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At least 145 records · Page 8

NASA Global Tropospheric Experiment

The rationale and program design for the NASA Global Tropospheric Experiment (GTE) are described. The GTE is intended to characterize the global tropospheric chemistry and its interaction with the stratosphere, the land, and the ocean. The program emphasis is laid on the potential global impact of human activities, particularly those which release CH4, N2O, and chlorofluorocarbons into the atmosphere. Specific tasks defined thus far include characterizing the tropospheric gas-phase chemistry of OH, NO, and NO2, determining concentrations and distributions of CO, CH4, O3, and N2O, as well as halogens, trace metals, and reduced sulfur species. Techniques are needed for measuring the chemical fluxes between earth surface sources and sinks, the boundary layer, the free troposphere, and the stratosphere. The first phase of the GTE will be to test and develop techniques and assay the detection limits for OH, NO, and NO2 and assess the reliability of laboratory calibrations. Improvements in modelling global-scale tropospheric processes will also be pursued.

Mcneal, R. J.↗

Future instrumentation and missions for measurements of tropospheric trace species from space: Workshop recommendations

It was recommended that gas filter correlation radiometry and high-resolution interferometry be exploited and expanded for measurements of the distribution of tropospheric trace gases. Instruments and missions were identified and discussed. Several instrument/measurement/mission feasibility studies were recommended, including: a three-layer measurement of carbon monoxide, using a nadir-viewing gas filter correlation radiometer; a lower or middle tropospheric measurement of methane, using a nadir-viewing gas filter correlation radiometer; and a survey of lower, middle, and upper tropospheric trace gases using a nadir-viewing high-resolution interferometer operating in the thermal emission mode. It was also concluded that lidar systems appear to have the potential of obtaining measurments of tropospheric trace gases and aerosols from space. In addition to the specific instrument/mission recommendations, the panels made several general recommendations that may lead to future spaceborne instruments, techniques, and missions for tropospheric research.

Source record↗

Use of satellite data to study tropospheric ozone in the tropics

Three independent examples are discussed which suggest that photochemical ozone production in the troposphere can be observed in the tropics from an analysis of total ozone data. The first finding shows that the seasonal cycle of total columnar ozone is dominated by the seasonal cycle of tropospheric ozone, even though tropospheric ozone accounts for only 5-15 percent of the total ozone. Second, a case study is presented which shows that enhanced total ozone observed over the Amazon Basin can be associated with the presence of biomass burning. In situ measurements have confirmed that biomass burning does result in the production of photochemically generated ozone, analogous to the formation of 'smog' near industrialized areas. Third, an analysis of the distribution of carbon monoxide obtained from a Space Shuttle platform is strongly correlated with the concurrent distribution of total ozone between 5 deg S and 10 deg N. Because all of the sources of carbon monoxide are located in the troposphere, this finding likewise suggests that the gradients of total ozone at low latitudes must also reflect processes occurring in the troposphere.

Fishman, Jack↗

Planetary wave activity in the troposphere and stratosphere during the Northern Hemisphere winter

The relation between planetary wave activity in the troposphere and stratosphere during the Northern Hemisphere winter from December 1981-March 1982 is studied. The Eliassen-Palm (E-P) flux diagnostics was applied to global tropospheric data for 1000 to 100 mb and global stratospheric data for 70 to 0.4 mb. The vertical component of the E-P flux, which is a measure of the vertical propagation of wave activity, and wave driving are examined. It is observed that the magnitude of the vertical component of the E-P flux varies with a period of 10-15 days in both the troposphere and the stratosphere; however, the correlation between the wave activity in the troposphere and stratosphere is different during the pre- and postwarming periods. The two types of correspondence between the wave activity are: (1) an out-of-plane relationship and (2) an upward propagation of wave activity from the troposphere to the stratosphere. The dynamical features of these two periods are described.

