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Lectures covering a broad spectrum of current research in tropospheric chemistry with particular emphasis on the interaction of measurements, modeling, and understanding of fundamental processes are presented.
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The latitudinal and seasonal variation of ozone in the troposphere is discussed. Of particular interest is the asymmetrical behavior of this gas with respect to the two hemispheres. These asymmetries, when coupled with a diagnostic photochemical model of the troposphere, lends support to the view that ozone cannot be viewed as an inert tracer of stratospheric origin. In the calculations it is noted that it is likely that the budgets of carbon monoxide and tropospheric ozone may be quite dependent on each other and the calculations are discussed in light of the uncertainty which currently exists about representative global tropospheric background concentrations of the nitrogen oxides. In addition, the seasonal variation of excess (C-14)O2 (a stratospheric tracer) is examined and compared with the seasonal ozone variation during the same period of observations at the same location and altitudes. The distinct maxima for ozone found during the summer in the lower troposphere are not present for the (C-14)O2 data. This finding likewise suggests that photochemical processes taking place in the troposphere are an important source term for tropospheric ozone.
Papers are presented which originate from a conference on 'The Non-Urban Troposphere Composition', held in 1976. Attention is given to distributions of nitrous oxide in the atmosphere, and to tropospheric and stratospheric compositions which are perturbed by NO(x) emissions from high-altitude aircraft. Ozone is studied in terms of in situ measurements; various meteorological analyses of tropopause folding, ozone measurements in the Boston area, and ozone measurements in rural areas are presented. A one-dimensional model used to study tropospheric photochemistry numerically is presented as are vertical profiles of tropospheric and stratospheric molecular hydrogen. The oxidation of ammonia, methane, and hydrogen sulfide is assessed in nonurban tropospheres along with nonurban measurements of ethane and methane for various atmospheric conditions. With reference to the particle size distribution of chloride in the marine aerosol, organic and inorganic chlorine concentrations are evaluated, and measurements of sea-air CO2 flux by eddy correlation are investigated.
Detailed wet tropospheric fluctuation information is presented in support of proposals to search for gravitational waves in ultra-precise Doppler data. The similarities between the solar wind and tropospheric effects on apparent signal path length are used to hypothesize a parametric model for low-frequency wet tropospheric path length fluctuation. Experimental observations of wet tropospheric signal delay fluctuations are interpreted as confirmation of this parametric form. The model is used to suggest the appropriate conditions for collection of experimental tropospheric fluctuation data.
Vertical profiles of CO and O3 in the troposphere and lower stratosphere have been constructed during a series of flights conducted in July and August 1974 over the American continents between 53 deg S and 67 deg N. The mixing ratios of both gases show large fluctuations with altitude in the Northern Hemisphere. Most of the observed bands of O3 in the free troposphere are coexistent with elevated CO concentrations indicating that this O3 is probably not of stratospheric origin, but most likely produced in the troposphere. From the observations, it is not clear whether these high concentrations of ozone were produced in situ in the remote troposphere or had been transported out of a polluted boundary layer. Isentropic trajectory calculations likewise indicate that the air containing these elevated ozone and carbon monoxide concentrations had been situated in the troposphere for at least 72 h prior to being sampled.
A detailed study of the photochemistry of iodine and its oxides indicates that iodine species may play an important role in the tropospheric photochemical system. Methyl iodide, often observed in the marine troposphere with an average concentration of 5-10 ppt, is photolyzed and thereby produces I atoms. Chemical interactions with O3, HxOy, and NOx cause I to be converted to other inorganic compounds such as IO, HOI, IONO2, and I2. The production of these species and their subsequent recycling back to I can lead to the catalytic removal of tropospheric O3, the enhancement of the NO2/NO ratio, the destruction of HxOy free radicals, and the conversion of HO2 to OH. Ultimately, tropospheric inorganic iodine is removed by heterogeneous processes. Calculations using a numerical model to simulate tropospheric photochemistry indicate that iodine may have a strong impact upon the atmospheric O3-NOx-HxOy system. The magnitude of these effects is dependent upon the value of several uncertain rate constants and the primary source distributions of CH3I and other organic and inorganic iodine compounds.
