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NASA NTRSDate not supplied

Tropospheric Ozone in the NASA GEOS Model: Effects of Satellite NO2 Data Assimilation and Improvements in Background NOx Chemistry

Tropospheric ozone is a major atmospheric oxidant, the primary source of the hydroxyl radical, and a greenhouse gas. In the troposphere, it is produced from the oxidation of carbon monoxide and volatile organic compounds in the presence of nitrogen oxides (NOx=NO+NO2) or has its origins in the stratosphere. The tropospheric ozone burdens in global atmospheric chemistry models disagree by a factor of 1.5, indicating an incomplete understanding of ozone sources and sinks. Here we examine the tropospheric ozone simulation in NASA Global Modeling and Assimilation Office’s (GMAO’s) GEOS model with the GEOS-Chem chemistry mechanism (version 14.2), using observations from satellites, aircraft, ozonesondes, and surface sites. This modeling framework is used to produce GMAO’s GEOS Composition Forecasts (GEOS-CF), and it has been updated extensively with new emission inventories, improved model physics, satellite data assimilation capability, and an up-to-date chemical mechanism that includes tropospheric halogen chemistry and NOx recycling from particulate nitrate. Earlier versions of the model using GEOS-Chem version 12.0 showed an underestimate in tropospheric ozone in the northern hemisphere. We evaluate the ozone simulation in the updated model, focusing on the effects of assimilating satellite NO2 data from the Ozone Monitoring Instrument (OMI), constraining stratospheric ozone to satellite data, and updates to the NOx chemistry. We will examine changes in the vertical profiles of tropospheric ozone over the US in support of the Tropospheric Emissions: Monitoring of Pollution (TEMPO), and discuss implications for the tropospheric ozone budget.

V. Shah↗

NASA NTRSDate not supplied

Tropospheric Ozone in the NASA GEOS Model: Effects of Satellite Data Assimilation and Improvements in Background NO x Chemistry

Tropospheric ozone is a major atmospheric oxidant, the primary source of the hydroxyl radical, and a greenhouse gas. In the troposphere, it is produced from the oxidation of carbon monoxide and volatile organic compounds in the presence of nitrogen oxides (NO x =NO+NO 2 ) or has its origins in the stratosphere. The tropospheric ozone burdens in global atmospheric chemistry models disagree by a factor of 1.5, indicating an incomplete understanding of ozone sources and sinks. Here we examine the tropospheric ozone simulation in NASA Global Modeling and Assimilation Office’s (GMAO’s) GEOS model with the GEOS-Chem chemistry mechanism (version 14.2), using observations from satellites, aircraft, ozonesondes, and surface sites. This modeling framework is used to produce GMAO’s GEOS Composition Forecasts (GEOS-CF), and it has been updated extensively with new emission inventories, improved model physics, satellite data assimilation capability, and an up-to-date chemical mechanism that includes tropospheric halogen chemistry and NOx recycling from particulate nitrate. Earlier versions of the model using GEOS-Chem version 12.0 showed an underestimate in tropospheric ozone in the northern hemisphere. We evaluate the ozone simulation in the updated model, focusing on the effects of assimilating satellite NO 2 data from the Ozone Monitoring Instrument (OMI), constraining stratospheric ozone to satellite data, and updates to the NOx chemistry. We will examine changes in the vertical profiles of tropospheric ozone over the US in support of the Tropospheric Emissions: Monitoring of Pollution (TEMPO), and discuss implications for the tropospheric ozone budget.

