitude range and over 10 degree latitude bins from 70degS to 70degN. Temporal-spatial evolution of aerosol surface area density (SAD) is adopted according to the Stratospheric Aerosol and Gas Experiment (SAGE) 11 data. A diurnal steady-state photochemical box model, constrained by the temperature, ozone, H2O, CH4, aerosol SAD and columns of O2 and O3 above the point of interest, has been used as the main tool to analyze these data. Total inorganic nitrogen (NO(y)) is obtained by three different methods: (1) as a sum of the UARS measured NO, NO2, HNO3, and ClONO2; (2) from the N2O-NO(y) correlation, and (3) from the CH4-NO(y) correlation. To validate our current understanding of stratospheric heterogeneous chemistry for post-Pinatubo conditions, the model-calculated NO(x)/NO(y) ratios and the NO, NO2, and HNO3 profiles are compared to the UARS-derived data. In general, the UARS-constrained box model captures the main features of nitrogen species partitioning in the post-Pinatubo years. However, the model underestimates the NO2 content, particularly, in the 30-7 mbar (approx. 23-32 km) range. Comparisons of the calculated temporal behavior of the partial columns of NO2 and HNO3 and ground based measurements at 45degS and 45degN are also presented. Our analysis indicates that ground-based and HALOE v. 18 measurements of the NO2 vertical columns are consistent within the range of their uncertainties and are systematically higher (up to 50%) than the model results at mid-latitudes in both hemispheres. Reasonable agreement is obtained for HNO3 columns at 45degS suggesting some problems with nitrogen species partitioning in the model. Outstanding uncertainties are discussed.

Danilin, M. Y.↗
NASA NTRS1998

Nitrogen Species in the Post-Pinatubo Stratosphere: Model Analysis Utilizing UARS Measurements

We present an analysis of the impact of heterogeneous chemistry on the partitioning of nitrogen species measured by the Upper Atmosphere Research Satellite (UARS) instruments. The UARS measurements utilized include: N2O, HNO3 and ClONO2 (Cryogen Limb Array Etalon Spectrometer (CLAES), version 7), temperature, methane, ozone, H2O, HCI, NO and NO2 (HALogen Occultation Experiment (HALOE), version 18). The analysis is carried out for the data from January 1992 to September 1994 in the 100-1 mbar (approximately 17-47 km) altitude range and over 10 degree latitude bins from 70 deg S to 70 deg N. Temporal-spatial evolution of aerosol surface area density (SAD) is adopted according to the Stratospheric Aerosol and Gas Experiment (SAGE) II data. A diurnal steady-state photochemical box model, constrained by the temperature, ozone, H2O, CH4, aerosol SAD and columns of O2 and O3 above the point of interest, has been used as the main tool to analyze these data. Total inorganic nitrogen (NOy) is obtained by three different methods: (1) as a sum of the UARS measured NO, NO2, HNO3, and CIONO2; (2) from the N2O-NOy correlation, (3) from the CH4-NOy correlation. To validate our current understanding of stratospheric heterogeneous chemistry for post-Pinatubo conditions, the model-calculated NOx/NOy ratios and the NO, NO2, and HNO3 profiles are compared to the UARS-derived data. In general, the UARS-constrained box model captures the main features of nitrogen species partitioning in the post-Pinatubo years. However, the model underestimates the NO2 content, particularly, in the 30-7 mbar (approximately 23-32 km) range. Comparisons of the calculated temporal behavior of the partial columns of NO2 and HNO3 and ground based measurements at 45 deg S and 45 deg N are also presented. Our analysis indicates that ground-based and HALOE v.18 measurements of the NO2 vertical columns are consistent within the range of their uncertainties and are systematically higher (up to 50%) than the model results at mid-latitudes in both hemispheres. Reasonable agreement is obtained for HNO3 columns at 45 deg S suggesting some problems with nitrogen species partitioning in the model. Outstanding uncertainties are discussed.

Danilin, M. Y.↗
NASA NTRS1998

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.↗
NASA NTRS1996

Continued development and validation of the AER two-dimensional interactive model

Results from two-dimensional chemistry-transport models have been used to predict the future behavior of ozone in the stratosphere. Since the transport circulation, temperature, and aerosol surface area are fixed in these models, they cannot account for the effects of changes in these quantities, which could be modified because of ozone redistribution and/or other changes in the troposphere associated with climate changes. Interactive two-dimensional models, which calculate the transport circulation and temperature along with concentrations of the chemical species, could provide answers to complement the results from three-dimension model calculations. In this project, we performed the following tasks in pursuit of the respective goals: (1) We continued to refine the 2-D chemistry-transport model; (2) We developed a microphysics model to calculate the aerosol loading and its size distribution; (3) The treatment of physics in the AER 2-D interactive model were refined in the following areas--the heating rate in the troposphere, and wave-forcing from propagation of planetary waves.