Shiotani, Masato↗

The effect of spatial and temporal wet-troposphere fluctuations on connected element interferometry

Numerical integrations of the structure function of tropospheric inhomogeneities have been performed to assess the impact of water vapor fluctuations on connected element interferometry (CEI). The expectation value of the RMS troposphere error for a differential spacecraft-quasar observation is derived by integrating the spatial refractivity structure function along raypaths to both the spacecraft and quasar from two spatially separated sites. Correlations between the tropospheric conditions at the two sites, which can become significant for short baseline observations, are fully accounted for in this calculation. Temporal effects are treated by assuming a frozen-flow model in which a fixed spatial distribution blows over both sites. Two nominal observation scenarios are considered, along with variations to study the dependence of the resultant differential troposphere errors on baseline length, observation time, source separation angle, and elevation. Consecutive differential observations are found to be almost completely uncorrelated, implying that averaging many repeated differential observations can quickly reduce the troposphere error.

Edwards, C. D.↗

Precise estimation of tropospheric path delays with GPS techniques

Tropospheric path delays are a major source of error in deep space tracking. However, the tropospheric-induced delay at tracking sites can be calibrated using measurements of Global Positioning System (GPS) satellites. A series of experiments has demonstrated the high sensitivity of GPS to tropospheric delays. A variety of tests and comparisons indicates that current accuracy of the GPS zenith tropospheric delay estimates is better than 1-cm root-mean-square over many hours, sampled continuously at intervals of six minutes. These results are consistent with expectations from covariance analyses. The covariance analyses also indicate that by the mid-1990s, when the GPS constellation is complete and the Deep Space Network is equipped with advanced GPS receivers, zenith tropospheric delay accuracy with GPS will improve further to 0.5 cm or better.

Lichten, S. M.↗

An assessment of potential impact of alternative fluorocarbons on tropospheric ozone

While the chlorofuorocarbons (CFCs) such as CFC-11 (CFCl3) and CFC-12 (CF2Cl2) are chemically inert in the troposphere, the hydrogen-containing halocarbons being considered as their replacements can, to a large extent, be removed in the troposphere by the HO radical. These alternative halocarbons include the hydrochlorofluorocarbons (HCFCs) 123 (CF3CHCl2), 141b (CFCl2CH3), 142b (CF2ClCH3), 22 (CHF2Cl), and 124 (CF3CHFCl) and the hydrofluorocarbons (HCFs) 134a (CF3CH2F), 152a (CHF2CH3) and 125 (CF3CHF2). Listed are the rate constants (k) for the HO radical reaction of these compounds and their estimated chemical lifetimes in the troposphere. In this table, values of the lifetimes of these selected HCFCs and HCFs are seen to vary by more than a factor of more than ten ranging from 1.6 years for HFC 152a and HCFC 125 to as long as 28 years for HFC 125. Clearly, from the standpoint of avoiding or minimizing impact on stratospheric O3, those halocarbons with short tropospheric lifetimes are the desirable alternates. However, potential environmental consequences of their degradation in the troposphere should be assessed and taken into account in the selection process.

Niki, Hiromi↗

Long-term tropospheric and lower stratospheric ozone variations from ozonesonde observations

An analysis is presented of the long-term mean pressure-latitude seasonal distribution of tropospheric and lower stratospheric ozone for the four seasons covering, in part, over 20 years of ozonesonde data. The observed patterns show minimum ozone mixing ratios in the equatorial and tropical troposphere except in regions where net photochemical production is dominant. In the middle and upper troposphere, and low stratosphere to 50 mb, ozone increases from the tropics to subpolar latitudes of both hemispheres. In mid stratosphere, the ozone mixing ratio is a maximum over the tropics. The observed vertical ozone gradient is small in the troposphere but increases rapidly above the tropopause. The amplitude of the annual variation increases from a minimum in the tropics to a maximum in polar regions. Also, the amplitude increases with height at all latitudes up to about 30 mb where the phase of the annual variation changes abruptly. The phase of the annual variation is during spring in the boundary layer, summer in mid troposphere, and spring in the upper troposhere and lower stratosphere.

