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NASA NTRS1999

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.↗
NASA NTRS1999

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 from the cryogenic limb array etalon spectrometer (CLAES), version 7 (v.7), and temperature, methane, ozone, H2O, HCl, NO and NO2 from the halogen occultation experiment (HALOE), version 18. The analysis is carried out for the UARS data obtained between January 1992 and September 1994 in the 100- to 1-mbar (approx. 17-47 km) altitude range and over 10 deg latitude bins from 70 deg S to 70 deg N. The spatiotemporal evolution of aerosol surface area density (SAD) is adopted from analysis of 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 ClONO2; (2) from the N2O-NOY correlation; and (3) from the CH4-NOY correlation. To validate our current understanding of stratospheric heterogeneous chemistry for post-Pinatubo conditions, the model-calculated monthly averaged NO(x)/NO(y) ratios and the NO, NO2, and HNO3 profiles are compared with the UARS-derived data. In general, the UARS-constrained box model captures the main features of nitrogen species partitioning in the post-Pinatubo years, such as recovery of NO(x) after the eruption, their seasonal variability and vertical profiles. However, the model underestimates the NO2 content, particularly in the 30- to 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 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 midlatitudes 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, Michael Y.↗
NASA NTRS2000

The GEOS Ozone Data Assimilation System: Specification of Error Statistics

A global three-dimensional ozone data assimilation system has been developed at the Data Assimilation Office of the NASA/Goddard Space Flight Center. The Total Ozone Mapping Spectrometer (TOMS) total ozone and the Solar Backscatter Ultraviolet (SBUV) or (SBUV/2) partial ozone profile observations are assimilated. The assimilation, into an off-line ozone transport model, is done using the global Physical-space Statistical Analysis Scheme (PSAS). This system became operational in December 1999. A detailed description of the statistical analysis scheme, and in particular, the forecast and observation error covariance models is given. A new global anisotropic horizontal forecast error correlation model accounts for a varying distribution of observations with latitude. Correlations are largest in the zonal direction in the tropics where data is sparse. Forecast error variance model is proportional to the ozone field. The forecast error covariance parameters were determined by maximum likelihood estimation. The error covariance models are validated using x squared statistics. The analyzed ozone fields in the winter 1992 are validated against independent observations from ozone sondes and HALOE. There is better than 10% agreement between mean Halogen Occultation Experiment (HALOE) and analysis fields between 70 and 0.2 hPa. The global root-mean-square (RMS) difference between TOMS observed and forecast values is less than 4%. The global RMS difference between SBUV observed and analyzed ozone between 50 and 3 hPa is less than 15%.

Stajner, Ivanka↗
NASA NTRS1997

Vertical Ozone Profile Comparisons Between Ozonesondes and Remote Instrumentation

Ozonesonde measurement quality is a critical factor for insuring measurement accuracy and is fundamentally indispensable for validating remotely measured ozone. Reasonable results from such ozone profile comparisons are best obtained by maintaining the smallest possible spatial and time differences between ozonesonde and remote measurement observations. Ozone profiles measured with the Halogen Occultation Experiment (HALOE) instrument and the Microwave Limb Sounder (MLS) instrument on NASA's Upper Atmosphere Research Satellite (UARS) are compared with ECC profiles. Comparisons with the GSFC ozone lidar also demonstrate good agreement. In this paper we show: (1) the process used by NASA to secure quality ozonesonde measurements, (2) comparisons of ozonesondes with various remote sensing instruments and, (3) the reliability obtained when both measurement types are obtained close in time and, when possible, in space.

Schmidlin, F. J.↗
NASA NTRS2000

Ionization Properties of Molecules Commonly Used for Plasma Processing of Semi-Conductors

Two types of processes are involved in plasma processing of semi-conductors. They are: plasma etching or cleaning and plasma deposition of the semi-conducting materials. For plasma etching of semi-conductors mostly halogen containing gases are used as additives to gases such as O2 and N2. For plasma deposition gases such as C2H2, SiH4, Si2H6 have been tested in the past. For an optimal performance of a reactor it is important to model the plasma. In this modeling effort electron impact excitation and ionization cross sections play a central role. For ionization balance calculations values of ionization cross sections are needed. Ion molecule reactions determine the ultimate composition of the plasma. Recently it has been discovered that the by products of many of these plasmas are per fluro hydrocarbons (PFCs) which are highly infrared absorbing species and have long life times in the atmosphere. They cause global warming. A lot of research is being pursued at the present time to find alternative molecules which do not produce global warming gases as the and product of the plasma processing reactor. There is also interest in the ionization and dissociative ionization properties of these molecules from the point view of the plasma abatement of the pollutant gases at the exhaust of the semi-conductor processing reactors. At the conference ionization and dissociative ionization properties of some of these molecules will be presented.