Viral Shah↗

NASA NTRS1994

A PV view of the zonal mean distribution of temperature and wind in the extratropical troposphere

The dependence of the temperature and wind distribution of the zonal mean flow in the extratropical troposphere on the gradient of pontential vorticity along isentropes is examined. The extratropics here refer to the region outside the Hadley circulation. Of particular interest is whether the distribution of temperature and wind corresponding to a constant potential vorticity (PV) along isentropes resembles the observed, and the implications of PV homogenization along isentropes for the role of the tropics. With the assumption that PV is homogenized along isentropes, it is found that the temperature distribution in the extratropical troposphere may be determined by a linear, first-order partial differential equation. When the observed surface temperature distribution and tropical lapse rate are used as the boundary conditions, the solution of the equation is close to the observed temperature distribution except in the upper troposphere adjacent to the Hadley circulation, where the troposphere with no PV gradient is considerably colder. Consequently, the jet is also stronger. It is also found that the meridional distribution of the balanced zonal wind is very sensitive to the meridional distribution of the tropopause temperature. The result may suggest that the requirement of the global momentum balance has no practical role in determining the extratropical temperature distribution. The authors further investigated the sensitivity of the extratropical troposphere with constant PV along isentropes to changes in conditions at the tropical boundary (the edge of the Hadley circulation). It is found that the temperature and wind distributions in the extratropical troposphere are sensitive to the vertical distribution of PV at the tropical boundary. With a surface distribution of temperature that decreases linearly with latitude, the jet maximum occurs at the tropical boundary and moves with it. The overall pattern of wind distribution is not sensitive to the change of the position of the tropical boundary. Finally, the temperature and wind distributions of an extratropical troposphere with a finite PV gradient are calculated. It is found that the larger the isentropic PV gradient, the warmer the troposphere and the weaker the jet.

Sun, De-Zheng↗

NASA NTRS1998

Global tropospheric ozone investigations

Ozone (O3) is one of the most important trace gases in the troposphere, and it is responsible for influencing many critical chemical and radiative processes. Ozone contributes to the formation of the hydroxyl radical (OH), which is central to most chemical reactions in the lower atmosphere, and it absorbs UV, visible, and infrared radiation which affects the energy budget and atmospheric temperatures. In addition, O3 can be used as a tracer of atmospheric pollution and stratosphere troposphere exchange. At elevated concentrations, O3 can also produce detrimental biological and human health effects. The US National Research Council (NRC) Board on Sustainable Development reviewed the US Global Change Research Program (USGCRP) [NRC, 1995], and it identified tropospheric chemistry as one of the high priority areas for the USGCRP in the next decade. The NRC identified the following specific challenges in tropospheric chemistry. Although we understand the reason for the high levels of 03 over several regions of the world, we need to better establish the distribution of O3 in the troposphere in order to document and understand the changes in the abundance of global tropospheric O3. This information is needed to quantify the contribution of O3 to the Earth' s radiative balance and to understand potential impacts on the health of the biosphere. Having recognized the importance of particles in the chemistry of the stratosphere, we must determine how aerosols and clouds affect the chemical processes in the troposphere. This understanding is essential to predict the chemical composition of the atmosphere and to assess the resulting forcing effects in the climate system. We must determine if the self-cleansing chemistry of the atmosphere is changing as a result of human activities. This information is required to predict the rate at which pollutants are removed from the atmosphere. Over nearly two decades, airborne Differential Absorption Lidar (DIAL) systems have been used in over fifteen major field experiments conducted all over the world to address important atmospheric processes affecting the amount and distribution of 03 and aerosols across the troposphere. This paper discusses some of these wide-ranging field experiments and their results and presents a direction for future global studies of O3 and aerosols from space.

Browell, Edward V.↗

NASA NTRS2000

Observing Tropospheric Ozone From Space

The importance of tropospheric ozone embraces a spectrum of relevant scientific issues ranging from local environmental concerns, such as damage to the biosphere and human health, to those that impact global change questions, Such is climate warming. From an observational perspective, the challenge is to determine the tropospheric ozone global distribution. Because its lifetime is short compared with other important greenhouse gases that have been monitored over the past several decades, the distribution of tropospheric ozone cannot be inferred from a relatively small set of monitoring stations. Therefore, the best way to obtain a true global picture is from the use of space-based instrumentation where important spatial gradients over vast ocean expanses and other uninhabited areas can be properly characterized. In this paper, the development of the capability to measure tropospheric ozone from space over the past 15 years is summarized. Research in the late 1980s successfully led to the determination of the climatology of tropospheric ozone as a function of season; more recently, the methodology has improved to the extent where regional air pollution episodes can be characterized. The most recent modifications now provide quasi-global (50 N) to 50 S) maps on a daily basis. Such a data set would allow for the study of long-range (intercontinental) transport of air pollution and the quantification of how regional emissions feed into the global tropospheric ozone budget. Future measurement capabilities within this decade promise to offer the ability to provide Concurrent maps of the precursors to the in situ formation of tropospheric ozone from which the scientific community will gain unprecedented insight into the processes that control global tropospheric chemistry