Ko, M. K. W.↗
NASA NTRS1994

Increase in Levels of Stratospheric Chlorine and Fluorine Loading between 1985 and 1992

Mixing ratios of 3.44 ppbv (parts per billion by volume) and 1.23 ppbv for HCl and HF above 50 km, surrogates for total chlorine and fluorine, have been measured by the Atmospheric Trace Molecule Spectroscopy (ATMOS) experiment on a March 1992 flight of the Space Shuttle. Compared to the measured values obtained on a 1985 flight, these correspond to a 37% and 62% increase for HCl and HF, respectively. The derived trend in HCl (approx. 0.13 ppbv per year) is in good agreement with the model-predicted increase in chlorine loading of 0.13 ppbv per year, and with the measured trends in HCl total column abundance from reported ground-based observations. The main source of this change can be attributed to the release of man-made chlorofluorocarbons (CFC's) and hydro-chloro-fluoro-carbons (HCFC's). This new value for HCl represents an upper limit to the inorganic chlorine concentration in the stratosphere available for participation in photochemical processes which destroy ozone.

Gunson, M. R.↗
NASA NTRS1994

Effect of lightning on the concentration of odd nitrogen species in the lower stratosphere: An update

Revised model estimates of the effect of lightning on the lower stratospheric NOy are presented. Several changes in the Atmospheric and Environmental Research Incorporated model were made since the last evaluation of the impact of lightning. Improvements were made in the model circulation and location of tropopause in the tropics, which is now calculated from the National Meteorological Center temperature data. Changes in model circulation reduced the mass flux from the troposphere to the tropical stratosphere. The calculated mass fluxes are found to agree better with some recent estimates. The circulation changes also reduced the advective mass flux from the tropical lower stratosphere to the midlatitudes. The change in circulation and the change in the tropopause height lead to increases in the calculated concentration of N2O, O3 and NOy in the tropical lower stratosphere. The effect of lightning is to increase the calculated concentration of NOy around 64 mbar by a factor of 2, compared to a factor of 10 enhancement in the previous calculations. Comparison with the Stratosphere Troposphere Exchange Project 1987 data indicates that the inclusion of a lightning source brings the model results in closer agreement with the observations.

Kotamarthi, V. R.↗
NASA NTRS1994

Secular evolution of the vertical column abundances of CHClF2 (HCFC-22) in the Earth's atmosphere inferred from ground-based IR solar observations at the Jungfraujoch and at Kitt Peak, and comparison with model calculations

Series of high-resolution infrared solar spectra recorded at the International Scientific Station of the Jungfraujoch, Switzerland, between 06/1986 and 11/1992, and at Kitt Peak National Observatory, Tucson, Arizona (U.S.A.), from 12/1980 to 04/1992, have been analyzed to provide a comprehensive ensemble of vertical column abundances of CHClF2 (HCFC-22; Freon-22) above the European and the North American continents. The columns were derived from nonlinear least-squares curve fittings between synthetic spectra and the observations containing the unresolved 2 nu(sub 6) Q-branch absorption of CHClF2 at 829.05/cm. The changes versus time observed in these columns were modeled assuming both an exponential and a linear increase with time. The exponential rates of increase at one-sigma uncertainties were found equal to (7.0 +/- 0.35)%/yr for the Junfraujoch data and (7.0 +/- 0.23)%/yr for the Kitt Peak data. The exponential trend of 7.0%/yr found at both stations widely separated in location can be considered as representative of the global increase of the CHClF2 burden in the Earth's atmosphere during the period 1980 to 1992. When assuming two realistic vertical volume mixing ratio profiles for CHClF2 in the troposphere, one quasi constant and the other decreasing by about 13% from the ground to the tropopause, the concentrations for mid-1990 were found to lie between 97 and 111 pptv (parts per trillion by volume) at the 3.58 km altitude of the Jungfraujoch and between 97 and 103 pptv at Kitt Peak, 2.09 km above sea level. Corresponding values derived from calculations using a high vertical resolution-2D model and recently compiled HCFC-22 releases to the atmosphere, were equal to 107 and 105 pptv, respectively, in excellent agreement with the measurements. The model calculated lifetime of CHClF2 was found equal to 15.6 years. The present results are compared critically with similar data found in the literature. On average, the concentrations found here are lower by 15-20% than those derived from in situ investigations; this difference cannot be explained by the absolute uncertainty of +/- 11% assigned presently to the infrared remote measurements.

Zander, R.↗
NASA NTRS1989

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

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

Sze, N. D.↗