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All sourcesNASA NTRSDOE OSTI
NASA NTRS1999

History of Ozone Research: From Schonbein to the Present

In 1840, C.F. Schonbein recognized that the smell generated in several different electrical and chemical processes was a single substance. He named this substance "ozein" from the Greek for "to smell". This substance we know today as ozone. Several periods can be distinguished in the continued development of our understanding of ozone. Throughout the late 19th century, the identity and properties of ozone were established and described. Ozone was recognized to be a constituent of normal air and tests were established to measure its concentration. Its disinfectant properties were recognized. New methods were developed for making ozone in the laboratory. In 1879, ultraviolet spectroscopic techniques were applied to the measurement of the solar spectrum and it was discovered by Comu that the spectrum was cut off at about 300 nm wavelength. Hartley suggested, based on laboratory measurements, that this cutoff was due to ozone in the atmosphere which he correctly asserted was somewhere in the upper atmosphere. This began the period of development of the amount and distribution of ozone throughout the atmosphere. In 1930, Chapman put forward the first theory of the formation and destruction of ozone. By the mid-1960s it was becoming obvious that the description of the chemical loss term was inadequate. By the early 1970s the chemical destruction of ozone by the oxides of hydrogen, nitrogen, chlorine, and bromine was recognized as an essential element in the chemical balance determining the ozone concentration. Today, ozone is a broad research project which crosses the boundaries of traditional disciplines. Stratospheric ozone loss due to chlorofluorocarbons is a newsworthy item. The Antarctic ozone hole opens up every spring. The provisions of the Montreal Protocol were agreed upon by countries around the world and promise to reduce the future levels of ozone-destroying chlorine in the stratosphere. Ozone concentrations in polluted cities are a subject of local and national regulations to limit its potential for causing health problems and corrosive effects on materials. A lot is known about ozone but many new questions are still being developed.

Stolarski, Richard S.↗
NASA NTRS1980

The vertical distribution of tropospheric ammonia

A one-dimensional tropospheric photochemical model is used to simulate measured profiles of NH3 obtained with the Infrared Heterodyne Radiometer. The relative roles of homogeneous loss, heterogeneous loss, and vertical eddy transport are discussed in terms of selecting parameters which best fit the measurements. The best fit was obtained for a vertical eddy diffusion coefficient of 200,000/sq cm per sec or greater (corresponding to a characteristic vertical transport time in excess of about 35 days), and a characteristic heterogeneous loss time in excess of 10 days. The characteristic homogeneous chemical loss time was found to be about 40 days at the surface and decreased to about 180 days at 10 km, and not very sensitive to model chemical perturbations. Increased ground-level concentrations of NH3 to about 10 ppb, compared to background surface concentrations of about 1 ppb, were measured several weeks after application of ammonium nitrate fertilizer. This suggests that the volatilization of ammonium nitrate fertilizer is rapid, and an important source of NH3. Because of the characteristic times for the loss mechanisms, synoptic time-scale phenomena may play an important role in determining the tropospheric distribution of NH3 concentrations.

Levine, J. S.↗
NASA NTRS1991

Effects of high pressure nitrogen on the thermal stability of SiC fibers

Polymer-derived SiC fibers were exposed to nitrogen gas pressures of 7 and 50 atm at temperatures up to 1800 C. The fiber weight loss, chemical composition, and tensile strength were then measured at room temperature in order to understand the effects of nitrogen exposure on fiber stability. High pressure nitrogen treatments limited weight loss to 3 percent or less for temperatures up to 1800 C. The bulk Si-C-O chemical composition of the fiber remained relatively constant up to 1800 C with only a slight increase in nitrogen content after treatment at 50 atm; however, fiber strength retention was significantly improved. To further understand the effects of the nitrogen atmosphere on the fiber stability, the results of previous high pressure argon treatments were compared to those of the high pressure nitrogen treatments. High pressure inert gas can temporarily maintain fiber strength by physically inhibiting the evolution of gaseous species which result from internal reactions. In addition to this physical effect, it would appear that high pressure nitrogen further improved fiber temperature capability by chemically reacting with the fiber surface, thereby reducing the rate of gas evolution. Subsequent low pressure argon treatments following the initial nitrogen treatments resulted in stronger fibers than after argon treatment alone, further supporting the chemical reaction mechanism and its beneficial effects on fiber strength.