Fishman, Jack↗

NASA NTRS2012

Analysis of Satellite-Derived Arctic Tropospheric BrO Columns in Conjunction with Aircraft Measurements During ARCTAS and ARCPAC

We derive tropospheric column BrO during the ARCTAS and ARCPAC field campaigns in spring 2008 using retrievals of total column BrO from the satellite UV nadir sensors OMI and GOME-2 using a radiative transfer model and stratospheric column BrO from a photochemical simulation. We conduct a comprehensive comparison of satellite-derived tropospheric BrO column to aircraft in-situ observations ofBrO and related species. The aircraft profiles reveal that tropospheric BrO, when present during April 2008, was distributed over a broad range of altitudes rather than being confined to the planetary boundary layer (PBL). Perturbations to the total column resulting from tropospheric BrO are the same magnitude as perturbations due to longitudinal variations in the stratospheric component, so proper accounting of the stratospheric signal is essential for accurate determination of satellite-derived tropospheric BrO. We find reasonably good agreement between satellite-derived tropospheric BrO and columns found using aircraft in-situ BrO profiles, particularly when satellite radiances were obtained over bright surfaces (albedo> 0.7), for solar zenith angle < 80 and clear sky conditions. The rapid activation of BrO due to surface processes (the bromine explosion) is apparent in both the OMI and GOME-2 based tropospheric columns. The wide orbital swath of OMI allows examination of the evolution of tropospheric BrO on about hourly time intervals near the pole. Low surface pressure, strong wind, and high PBL height are associated with an observed BrO activation event, supporting the notion of bromine activation by high winds over snow.

Choi, S.↗

NASA NTRS2019

Trends in Global Tropospheric Ozone Inferred from a Composite Record of TOMS/OMI/MLS/OMPS Satellite Measurements and the MERRA-2 GMI Simulation

Past studies have suggested that ozone in the troposphere has increased globally throughout much of the 20th century due to increases in anthropogenic emissions and transport. We show, by combining satellite measurements with a chemical transport model, that during the last four decades tropospheric ozone does indeed indicate increases that are global in nature, yet still highly regional. Satellite ozone measurements from Nimbus-7 and Earth Probe Total Ozone Mapping Spectrometer (TOMS) are merged with ozone measurements from the Aura Ozone Monitoring Instrument/Microwave Limb Sounder (OMI/MLS) to determine trends in tropospheric ozone for 1979–2016. Both TOMS (1979–2005) and OMI/MLS (2005–2016) depict large increases in tropospheric ozone from the Near East to India and East Asia and further eastward over the Pacific Ocean. The 38-year merged satellite record shows total net change over this region of about +6 to +7 Dobson units (DU) (i.e., ∼15 %–20 % of average background ozone), with the largest increase (∼4 DU) occurring during the 2005–2016 Aura period. The Global Modeling Initiative (GMI) chemical transport model with time-varying emissions is used to aid in the interpretation of tropospheric ozone trends for 1980–2016. The GMI simulation for the combined record also depicts the greatest increases of +6 to +7 DU over India and East Asia, very similar to the satellite measurements. In regions of significant increases in tropospheric column ozone (TCO) the trends are a factor of 2–2.5 larger for the Aura record when compared to the earlier TOMS record; for India and East Asia the trends in TCO for both GMI and satellite measurements are ∼+3 DU decade(exp −1) or greater during 2005–2016 compared to about +1.2 to +1.4 DU decade(exp −1) for 1979–2005. The GMI simulation and satellite data also reveal a tropospheric ozone increases in ∼+4 to +5 DU for the 38-year record over central Africa and the tropical Atlantic Ocean. Both the GMI simulation and satellite-measured tropospheric ozone during the latter Aura time period show increases of ∼+3 DU decade−1 over the N Atlantic and NE Pacific.