Srivastava, S. K.↗
NASA NTRS1996

A Comparison of Aircraft and Ground-Based Measurements at Mauna Loa Observatory, Hawaii, During GTE PEM-West and MLOPEX 2

During October 19-20, 1991, one flight of the NASA Global Tropospheric Experiment (GTE) Pacific Exploratory Mission (PEM-West A) mission was conducted near Hawaii as an intercomparison with ground-based measurements of the Mauna Loa Observatory Photochemistry Experiment (MLOPEX 2) and the NOAA Climate Modeling and Diagnostics Laboratory (CMDL). Ozone, reactive nitrogen species, peroxides, hydrocarbons, and halogenated hydrocarbons were measured by investigators aboard the DC-8 aircraft and at the ground site. Lidar cross sections of ozone revealed a complex air mass structure near the island of Hawaii which was evidenced by large variation in some trace gas mixing ratios. This variation limited the time and spatial scales for direct measurement intercomparisons. Where differences occurred between measurements in the same air masses, the intercomparison suggested that biases for some trace gases was due to different calibration scales or, in some cases, instrumental or sampling biases. Relatively large uncertainties were associated with those trace gases present in the low parts per trillion by volume range. Trace gas correlations were used to expand the scope of the intercomparison to identify consistent trends between the different data sets.

Atlas, E.↗
NASA NTRS2000

An Investigation of Polar Ozone Recovery in the 1997 Southern Hemisphere Spring

A chemical transport model is used to investigate the processes that control the depth and duration of the ozone 'hole' in the lower stratosphere through comparisons of model output with measurements from the Total Ozone Mapping Spectrometer (TOMS) and from the Microwave Limb Sounder (MLS) and Halogen Occultation Experiment (HALOE), both on the Upper Atmosphere Research Satellite (UARS). This study extends previous model comparisons with observations into October and November and examine levels in (greater than 31 hPa) and above (less than 31 hPa) the chemical loss region. Averages of column ozone in the model decrease through mid-October below 31 hPa but begin to increase in mid-September above 31 hPa. An investigation of model-tracer data comparisons and other meteorological parameters indicate that the model presents a consistent picture of top-down recovery and tracer transport. An O03budget study at 500 K (below 31 hPa) and 840 K (above 31 hPa) is carried out to investigate the processes that control the timing of the transition of ozone from a chemical to dynamically driven regime. The model ozone decrease at 500 K is due to chemical loss in August and September but is due to upward motion in October. The ozone increase at 840 K is primarily due to photochemical production, with a smaller contribution from transport. These results show that chemistry and dynamics can play different roles in polar vortex ozone recovery at different levels.

Pierson, J. M.↗
NASA NTRS2000

Satellite Measured Solar Protons from 1963-1993 and Their Influence on Ozone in a Changing Stratosphere

The fluxes of solar protons have been measured by a series of Interplanetary Monitoring Platform (IMP) satellites since 1963. Eight IMP satellites have been launched since 1963 providing excellent coverage of solar protons with energies from a few MeV to several hundred MeV. IMP 8, launched in October 1973, continues to provide proton measurements, twenty-six and a half (26 1/2) years after launch. These high energy solar protons rain down on the earth's polar atmosphere sporadically, primarily during solar proton events (SPEs) which typically last a few days. Solar protons with energies of 30 MeV or greater are capable of reaching the stratosphere and causing increases in odd nitrogen (NO(y)) constituents at polar latitudes ($>$ 60 degrees geomagnetic) which last for several months to years past the events. These enhanced NO(y) species can lead to significant upper stratospheric ozone depletions $ greater than $10\% during the gigantic SPEs that occurred in August 1972 and October 1989. We studied the effects of SPEs on the stratosphere from 1963 to the mid 1990s. During this time period, the stratospheric chlorine levels changed from relatively small in 1963 ($\sim$ 1 ppbv) to fairly substantial amounts in the mid-1990s ($\sim$ 3.3 ppbv). Our recently improved two-dimensional chemistry and transport atmospheric model was used to compute the effects of SPEs in this changing stratosphere. The long-lived SPE-produced NO(y) constituents were transported to lower stratospheric levels during winter after the events and caused impacts in the middle and lower stratosphere. Generally, the SPEs resulted in a decrease in ozone. However, during periods of high halogen loading these impacts resulted in interference with the chlorine and bromine loss cycles for ozone destruction. This interference actually led to a predicted total ozone increase that was especially notable in the time period 1992-4, a few years after the October 1989 SPE.