Jaskowiak, Martha H.↗
NASA NTRS1997

A Three-Wave Model of the Stratosphere with Coupled Dynamics, Radiation and Photochemistry

A zonal mean chemistry transport model (2-D CTM) coupled with a semi-spectral dynamical model is used to simulate the distributions of trace gases in the present day atmosphere. The zonal-mean and eddy equations for the velocity and the geopotential height are solved in the semi-spectral dynamical model. The residual mean circulation is derived from these dynamical variables and used to advect the chemical species in the 2- D CTM. Based on a linearized wave transport equation, the eddy diffusion coefficients for chemical tracers are expressed in terms of the amplitude, frequency and growth rate of dynamical waves; local chemical loss rates; and a time constant parameterizing small scale mixing. The contributions to eddy flux are from the time varying wave amplitude (transient eddy), chemical reactions (chemical eddy) and small scale mixing. In spite of the high truncation in the dynamical module (only three longest waves are resolved), the model has simulated many observed characteristics of stratospheric dynamics and distribution of chemical species including ozone. Compared with the values commonly used in 2-D CTMs, the eddy diffusion coefficients for chemical species calculated in this model are smaller, especially in the subtropics. It is also found that the chemical eddy diffusion has only a small effects in determining the distribution of most slow species, including ozone in the stratosphere.

Shia, Run-Lie↗
NASA NTRS2001

The Impact of Increasing Carbon Dioxide on Ozone Recovery

We have used the GSFC coupled two-dimensional (2D) model to study the impact of increasing carbon dioxide from 1980 to 2050 on the recovery of ozone to its pre-1980 amounts. We find that the changes in temperature and circulation arising from increasing CO2 affect ozone recovery in a manner which varies greatly with latitude, altitude, and time of year. Middle and upper stratospheric ozone recovers faster at all latitudes due to a slowing of the ozone catalytic loss cycles. In the lower stratosphere, the recovery of tropical ozone is delayed due to a decrease in production and a speed up in the overturning circulation. The recovery of high northern latitude lower stratospheric ozone is delayed in spring and summer due to an increase in springtime heterogeneous chemical loss, and is speeded up in fall and winter due to increased downwelling. The net effect on the higher northern latitude column ozone is to slow down the recovery from late March to late July, while making it faster at other times. In the high southern latitudes, the impact of CO2 cooling is negligible. Annual mean column ozone is predicted to recover faster at all latitudes, and globally averaged ozone is predicted to recover approximately ten years faster as a result of increasing CO2.

Rosenfield, Joan E.↗
NASA NTRSDate not supplied

Regional and Seasonal Trends in Tropical Ozone from SHADOZ Profiles: Reference for Models and Satellite Products

Understanding lowermost stratosphere (LMS) ozone variability is an important topic in the trends and climate assessment communities because of feedbacks among changing temperature, dynamics, water vapor and ozone. LMS evaluations are usually based on satellite observations. Free tropospheric (FT) ozone assessments typically rely on profiles from commercial aircraft. Ozonesonde measurements constitute an independent dataset encompassing both LMS and FT. We used Southern Hemisphere Additional Ozonesondes (SHADOZ) data from 1998-2019 in the GSFC Multiple Linear Regression (MLR) model to analyze monthly mean FT and LMS ozone across five well-distributed tropical sites, three based on combination of nearby individual stations (Figure 1). Our findings: (1) both FT (defined as 5-15 km) and LMS (15-20 km) ozone trends exhibit marked regional and seasonal variability. (2) Stations with the largest FT ozone increases, in the equatorial Americas and western Pacific/east Indian Ocean, show these trends most strongly in February-May when there is convectively-driven wave activity. (3) LMS ozone losses are greatest in the 2nd half of the year (solid lines in Figure 2) when the losses are correlated with an increase in tropopause height (TH) as derived from SHADOZ radiosonde data. ( 4) When the upper FT and LMS are defined by tropopause-relative coordinates, the LMS ozone trend calculated by MLR becomes insignificant, as shown in the dashed lines in Figure 2. Thus, the 20-year decline in tropical LMS ozone reported in recent satellite- and model-based studies does not point to a chemical loss but is rather a signature of a tropopause that has been perturbed by a changing climate. Output based on our regional and monthly averaged FT and LMS ozone trends will be available as a reference for satellite- and model-based analyses.