Ziemke, Jerald R.↗

NASA NTRS2013

Evaluation of ACCMIP Outgoing Longwave Radiation from Tropospheric Ozone Using TES Satellite Observations.

We use simultaneous observations of tropospheric ozone and outgoing longwave radiation (OLR) sensitivity to tropospheric ozone from the Tropospheric Emission Spectrometer (TES) to evaluate model tropospheric ozone and its effect on OLR simulated by a suite of chemistry-climate models that participated in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The ensemble mean of ACCMIP models show a persistent but modest tropospheric ozone low bias (5-20 ppb) in the Southern Hemisphere (SH) and modest high bias (5-10 ppb) in the Northern Hemisphere (NH) relative to TES ozone for 2005-2010. These ozone biases have a significant impact on the OLR. Using TES instantaneous radiative kernels (IRK), we show that the ACCMIP ensemble mean tropospheric ozone low bias leads up to 120mW/ sq. m OLR high bias locally but zonally compensating errors reduce the global OLR high bias to 39+/- 41mW/ sq. m relative to TES data. We show that there is a correlation (Sq. R = 0.59) between the magnitude of the ACCMIP OLR bias and the deviation of the ACCMIP preindustrial to present day (1750-2010) ozone radiative forcing (RF) from the ensemble ozone RF mean. However, this correlation is driven primarily by models whose absolute OLR bias from tropospheric ozone exceeds 100mW/ sq. m. Removing these models leads to a mean ozone radiative forcing of 394+/- 42mW/ sq. m. The mean is about the same and the standard deviation is about 30% lower than an ensemble ozone RF of 384 +/- 60mW/ sq. m derived from 14 of the 16 ACCMIP models reported in a companion ACCMIP study. These results point towards a profitable direction of combining satellite observations and chemistry-climate model simulations to reduce uncertainty in ozone radiative forcing.

troposphere↗

NASA NTRS2022

Tropospheric Ozone Retrieval By A Combination of TROPOMI/S5P Measurements With BASCOE Assimilated Data

We present a new tropospheric ozone dataset based on TROPOspheric Monitoring Instrument (TROPOMI)/Sentinel-5 Precursor (S5P) total ozone measurements combined with stratospheric ozone data from the Belgian Assimilation System for Chemical ObsErvations (BASCOE) constrained by assimilating ozone observations from the Microwave Limb Sounder (MLS). The BASCOE stratospheric data are interpolated to the S5P observations and subtracted from the TROPOMI total ozone data. The difference is equal to the tropospheric ozone residual column from the surface up to the tropopause. The tropospheric ozone columns are retrieved at the full spatial resolution of the TROPOMI sensor (5.5×3.5 km 2 ) with daily global coverage. Compared to the Ozone Mapping and Profiler Suite Modern-Era Retrospective analysis for Research and Applications 2 (OMPS-MERRA-2) data, a global mean positive bias of 3.3 DU is found for the analysed period April 2018 to June 2020. A small negative bias of about −0.91 DU is observed in the tropics relative to the operational TROPOMI tropical tropospheric data based on the convective cloud differential (CCD) algorithm throughout the same period. The new tropospheric ozone data (S5P-BASCOE) are compared to a set of globally distributed ozonesonde data integrated up to the tropopause level. We found 2254 comparisons with cloud-free TROPOMI observations within 25 km of the stations. In the global mean, S5P-BASCOE deviates by 2.6 DU from the integrated ozonesondes. Depending on the latitude the S5P-BASCOE deviate from the sondes and between −4.8 and 7.9 DU, indicating a good agreement. However, some exceptional larger positive deviations up to 12 DU are found, especially in the northern polar regions (north of 70∘). The monthly mean tropospheric column and time series for selected areas showed the expected spatial and temporal pattern, such as the wave one structure in the tropics or the seasonal cycle, including a summer maximum, in the mid-latitudes.