Jackman, Charles H.↗
NASA NTRS2000

Evaluation of Upper-Tropospheric and Lower-Stratospheric Ozone Profiles from a Global Ozone Data Assimilation System

The Data Assimilation Office at NASA's Goddard Space Flight Center provides global 3D ozone fields at six-hour time intervals. Data from Total Ozone Mapping Spectrometer (TOMS) and the Solar Backscatter Ultraviolet (SBUV) instrument are used in the assimilation. TOMS provides total column information and SBUV provides profile information, primarily above the ozone peak. Information below the ozone peak comes from the model. This paper will explore the realism of the assimilated ozone in the upper troposphere and lower stratosphere through validation with ozonesondes, Halogen Occultation Experiment (HALOE), and Polar Ozone and Aerosol Measurement (POAM) observations. This work is in preparation of using the assimilated ozone in the radiative calculation for the meteorological assimilation as well as in the derivation of tropospheric ozone.

Rood, Richard B.↗
NASA NTRS1999

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 from the cryogenic limb array etalon spectrometer (CLAES), version 7 (v.7), and temperature, methane, ozone, H2O, HCl, NO and NO2 from the halogen occultation experiment (HALOE), version 18. The analysis is carried out for the UARS data obtained between January 1992 and September 1994 in the 100-to 1-mbar (approx. 17-47 km) altitude range and over 10 degrees latitude bins from 70 S to 70 N. The spatiotemporal evolution of aerosol surface area density (SAD) is adopted from analysis of 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 ClONO2; (2) from the N2O-NOy correlation, and (3) from the CH4-NOy correlation. To validate our current understanding of stratospheric heterogeneous chemistry for post-Pinatubo conditions, the model-calculated monthly averaged NOx/NOy ratios and the NO, NO2, and HNO3 profiles are compared with the UARS-derived data. In general, the UARS-constrained box model captures the main features of nitrogen species partitioning in the post-Pinatubo years, such as recovery of NOx after the eruption, their seasonal variability and vertical profiles. However, the model underestimates the NO2 content, particularly in the 30- to 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 45 S and 45 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 midlatitudes in both hemispheres. Reasonable agreement is obtained for HNO3 columns at 45 S, suggesting some problems with nitrogen species partitioning in the model. Outstanding uncertainties are discussed.

Danilin, Michael Y.↗
NASA NTRS2001

Properties of Stratospheric Aerosol Estimated from HALOE Data

Extinction coefficients for stratospheric aerosols at 8 HALOE (HALogen Occultation Experiment) wavelengths are determined by comparing transmittances data for two adjacent solar occultation measurements, where one limb path is loaded with aerosols but the other path is free of aerosols. These extinction coefficients are used to infer the aerosol properties such as composition and size distribution parameters. Mie theory has been used to calculate the extinction coefficients, and a nonlinear least square method is applied to determine the aerosol properties. Sixteen cases are selected for the retrieval in southern hemisphere at latitudes from 21 to 48 deg S for the period of 29 Mar - 31 May 1992. Retrieved size width ranges from 1.1 to 1.5 and radius ranges from 0.25 to 0.45 micrometers. These size parameters are within the ranges of in situ measurements at Laramie, Wyoming. Retrieved weight percent of H2SO4 is larger than the equilibrium value by about 5 to approximately 10 weight percent, similar to the results for northern hemisphere at latitudes 20 to 55 deg N for the period from Nov 1991 to Feb. 1992.