Free Tropospheric (FT) ozone assessments↗
NASA NTRS1996

Decadal evolution of the Antarctic ozone hole

Ozone column amounts obtained by the total ozone mapping spectrometer (TOMS) in the southern polar region are analyzed during late austral winter and spring (days 240-300) for 1980-1991 using area-mapping techniques and area-weighted vortex averages. The vortex here is defined using the -50 PVU (1 PVU = 1.0 x 10(-6) K kg-1 m2 s-1) contour on the 500 K isentropic surface. The principal results are: (1) there is a distinct change after 1985 in the vortex-averaged column ozone depletion rate during September and October, the period of maximum ozone loss, and (2) the vortex-averaged column ozone in late August (day 240) has dropped by 70 Dobson units (DU) in a decade due to the loss in the dark and the dilution effect. The mean ozone depletion rate in the vortex between day 240 and the day of minimum vortex-averaged ozone is about 1 DU d-1 at the beginning of the decade, increasing to about 1.8 DU d-1 by 1985, and then apparently saturating thereafter. The vortex-average column ozone during September and October has declined at the rate of 11.3 DU yr-1 (3.8%) from 1980 to 1987 (90 DU over 8 years) and at a smaller rate of 2 DU yr-1 (0.9%) from 1987 to 1991 (10 DU over 5 years, excluding the anomalous year 1988). We interpret the year-to-year trend in the ozone depletion rate during the earlier part of the decade as due to the rise of anthropogenic chlorine in the atmosphere. The slower trend at the end of the decade indicates saturation of ozone depletion in the vortex interior, in that chlorine amounts in the mid-1980s were already sufficiently high to deplete most of the ozone in air within the isolated regions of the lower-stratospheric polar vortex. In subsequent years, increases in stratospheric chlorine may have enhanced wintertime chemical loss of ozone in the south polar vortex even before major losses during the Antarctic spring.

Non-NASA Center↗
NASA NTRS1978

Artificially created holes in the ionosphere

The artificial creation of ionospheric holes by the release of highly reactive molecules into the F region is investigated. Through ion-atom interchange or charge transfer reactions, H2 or H2O reacts with O(+) to form OH(+) or H2O(+), respectively, which subsequently dissociatively recombines with electrons at a very rapid rate. The diffusion of H2 is also modified by chemical loss to the ambient atomic oxygen atmosphere. The limited spatial and temporal extent of the hole-making process allows several approximations to be made which permit three-dimensional analytic solutions of the continuity equations for the released particles, the O(+) and e(-) densities, and the intermediary molecular ions. A versatile formalism is developed whereby the hole-making capability of virtually any spatial-temporal configuration of released particles can be determined by convolving a set of destruction operators which can be viewed as Green's functions for the problem. As a specific application of the techniques developed, the modification of a winter nighttime ionosphere is described by simulating the release of 1000 kg of water vapor near a height of 300 km.

Mendillo, M.↗
NASA NTRS1979

The behavior of tropical ozone during the stratospheric warming of March-April 1976

The backscatter ultraviolet spectrometer on the Atmosphere Explorer-E satellite obtained ozone data for the upper stratosphere and lower mesosphere from an equatorial orbit near the time of the March-April 1976 stratospheric warming. A simple inversion technique allows the extraction of information on the absolute ozone abundance and its longitudinal variation from the measured radiances. Between altitudes of 35 and 60 km tropical O3 in constant pressure layers exhibits increased spatial variations on length scales of 20 to 30 deg in longitude after the onset of the polar warming, indicating enhanced wave activity. One week after the polar vortex breakdown, upper stratospheric O3 begins a relaxation toward the unperturbed state, while that in the lower mesosphere continues to show maximum variations near + or 10% of the longitudinally averaged value. Although the degree of horizontal structure increases during the warming, the absolute O3 amounts averaged over longitude between 35 and 60 km in altitude remain nearly constant in time. The observed behavior is consistent with that expected from enhanced vertical transport of O3 in the tropics with accompanying adiabatic temperature changes which alter the chemical loss rate.

Frederick, J. E.↗
NASA NTRS1984

Wet model of Saturn's ionosphere: Water from the rings

Current theoretical models of Saturn's ionosphere are difficult to reconcile with the ionospheric electron density profiles obtained from the Pioneer and Voyager radio occultation observations and the large diurnal variation of maximum ionospheric electron density deduced from studies of Saturn lightning discharges. A model of Saturn's ionosphere is proposed in which water plays a major role as a minor constituent present by virtue of downward diffusion from an external source. This model of the Saturn ionosphere is a classical 'F2' type layer resulting from the photodissociative production of H(+) from H2 and rapid chemical loss due to a series of charge exchange reactions with water. A planet-wide influx of about 4x10 to the 7th power molecules/sec/sq cm of water from the rings is consistent with the observed ionospheric electron densities and estimates of influx due to micrometeoride bombardment of the rings. An enhanced influx of water occurs at latitudes (-38 deg, +44 deg) magnetically connected to the inner edge of Saturn's B ring which results from an electromagnetic erosion process contributing substantially to the (local) upper atmosphere water content. Present day influx at these latitudes is possibly as large as 2x10 to the 9th power molecules/sec/sq cm.

Connerney, J. E. P.↗
NASA NTRS1984

New model of Saturn's ionosphere with an influx of water from the rings

A radically different model of Saturn's ionosphere is proposed in which water plays a major role as a minor constituent present by downward diffusion from an external source. The model ionosphere is a classical F2 type layer resulting from the photodissociative production of H(+) from H2 and rapid chemical loss by a series of charge exchange reactions with water. A planet-wide influx of about 4 x 10 to the 7th molecules/sq cm/s of water from the rings is consistent with the observed ionospheric electron densities. An enhanced influx of water occurs at latitudes (-38, +44 deg) connected magnetically at the inner edge of Saturn's B ring, where an electromagnetic erosion process takes place. The present-day influx at these latitudes may be as large as 2 x 10 to the 9th molecules/sq cm/s.