Satellite Retrieval↗

NASA NTRS1979

Observational and theoretical evidence in support of a significant in-situ photochemical source of tropospheric ozone

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.

Fishman, J.↗

NASA NTRS1985

The role of isoprene oxidation in the tropospheric ozone budget in the tropics

A comprehensive chemical mechanism for the oxidation of isoprene (a hydrocarbon, C5H8 emitted primarily by vegetation) by OH and O3 in the troposphere was developed and incorporated into a one-dimensional steady-state photochemical model of the troposphere. Flux boundary conditions for NOx (NO + NO2), HNO3, O3, and CO were used to investigate the changes produced in the tropospheric concentrations and integrated column of ozone from including isoprene chemistry in the model. Two calculations were performed at 15 deg N latitude for annual conditions using identical flux boundary conditions for NOx, HNO3, O3, and CO; in one calculation, the chemistry describing isoprene oxidation was included while in the other it was not. Both sets of calculations included reactions describing the chemistry of anthropogenic nonmethane hydrocarbons. The calculations showed decreases in concentrations of ozone throughout the troposphere when isoprene chemistry was included. Concentrations of NOx and HNO3 increased in the lower troposphere and decreased in the upper troposphere while concentrations of CO and PAN increased throughout the troposphere when isoprene chemistry was included. Implications of this study to the budgets of these species in the tropics is discussed.

Brewer, D. A.↗

NASA NTRS1990

Measurements of tropospheric nitric acid over the Western United States and Northeastern Pacific Ocean

Over 240 measurements of nitric acid (HNO3) were made in the free troposphere as well as in the boundary layer. Marine HNO3 measurement results were strikingly similar to results from GAMETAG and other past atmospheric field experiments. The marine boundary layer HNO3 average, 62 parts-per-trillion by volume (pptv), was 1/3 lower than the marine free tropospheric average, 108 pptv, suggesting that the boundary layer is a sink for tropospheric nitric acid, probably by dry deposition. Nitric acid measurements on a nighttime continental flight gave a free tropospheric average of 218 pptv, substantially greater than the daytime continental free tropospheric 5-flight average of 61 pptv. However, the nighttime results may be influenced by highly convective conditions that existed from thunderstorms in the vicinity during that night flight. The continental boundary layer HNO3 average of 767 pptv is an order of magnitude greater than the free tropospheric average, indicating that the boundary layer is a source of free tropospheric HNO3. The distribution of continental boundary layer HNO3 data, from averages of 123 over rural Nevada and Utah to 1057 pptv in the polluted San Joaquin Valley of California suggest a close tie between boundary layer HNO3 and anthropogenic activity.

Lebel, P. J.↗

NASA NTRS1992

Free tropospheric ozone production following entrainment of urban plumes into deep convection

It is shown that rapid vertical transport of air from urban plumes through deep convective clouds can cause substantial enhancement of the rate of O3 production in the free troposphere. Simulation of convective redistribution and subsequent photochemistry of an urban plume from Oklahoma City during the 1985 PRESTORM campaign shows enhancement of O3 production in the free tropospheric cloud outflow layer by a factor of almost 4. In contrast, simulation of convective transport of an urban plume from Manaus, Brazil, into a prestine free troposphere during GTE/ABLE 2B (1987), followed by a photochemical simulation, showed enhancement of O3 production by a factor of 35. The reasons for the different enhancements are (1) intensity of cloud vertical motion; (2) initial boundary layer O3 precursor concentrations; and (3) initial amount of background free tropospheric NO(x). Convective transport of ozone precursors to the middle and upper troposphere allows the resulting O3 to spread over large geographic regions, rather than being confined to the lower troposphere where loss processes are much more rapid. Conversely, as air with lower NO descends and replaces more polluted air, there is greater O3 production efficiency per molecule of NO in the boundary layer following convective transport. As a result, over 30 percent more ozone could be produced in the entire tropospheric column in the first 24 hours following convective transport of urban plumes.