The budget of tropospheric ozone is re-examined in the light of lower observed nitrogen oxide densities and revised reaction rates. To estimate the relative importance of transport and photochemistry, model calculations are presented which determine one-dimensional vertical ozone profiles at midlatitudes for equinoctial conditions. These calculations imply that both photochemistry and transport are important in controlling the abundance of tropospheric ozone. It is estimated that photochemical processes produce about 0.6 times 10 to the eleventh and destroy about 1.4 times 10 to the eleventh tropospheric ozone molecules per sq cm per sec, while mixing processes transport about 1.4 times 10 to the eleventh ozone molecules per sq cm per sec from the stratosphere into the troposphere and ground level fluxes destroy about 0.6 times 10 to the eleventh ozone molecules per sq cm per sec. The sensitivity of our model calculations to transport parameters, key rate coefficients, and nitrogen oxide densities are discussed.
Examination of the distribution of tropospheric ozone indicates that surface destruction in the Northern Hemisphere (NH) should be about three times larger than in the Southern Hemisphere (SH). If, according to the traditional understanding of ozone, this species were a passive tracer in the troposphere, a threefold larger flux out of the stratosphere should exist in the NH than in the SH. However, meteorological analyses fail to support such pronounced hemispheric differences in stratosphere-troposphere exchange. Alternatively, therefore, it is hypothesized that photochemical synthesis of ozone in the troposphere may be particularly important in the NH because of asymmetries in the sources and distribution of carbon monoxide, hydrocarbons and nitric oxide.
The possibility of planetary wave coupling between the troposphere and solar-induced alterations in the upper atmosphere providing a viable mechanism for giving rise to sun-weather relationships is investigated. Some of the observational evidence for solar-activity-induced effects on levels of the upper atmosphere ranging from the thermosphere down to the lower stratosphere are reviewed. It is concluded that there is evidence for such effects extending down to the middle stratosphere and below. Evidence is also reviewed that these effects are due to changes in solar ultraviolet emission during disturbed solar conditions. A theoretical planetary wave model is then used to see at what levels in the upper atmosphere moderate changes in the mean zonal wind state would result in tropospheric changes. It is concluded that changes in the mean zonal flow of about 20% at levels in the vicinity of 35 km or below would give rise to changes in the tropospheric planetary wave pattern that are less than but on the same order as the observed interannual variability in the tropospheric wave pattern at middle and high latitudes.
The existence of tropospheric-stratospheric feedback mechanisms affecting variations in stratospheric ozone indicates the need to model the complete tropospheric-stratospheric system. For instance, a decrease in stratospheric ozone results in increased photolytic destruction of nitrous oxide in the troposphere and thereby reduced production of nitric oxide in the stratosphere. Estimates indicate that this mechanism will result in a recovery in atmospheric ozone of about 6 to 13 percent of the initial perturbation.
The effects of tropospheric and ionospheric refraction errors are analyzed for the GEOS-C altimeter project in terms of their resultant effects on C-band orbits and the altimeter measurement itself. Operational procedures using surface meteorological measurements at ground stations and monthly means for ocean surface conditions are assumed, with no corrections made for ionospheric effects. Effects on the orbit height due to tropospheric errors are approximately 15 cm for single pass short arcs (such as for calibration) and 10 cm for global orbits of one revolution. Orbit height errors due to neglect of the ionosphere have an amplitude of approximately 40 cm when the orbits are determined from C-band range data with predominantly daylight tracking. Altimeter measurement errors are approximately 10 cm due to residual tropospheric refraction correction errors. Ionospheric effects on the altimeter range measurement are also on the order of 10 cm during the GEOS-C launch and early operation period.