London, J.↗

The effect of tropospheric fluctuations on the accuracy of water vapor radiometry

Line-of-sight path delay calibration accuracies of 1 mm are needed to improve both angular and Doppler tracking capabilities. Fluctuations in the refractivity of tropospheric water vapor limit the present accuracies to about 1 nrad for the angular position and to a delay rate of 3x10(exp -13) sec/sec over a 100-sec time interval for Doppler tracking. This article describes progress in evaluating the limitations of the technique of water vapor radiometry at the 1-mm level. The two effects evaluated here are: (1) errors arising from tip-curve calibration of WVR's in the presence of tropospheric fluctuations and (2) errors due to the use of nonzero beamwidths for water vapor radiometer (WVR) horns. The error caused by tropospheric water vapor fluctuations during instrument calibration from a single tip curve is 0.26 percent in the estimated gain for a tip-curve duration of several minutes or less. This gain error causes a 3-mm bias and a 1-mm scale factor error in the estimated path delay at a 10-deg elevation per 1 g/cm(sup 2) of zenith water vapor column density present in the troposphere during the astrometric observation. The error caused by WVR beam averaging of tropospheric fluctuations is 3 mm at a 10-deg elevation per 1 g/cm(sup 2) of zenith water vapor (and is proportionally higher for higher water vapor content) for current WVR beamwidths (full width at half maximum of approximately 6 deg). This is a stochastic error (which cannot be calibrated) and which can be reduced to about half of its instantaneous value by time averaging the radio signal over several minutes. The results presented here suggest two improvements to WVR design: first, the gain of the instruments should be stabilized to 4 parts in 10(exp 4) over a calibration period lasting 5 hours, and second, the WVR antenna beamwidth should be reduced to about 0.2 deg. This will reduce the error induced by water vapor fluctuations in the estimated path delays to less than 1 mm for the elevation range from zenith to 6 deg for most observation weather conditions.

Wilcox, J. Z.↗

Airborne lidar measurements of ozone and aerosols in the summertime Arctic troposphere

Ozone (O3) and aerosol distributions were remotely measured from an aircraft using a differential absorption lidar (DIAL) system as part of the 1988 NASA Global Tropospheric Experiment - Arctic Boundary Layer Experiment (ABLE-3A). The airborne DIAL system made simultaneous measurements of O3 and aerosols from the surface to above the tropopause. These measurements were made in a broad range of atmospheric conditions over the tundra, ice, and ocean regions near Barrow and Bethel, Alaska, during July and August 1988. The tropospheric composition over the Arctic was found to be strongly influenced by stratospheric intrusions. Regions of low aerosol scattering and enhanced O3 mixing ratios were usually correlated with descending air from the upper troposphere or lower stratosphere. Several cases of enhanced O3 were observed during ABLE-3A in conjunction with enhanced aerosol layers in the free troposphere resulting from biomass burning. As was found in the Amazon, the products of biomass burning can significantly alter O3 concentrations in the troposphere. This paper describes the NASA airborne DIAL system and discusses the large-scale variations of O3 and aerosols observed with the airborne DIAL system during ABLE-3A.

Browell, Edward V.↗

Distribution of tropical tropospheric water vapor

Utilizing a conceptual model for tropical convection and observational data for water vapor, the maintenance of the vertical distribution of the tropical tropospheric water vapor is discussed. While deep convection induces large-scale subsidence that constrains the turbulent downgradient mixing to within the convective boundary layer and effectively dries the troposphere through downward advection, it also pumps hydrometeors into the upper troposphere, whose subsequent evaporation appears to be the major source of moisture for the large-scale subsiding motion. The development of upper-level clouds and precipitation from these clouds may also act to dry the outflow, thus explaining the low relative humidity near the tropopause. A one-dimensional model is developed to simulate the mean vertical structure of water vapor in the tropical troposphere. It is also shown that the horizontal variation of water vapor in the tropical troposphere above the trade-wind boundary layer can be explained by the variation of a moisture source that is proportional to the amount of upper-level clouds. Implications for the nature of water vapor feedback in global warming are discussed.