Pickering, Kenneth E.↗

NASA NTRS1994

Ozone and aerosol distributions in the summertime troposphere over Canada

Measurements of ozone (O3) and aerosol distributions were made with an airborne lidar system in the lowland and boreal forest regions of eastern Canada during July - August 1990 as part of the NASA Global Tropospheric Experiment/Arctic Boundary Layer Expedition (ABLE) 3B. Aerosol and O3 profiles were measured simultaneously above and below the Electra aircraft from near the surface to above the tropopause on long-range flights over these important ecosystems. A broad range of atmospheric conditions were encountered during repeated flights over intensive study sites in the Hudson Bay lowlands near Moosonee, Ontario, and over the boreal forest near Schefferville, Quebec. The tropospheric composition in this high-latitude region was found to be strongly influenced by stratospheric intrusions. Regions of low aerosol scattering and enhanced O3 mixing ratios were correlated with descending air from the lower stratosphere. Over 33% of the troposphere (0-12 km) along our flight track at latitudes from about 45 deg to 55 deg N had significantly enhanced O3 due to stratospheric intrusions, and in the middle to upper troposphere the extent of the enhanced O3 gnerally exceeded 40%. Ozone mixing ratios of 80 parts per billion by volume (ppbv) near 6 km were common in strong intrusions. In the boundary layer over the lowlands, O3 was in the 20-30 ppbv range with a vertical O3 gradient of 6.7 ppbv/km to about 45 ppbv at 3 km. Above 6 km the background tropospheric O3 profile was nearly constant with an average value of 53 ppbv. Due to forest fires in Canada and Alaska, plumes from biomass-burning sources were observed on many flights. Biomass-burning plumes influenced about 25% of the free troposphere below 4 km, and in some of the plumes, O3 was enhanced by 10-20 ppbv over ambient levels of 30-45 ppbv. Several air masses transported from the tropical Pacific were observed over Canada in the middle to upper troposphere with O3 levels 10-20 ppbv below background values of 50-55 ppbv.

Browell, E. V.↗

NASA NTRS1994

Comparison of upper tropospheric water vapor from GOES, Raman lidar, and Cross-chain Loran Atmospheric Sounding System measurements

Observations of upper tropospheric relative humidity obtained from Raman lidar and Cross-chain Loran Atmospheric Sounding System (CLASS) sonde instruments obtained during the First ISCCP Regional Experiment (FIRE) Cirrus-II field program are compared with satellite measurements from the GOES 6.7-micron channel. The 6.7-micron channel is sensitive to water vapor integrated over a broad layer in the upper troposphere (roughly 500-200 mbar). Instantaneous measurements of the upper tropospheric relative humidity from GOES are shown to agree to within roughly 6% of the nearest lidar observations and 9% of the nearest CLASS observations. The CLASS data exhibit a slight yet systematic dry bias in upper tropospheric humidity, a result which is consistent with previous radiosonde intercomparisons. Temporal stratification of the CLASS data indicates that the magnitude of the bias is dependent upon the time of day, suggesting a solar heating effect in the radiosonde sensor. Using CLASS profiles, the impact of vertical variability in relative humidity upon the GOES upper tropospheric humidity measurements is also examined. The upper tropospheric humidity inferred from the GOES 6.7-micron channel is demonstrated to agree to within roughly 5% of the relative humidity vertically averaged over the depth of atmosphere to which the 6.7-micron channel is sensitive. The results of this study encourage the use of satellite measurements in the 6.7-micron channel to quantitatively describe the distribution and temporal evolution of the upper tropospheric humidity field.