An investigation was conducted of the spatial and temporal relationships existing between the radiometrically observed water vapor patterns in cloud free areas and the conventionally derived water vapor patterns. The upper and middle tropospheric water vapor budget and the associated dynamics were examined to obtain a basis for a more definite evaluation of the significance of the Nimbus 4 radiometric 6.7-micrometer observations for the study of tropospheric dynamics in cloud free areas. A large-amplitude trough situated to the lee of the Rocky Mountains over the central U.S. between April 30 and May 1, 1970, was selected for the investigation because it best illustrated large upper tropospheric dynamic variations.
The mechanisms by which phenomena occurring in the troposphere can affect that atmospheric region lying above the tropopause and below the mesopause are discussed as well as mechanisms by which middle atmospheric phenomena affect the tropospheric circulation, and how the middle atmosphere may act as a medium by which extraterrestrial effects may give rise to changes in tropospheric circulation. Energetics and external energy sources are considered. Aspects of vertical coupling examined include upward, downward, radiational, chemical, and electrical modes.
The effect of tropospheric fluctuation on the accuracy of phase measurements of coordinates is discussed. The nature of the averaging of the tropospheric effects, if N coordinate measurements of duration T with period mu are made, is investigated. Various averaging modes depending on the relation of the various time parameters are investigated. Equations taking into account the correlations between individual observations are presented. It is shown that the correlation interval between the individual observations is always greater than the fluctuation period of tropospheric inhomogeneities typical for a given baseline.
A preliminary analysis of zonally averaged, ozone concentration data obtained from commercial (GASP) aircraft between the equator and 60 deg North indicates that ozone in the upper troposphere exhibits a primary maximum during the spring, and, in middle latitudes, a secondary maximum in the summer of both 1975 and 1976. A late-fall/early-winter minimum also appears and seems consistent with previous upper air measurements. The April ozone maximum has been well documented and appears at the time when the stratospheric ozone content is greatest and cyclogenetic activity is most vigorous. However, the secondary maximum in June has not been widely observed or quoted as a unique feature. It is hypothesized that the rapid ascent of the tropopause between midspring and summer could account for the incorporation of ozone-rich, stratospheric air into the upper troposphere with a subsequent dilution during the following months. This may explain certain aspects of the annual ozone cycle in the lower troposphere which occasionally exhibit a bimodal distribution during the warm season.
A microprocessor controlled lidar system under construction at the NASA Goddard Space Flight Center is described and the problems in making space-based measurements of tropospheric ozone are considered. The differential absorption lidar using a dual wavelength, pulsed CO2 laser and direct detection receiver can significantly improve the existing global data base on tropospheric ozone burden. Sensitivity to tropospheric ozone can be obtained in the spaceborne version of lidar by selecting laser lines located in the wings of the target zone lines. Simulation studies using various laser line pairs in the P-branch of the CO2 9.4 micron band show that the ozone burden retrieval may be weighted to particular altitude regions. These simulation studies are based on numerical integration of differences in absorption coefficient at the two selected laser wavelengths using the AFGL absorption line parameter compilations, U.S. Standard Atmosphere ozone profile, and laser software. Simulation, data collection and reduction are performed by a microprocessor subsystem of the CO2 lidar.
Tropospheric delay calibrations are implemented in the Mark 3 system with two subsystems. Estimates of the dry component of tropospheric delay are provided by accurate barometric data from a subsystem of surface meteorological sensors (SMS). An estimate of the wet component of tropospheric delay is provided by a water vapor radiometer (WVR). Both subsystems interface directly to the ASCII Transceiver bus of the Mark 3 system and are operated by the control computer. Seven WVR's under construction are designed to operate in proximity to a radio telescope and can be commanded to point along the line-of-sight to a radio source. They should provide a delay estimate that is accurate to the + or - 2 cm level.