Sun, De-Zheng↗

Summertime partitioning and budget of NO(y) compounds in the troposphere over Alaska and Canada: ABLE 3B

As part of NASA's Arctic Boundary Layer Expedition 3A and 3B field measurement programs, measurements of NO(x), HNO3, PAN, PPN, and NO(y) were made in the middle to lower troposphere over Alaska and Canada during the summers of 1988 and 1990. These measurements are used to assess the degree of closure within the reactive odd nitrogen (N(x)O(y)) budget through the comparison of the values of NO(y) measured with a catalytic convertor to the sum of individually measured NO(y) (i) compounds (i.e., sigmaNO(y)(i) = NO(x) + HNO3 + PAN + PPN). Significant differences were observed between the various study regions. In the lower 6 km of the troposphere over Alaska and the Hudson Bay lowlands of Canada a significant fraction of the NO(y) budget (30 to 60%) could not be accounted for by the measured sigmaNO(y)i. This deficit in the NO(y) budget is about 100 to 200 parts per trillion by volume (pptv) in the lower troposphere (0.15 to 3 km) and about 200 to 400 pptv in the middle free troposphere (3 to 6.2 km). Conversely, the NO(y) budget in the northern Labrador and Quebec regions of Canada is almost totally accounted for within the combined measurement uncertainties of NO(y) and the various NO(y)(i) compounds. A substantial portion of the NO(y) budget's 'missing compounds' appears to be coupled to the photochemical and/or dynamical parameters influencing the tropospheric oxidative potential over these regions. A combination of factors are suggested as the causes for the variability observed in the NO(y) budget. In addition, the apparent stability of compounds represented by the NO(y) budget deficit in the lower-altitude range questions the ability of these compounds to participate as reversible reservoirs for 'active' odd nitrogen and suggest that some portion of the NO(y) budget may consist of relatively unreactive nitrogen-containing compounds.

Sandholm, S.↗

Evidence of seasonally dependent stratosphere-troposphere exchange and purging of lower stratospheric aerosol from a multiyear lidar data set

Tropospheric and lower stratospheric aerosol backscatter data obtained from a calibrated backscatter lidar at Pasadena, California (34 deg N latitude) over the 1984-1993 period clearly indicate tightly coupled aerosol optical properties in the upper troposphere and lower stratosphere in the winter and early spring, due to the active midlatitude stratospheric-tropospheric (ST) exchange processes occurring at this time of year. Lidar data indicate that during pre-Pinaturbo background conditions, the subsequent purging of the aerosol in the upper troposphere caused a significant reduction in the aerosol content throughout the 8 - 18 km altitude region in the early spring period. The post-Pinatubo evidence of intense exchange in the winter and early spring is a significant increase in the upper tropospheric aerosol content, such that the backscatter levels reach values nearly equivalent to the enhanced backscatter levels existing in the lower stratosphere. The calculated stratospheric mass extrusion rate is consistent with a 45-day lifetime of lower stratospheric aerosol during this part of the year, which implies that midlatitude ST exchange is a significant sink for stratospheric aerosol.

Menzies, Robert T.↗

Origin of Ozone NO(x) in the Tropical Troposphere: A Photochemical Analysis of Aircraft Observations Over the South Atlantic Basin