Lee, Kwang-Mog↗
NASA NTRS2001

High Resolution Chemical Study of ALH84001

We have studied the chemistry of a sample of the SNC meteorite ALH84001 using an environmental scanning electron microscope (ESEM) with an energy dispersive chemical analytical detector and a focused ion beam secondary ion mass spectrometer (FIB-SIMS). Here we present the chemical data, both spectra and images, from two techniques that do not require sample preparation with a conductive coating, thus eliminating the possibility of preparation-induced textural artifacts. The FIB-SIMS instrument includes a column optimized for SEM with a quadrupole type mass spectrometer. Its spatial and spectral resolution are 20 nm and 0.4 AMU, respectively. The spatial resolution of the ESEM for chemical analysis is about 100 nm. Limits of detection for both instruments are mass dependent. Both the ESEM and the FIB-SIMS instrument revealed contrasting surficial features; crumbled, weathered appearance of the matrix in some regions as well as a rather ubiquitous presence of euhedral halite crystals, often associated with cracks or holes in the surface of the rock. Other halogen elements present in the vicinity of the NaCl crystals include K and Br. In this report, elemental inventories are shown as mass spectra and as X-ray maps.

Conrad, Pamela G.↗
NASA NTRS2001

HALOE Algorithm Improvements for Upper Tropospheric Sounding

This report details the ongoing efforts by GATS, Inc., in conjunction with Hampton University and University of Wyoming, in NASA's Mission to Planet Earth Upper Atmospheric Research Satellite (UARS) Science Investigator Program entitled 'HALOE Algorithm Improvements for Upper Tropospheric Sounding.' The goal of this effort is to develop and implement major inversion and processing improvements that will extend Halogen Occultation Experiment (HALOE) measurements further into the troposphere. In particular, O3, H2O, and CH4 retrievals may be extended into the middle troposphere, and NO, HCl and possibly HF into the upper troposphere. Key areas of research being carried out to accomplish this include: pointing/tracking analysis; cloud identification and modeling; simultaneous multichannel retrieval capability; forward model improvements; high vertical-resolution gas filter channel retrievals; a refined temperature retrieval; robust error analyses; long-term trend reliability studies; and data validation. The current (first year) effort concentrates on the pointer/tracker correction algorithms, cloud filtering and validation, and multichannel retrieval development. However, these areas are all highly coupled, so progress in one area benefits from and sometimes depends on work in others.

Thompson, Robert Earl↗
NASA NTRS2001

Two-Step Calibration of a Multiwavelength Pyrometer for High Temperature Measurement Using a Quartz Lamp

There is no theoretical upper temperature limit for pyrometer application in temperature measurements. NASA Glenn's multiwavelength pyrometer can make measurements over wide temperature ranges. However, the radiation spectral response of the pyrometer's detector must be calibrated before any temperature measurement is attempted, and it is recommended that calibration be done at temperatures close to those for which measurements will be made. Calibration is a determination of the constants of proportionality at all wavelengths between the detector's output (voltage) and its input signals (usually from a blackbody radiation source) in order to convert detector output into radiation intensity. To measure high temperatures, the detectors are chosen to be sensitive in the spectral range from 0.4 to 2.5 micrometers. A blackbody furnace equilibrated at around 1000 C is often used for this calibration. Though the detector may respond sensitively to short wavelengths radiation, a blackbody furnace at 1000 C emits only feebly at very short wavelengths. As a consequence, the calibration constants that result may not be the most accurate. For pyrometry calibration, a radiation source emitting strongly at the short wavelengths is preferred. We have chosen a quartz halogen lamp for this purpose.

Ng, Daniel↗
NASA NTRS2001

Sources of Variability in the Stratospheric Column of Nitrogen Dioxide

Instruments such as the Global Ozone Monitoring Experiment (GOME, on the European Remote Sensing Satellite (ERS-2), launched 1995), the Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY, on ENVISAT, to be launched July 2001) and the Ozone Monitoring Instrument (OMI on EOS Aura, to be launched 2003) make measurements of the total column of NO2. There is interest in separating the stratospheric and tropospheric contributions to the column, as the tropospheric column provides a measure of pollution. We are using a 3D chemistry and transport model driven by winds from the Goddard Space Flight Center Data Assimilation System to examine variability in the stratospheric NO2 column. Model results for NOx = NO + NO2 + 2N2O5 will be shown to compare well with sunset observations from the Halogen Occultation Experiment on the Upper Atmosphere Research Satellite, and to exhibit similar temporal and spatial dependence. Partitioning between NO, NO2, and N2O5 is also shown to compare well with observations. This good agreement supports the use of simulated fields in the stratosphere to derive the tropospheric column from the total column. Preliminary comparisons of the tropospheric column with model simulations for the troposphere will also be shown.