Connerney, J. E. P.↗
NASA NTRS1985

Middle atmosphere modeling

Breaking gravity waves generate and maintain a background level of turbulence which is capable of producing substantial cooling and/or heating in the upper mesosphere and lower thermosphere. The net thermodynamic effect of breaking gravity waves is critically dependent on the eddy Prandt number (P sub t) applicable to mesospheric turbulence. When P sub t is approximately 1, the calculations of the heat budget for the mesopause region imply that the globally averaged eddy or turbulent diffusion coefficient cannot exceed .000001 sq cm/s. This upper limit on turbulant diffusion applies to both potential temperature transport and chemically inert tracer transport when radiative damping is neglible. For chemically active species larger diffusion coefficients are permitted, because the effective eddy diffusion coefficient is increased by an additive term L/2 gamma (sup 2), where L is the chemical loss rate and gamma is the vertical wavenumber. For P sub t is approximately 4 to 6, the turbulent diffusion of momentum (D sub M) is sufficiently greater than the turbulent diffusion of heat (D sub H) that the conversion of gravity wave energy to heat with high efficiency nearly balances the divergence of the downward eddy heat flux in the wave breaking zone. Therefore the heat budget of the mesopause region would no longer provide a powerful and useful constraint on D sub H. If P sub t exceeds 6 with high efficiency for energy conversion to heat, gravity waves would heat the mesosphere throughout the wave breaking region.

Strobel, D. F.↗
NASA NTRS1986

Tracer transport by the diabatic circulation deduced from satellite observations

Nimbus-7 sensor data were used to track the diabatic circulation in the stratosphere to study the advective transport of CH4 and N2O as tracer species. Advective transport by the mean circulation was found to be a function of the temperature field and associated deviations from radiative equilibrium. A photochemical model was applied to account for the disappearance of the tracer species from the stratosphere. Comparisons between the SAMS data and modeling on the basis of the chemical loss rates of the tracers and the LIMS circulation data showed that the model predictions underestimated the resident abundances, although the global distributions and circulations exhibited a good match.

Solomon, S.↗
NASA NTRS1987

Current review of the Jupiter, Saturn, and Uranus ionospheres

The ionospheres of the major planets Jupiter, Saturn, and Uranus are reviewed in light of Pioneer and Voyager observations. Some refinements to pre-Voyager theoretical models are required to explain the results, most notably the addition of significant particle ionization from 'electroglow' and auroral processes and the need for additional chemical loss of protons via charge exchange reactions with water. Water from the Saturn rings has been identified as a major modifier of the Saturn ionosphere and water influx from satellites and/or meteorites may also be important at Jupiter and Uranus as well, as evidenced by the observed ionospheric structure and the identification of cold stratospheric carbon monoxide at Jupiter.

Waite, J. H., Jr.↗
NASA NTRS1988

Interactions between HCl, NO(x), and H2O ice in the Antarctic stratosphere - Implications for ozone

The role of PSC particles in determining the distributions of HCl and chlorine radicals is studied. The thermodynamics of HCl in ice is discussed, showing that significant quantities of HCl may be dissolved in ice when PSCs form. It is argued that HCl and HNO3 will be removed from the gas phase early in the condensation process, when only small quantities of H2O have been condensed, reflecting the thermodynamic properties of the solid phases of HCl, HNO3, and H2O. Rapid heterogeneous chemical reactions then volatilize reactive chlorine gases and convert NO(x) to solid-phase nitrates, which can be removed by gravitational settling. Analysis of the suite of heterogeneous chemical processes in the polar stratosphere implies a threshold for HCl concentrations, above which chemical loss rates for ozone increase dramatically.

Wofsy, S. C.↗
NASA NTRS1990

Distributions of He(+) at middle and equatorial latitudes during solar maximum

The properties of the plasma composition in the topside ionosphere between 15 and 35 deg magnetic latitude are examined. Calculations are used to show that the distribution of neutral species at solar maximum, together with the appropriate ionization rates, can readily account for the dominance of He(+) at midlatitudes. The relative abundance of the atmospheric species is a sensitive function of local time and the associated evolution of the topside O(+) concentration profile. The existence of an ExB drift motion of the plasma is needed to explain the He(+) minimum at the dip equator. While the He(+) concentration there is produced in one day against the chemical loss process, at midlatitudes a large flux tube volume provides a reservoir in which the He(+) can accumulate each day.

Heelis, R. A.↗