The photochemistry of the troposphere over the South Atlantic basin is examined by modeling of aircraft observations up to 12-km altitude taken during the TRACE A expedition in September-October 1992. A close balance is found in the 0 to 12-km column between photochemical production and loss Of O3, with net production at high altitudes compensating for weak net loss at low altitudes. This balance implies that O3 concentrations in the 0-12 km column can be explained solely by in situ photochemistry; influx from the stratosphere is negligible. Simulation of H2O2, CH3OOH, and CH2O concentrations measured aboard the aircraft lends confidence in the computations of O3 production and loss rates, although there appears to be a major gap in current understanding of CH2O chemistry in the marine boundary layer. The primary sources of NO(x) over the South Atlantic Basin appear to be continental (biomass burning, lightning, soils). There is evidence that NO(x) throughout the 0 to 12-km column is recycled from its oxidation products rather than directly transported from its primary sources. There is also evidence for rapid conversion of HNO3 to NO(x) in the upper troposphere by a mechanism not included in current models. A general representation of the O3 budget in the tropical troposphere is proposed that couples the large scale Walker circulation and in situ photochemistry. Deep convection in the rising branches of the Walker circulation injects NO(x) from combustion, soils, and lightning to the upper troposphere, leading to O3 production; eventually, the air subsides and net O3 loss takes place in the lower troposphere, closing the O3 cycle. This scheme implies a great sensitivity of the oxidizing power of the atmosphere to NO(x) emissions in the tropics.

Jacob, D. J.↗

Chemical Characteristics of Continental Outflow from Asia to the Troposphere over the Western Pacific Ocean during September - October 1991: Results from PEM-West A

An important objective of the Pacific Exploratory Mission-West A (PEM-West A) was the chemical characterization of the outflow of tropospheric trace gases and aerosol particles from the Asian continent over the western Pacific Ocean. This paper summarizes the chemistry of this outflow during the period September - October 1991. The vertical distributions of CO, C2H6, and NO(x), showed regions of outflow at altitudes below 2 km and from 8 to 12 km. Mixing ratios of CO were approx. equals 130 parts per billion by volume (ppbv), approx. equals 1OOO parts per trillion by volume (pptv) for C2H6, and approx. equals 100 pptv for NO(x) in both of these regions. Direct outflow of Asian industrial materials was clearly evident at altitudes below 2 km, where halocarbon tracer compounds such as CH3CCl3 and C2Cl4 were enhanced about threefold compared to aged Pacific air. The source attribution of species outflowing from Asia to the Pacific at 8-12 km altitude was not straightforward. Above 10 km altitude there were substantial enhancements of NO(y), O3, CO, CH4, SO2, C2H6, C3H8, C2H2, and aerosol Pb-210 but not halocarbon industrial tracers. These air masses were rich in nitrogen relative to sulfur and contained ratios of C2H2/CO and C3H8/C2H6 (approx. equals l.5 and 0.1 respectively) indicative of several- day-old combustion emissions. It is unclear if these emissions were of Asian origin, or if they were rapidly transported to this region from Europe by the high wind speeds in this tropospheric region (60 - 70 m/s). The significant cyclonic activity over Asia at this time could have transported to the upper troposphere emissions from biomass burning in Southeast Asia or emissions from the extensive use of various biomass materials for cooking and space heating. Apparently, the emissions in the upper troposphere were brought there by wet convective systems since water-soluble gases and aerosols were depleted in these air masses. Near 9 km altitude there was a distinct regional outflow that appeared to be heavily influenced by biogenic processes on the Asian continent, especially from the southeastern area. These air masses contained CH4 in excess of 1800 ppbv, while CO2 and OCS were significantly depleted (349 - 352 ppmv and 450 - 500 pptv, respectively). This signature seemingly reflected CH4 emissions from wetlands and rice paddies with coincident biospheric uptake of tropospheric CO2 and OCS.