Douglass, Anne↗
NASA NTRS2001

Data Comparison: Satellite and Falling Sphere Temperatures

Small meteorological rocketsondes providing temperature data have beam used for comparison with, and validation of measurements from satellite-borne instruments. A significant number of rocket-borne falling spheres were launched in conjunction with the Upper Atmosphere Research Satellite (UARS) for validation of the Halogen Occultation Experiment (HALOE), High Resolution Doppler Interferometer (HRDI), and the Microwave Limb Sounder (MLS) instruments. Upper stratosphere and mesosphere temperatures measured with these instruments on UARS are compared with inflatable spheres launched from Wallops Island (1992-1999), Brazil (1994), Hawaii (1992), Norway (1992), and Sweden (1993 and 1996). Time and space differences varied between the satellite measurement and the rocketsonde launch, for example HALOE overpasses occurred within 5 days and in some cases there were spatial differences of up to 30 degrees longitude. Validation measurements of the HRDI instrument occurred at Wallops Island when it passed within 20 minutes and 330 kilometers of the launch site. Because of discontinuity in the falling sphere drag coefficients when fall speed neared MACH 1 falling sphere temperatures near 70 kilometers attitude are biased toward lower temperatures. Availability of improved software and a new atmospheric model have helped to reduce this bias. The validated remote instrument measurements permit a new perspective of atmospheric structure to be formed, not always possible with the limited number of falling sphere measurements. Features of the remote measurement temperature profiles and their possible use to extend the climatological data base at the rocketsonde sites will be discussed.

Schmidlin, Francis J.↗
NASA NTRS1995

Ab Initio Studies of Stratospheric Ozone Depletion Chemistry

An overview of the current understanding of ozone depletion chemistry, particularly with regards the formation of the so-called Antarctic ozone hole, will be presented together with an outline as to how ab initio quantum chemistry can be used to further our understanding of stratospheric chemistry. The ability of modern state-of-the art ab initio quantum chemical techniques to characterize reliably the gas-phase molecular structure, vibrational spectrum, electronic spectrum, and thermal stability of fluorine, chlorine, bromine and nitrogen oxide species will be demonstrated by presentation of some example studies. The ab initio results will be shown to be in excellent agreement with the available experimental data, and where the experimental data are either not known or are inconclusive, the theoretical results are shown to fill in the gaps and to resolve experimental controversies. In addition, ab initio studies in which the electronic spectra and the characterization of excited electronic states of halogen oxide species will also be presented. Again where available, the ab initio results are compared to experimental observations, and are used to aid in the interpretation of experimental studies.

Lee, Timothy J.↗
NASA NTRS2002

Evaluation of SAGE II and Balloon-Borne Stratospheric Aerosol Measurements: Evaluation of Aerosol Measurements from SAGE II, HALOE, and Balloonborne Optical Particle Counters

Stratospheric aerosol measurements from the University of Wyoming balloonborne optical particle counters (OPCs), the Stratospheric Aerosol and Gas Experiment (SAGE) II, and the Halogen Occultation Experiment (HALOE) were compared in the period 1982-2000, when measurements were available. The OPCs measure aerosol size distributions, and HALOE multiwavelength (2.45-5.26 micrometers) extinction measurements can be used to retrieve aerosol size distributions. Aerosol extinctions at the SAGE II wavelengths (0.386-1.02 micrometers) were computed from these size distributions and compared to SAGE II measurements. In addition, surface areas derived from all three experiments were compared. While the overall impression from these results is encouraging, the agreement can change with latitude, altitude, time, and parameter. In the broadest sense, these comparisons fall into two categories: high aerosol loading (volcanic periods) and low aerosol loading (background periods and altitudes above 25 km). When the aerosol amount was low, SAGE II and HALOE extinctions were higher than the OPC estimates, while the SAGE II surface areas were lower than HALOE and the OPCS. Under high loading conditions all three instruments mutually agree to within 50%.

Hervig, Mark↗