Talbot, R. W.↗

Global Troposphere Experiment Project

For the Global Troposphere Experiment project Pacific Exploratory Measurements West B (PEM West B), we made determinations of sulfur dioxide (SO2) and dimethyl sulfide (DMS) using gas chromatography-mass spectrometry with isotopically labelled internal standards. This technique provides measurements with precision of 1 part-per-trillion by volume below 20 pptv and 1% above 20 pptv. Measurement of DMS and SO2 were performed with a time cycle of 5-6 minutes with intermittent zero checks. The detection limits were about 1 pptv for SO2 and 2 pptv for DMS. Over 700 measurements of each compound were made in flight. Volcanic impacts on the upper troposphere were again found as a result of deep convection in the tropics. Extensive emission of SO2 from the Pacific Rim land masses were primarily observed in the lower well-mixed part of the boundary layer but also in the upper part of the boundary layer. Analyses of the SO2 data with aerosol sulfate, beryllium-7, and lead-210 indicated that SO2, contributed to half or more of the observed total oxidized sulfur (SO2 plus aerosol sulfate) in free tropospheric air. Cloud processing and rain appeared to be responsible for lower SO2 levels between 3 and 8.5 km than above or below this region. During both phases of PEM-West, dimethyl sulfide did not appear to be a major source of sulfur dioxide in the upper free troposphere over the western Pacific Ocean. In 1991 the sources Of SO2 at high altitude appeared to be both anthropogenic and volcanic with an estimated 1% being solely from DMS. The primary difference for the increase in the DMS source was the very low concentration of SO2 at high altitude. In the midlatitude region near the Asian land masses, DMS in the mixed layer was lower than in the tropical region of the western Pacific. Convective cloud systems near volcanoes in the tropical convergence in the western Pacific troposphere were a major source of SO2 at high altitudes during PEM-West B. High levels of SO2 were observed in several instances with large number concentrations of ultrafine CN above 9 km in the tropical convergence zone. Conversion of SO2, by OH to SO3 and subsequently to sulfuric acid may have been enhanced by lightning-produced NO levels exceeding 1 part per billion. Coupling of strong convection and volcanic sources of SO2 apparently is an important source of new particle formation at high altitude in the tropical convergence zone.

Bandy, Alan R.↗

Hydrogen Radicals, Nitrogen Radicals, and the Production of O3 in the Upper Troposphere

The concentrations of the hydrogen radicals OH and HO2 in the middle and upper troposphere were measured simultaneously with those of NO, O3, CO, H2O, CH4, non-methane hydrocarbons, and with the ultraviolet and visible radiation field. The data allow a direct examination of the processes that produce O3 in this region of the atmosphere. Comparison of the measured concentrations of OH and HO2 with calculations based on their production from water vapor, ozone, and methane demonstrate that these sources are insufficient to explain the observed radical concentrations in the upper troposphere. The photolysis of carbonyl and peroxide compounds transported to this region from the lower troposphere may provide the source of HO, required to sustain the measured abundances of these radical species. The mechanism by which NO affects the production Of O3 is also illustrated by the measurements. In the upper tropospheric air masses sampled, the production rate for ozone (determined from the measured concentrations of HO2 and NO) is calculated to be about I part per billion by volume each day. This production rate is faster than previously thought and implies that anthropogenic activities that add NO to the upper troposphere, such as biomass burning and aviation, will lead to production of more 03 than expected.

Wennberg, P. O.↗

Hydrogen Radicals, Nitrogen Radicals, and the Production of O3 in the Upper Troposphere

The concentrations of the hydrogen radicals OH and HO2 in the middle and upper troposphere were measured simultaneously with those of NO, O3, CO, H2O, CH4, non-methane hydrocarbons, and with the ultraviolet and visible radiation field. The data allow a direct examination of the processes that produce O3 in this region of the atmosphere. Comparison of the measured concentrations of OH and HO2 with calculations based on their production from water vapor, ozone, and methane demonstrate that these sources are insufficient to explain the observed radical concentrations in the upper troposphere. The photolysis of carbonyl and peroxide compounds transported to this region from the lower troposphere may provide the source of HO(sub x) required to sustain the measured abundances of these radical species. The mechanism by which NO affects the production of O3 is also illustrated by the measurements. In the upper tropospheric air masses sampled, the production rate for ozone (determined from the measured concentrations of HO2 and NO) is calculated to be about 1 part per billion by volume each day. This production rate is faster than previously thought and implies that anthropogenic activities that add NO to the upper troposphere, such as biomass burning and aviation, will lead to production of more O3 than expected.

Wennberg, P. O.↗