Soden, B. J.↗

NASA NTRS1995

Monthly mean large-scale analyses of upper-tropospheric humidity and wind field divergence derived from three geostationary satellites

This paper describes the results from a collaborative study between the European Space Operations Center, the European Organization for the Exploitation of Meteorological Satellites, the National Oceanic and Atmospheric Administration, and the Cooperative Institute for Meteorological Satellite Studies investigating the relationship between satellite-derived monthly mean fields of wind and humidity in the upper troposphere for March 1994. Three geostationary meteorological satellites GOES-7, Meteosat-3, and Meteosat-5 are used to cover an area from roughly 160 deg W to 50 deg E. The wind fields are derived from tracking features in successive images of upper-tropospheric water vapor (WV) as depicted in the 6.5-micron absorption band. The upper-tropospheric relative humidity (UTH) is inferred from measured water vapor radiances with a physical retrieval scheme based on radiative forward calculations. Quantitative information on large-scale circulation patterns in the upper-troposphere is possible with the dense spatial coverage of the WV wind vectors. The monthly mean wind field is used to estimate the large-scale divergence; values range between about-5 x 10(exp -6) and 5 x 10(exp 6)/s when averaged over a scale length of about 1000-2000 km. The spatial patterns of the UTH field and the divergence of the wind field closely resemble one another, suggesting that UTH patterns are principally determined by the large-scale circulation. Since the upper-tropospheric humidity absorbs upwelling radiation from lower-tropospheric levels and therefore contributes significantly to the atmospheric greenhouse effect, this work implies that studies on the climate relevance of water vapor should include three-dimensional modeling of the atmospheric dynamics. The fields of UTH and WV winds are useful parameters for a climate-monitoring system based on satellite data. The results from this 1-month analysis suggest the desirability of further GOES and Meteosat studies to characterize the changes in the upper-tropospheric moisture sources and sinks over the past decade.

Schmetz, Johannes↗

NASA NTRS1996

A New Method of Deriving Time-Averaged Tropospheric Column Ozone over the Tropics Using Total Ozone Mapping Spectrometer (TOMS) Radiances: Intercomparison and Analysis Using TRACE A Data

Error analysis of archived total 03 from total ozone mapping spectrometer (TOMS) (version 6) presented. Daily total 03 maps for the tropics, from the period October 6-21, 1992, are derived from TOMS radiances following correction for these errors. These daily maps, averaged together, show a wavelike feature, which is observed in all latitude bands, underlying sharp peaks which occur at different longitudes depending on the latitude. The wave pattern is used to derive both time-averaged stratospheric and tropospheric 03 fields. The nature of the wave pattern (stratospheric or tropospheric) cannot be determined with certainty due to missing data (no Pacific sondes, no lower stratospheric Stratospheric Aerosol and Gas Experiment (SAGE) ozone for 18 months after the Mt. Pinatubo eruption) and significant uncertainties in the corroborative satellite record in the lower stratosphere (solar backscattered ultraviolet (SBUV), microwave limb sounder (MLS)). However, the time- averaged tropospheric ozone field, based on the assumption that the wave feature is stratospheric, agrees within 10% with ultraviolet differential absorption laser Transport and Atmospheric Chemistry near the Equator-Atlantic) (TRACE A) 03 measurements from the DC-8 and with ozonesonde measurements over Brazzaville, Congo, Ascension Island, and Natal, Brazil, for the period October 6-21, 1992. The derived background (nonpolluted) Indian Ocean tropospheric ozone amount, 26 Dobson units (DU), agrees with the cleanest African ozonesonde profiles for September-October 1992. The assumption of a totally tropospheric wave (flat stratosphere) gives 38 DU above the western Indian Ocean and 15-40% disagreements with the sondes. Tropospheric column 03 is high from South America to Africa, owing to interaction of dynamics with biomass burning emissions. Comparison with fire distributions from advanced very high resolution radiometer (AVHHR) during October 1992 suggests that tropospheric 03 produced from biomass burning in South America and Africa dominates the 03 budget in the tropical southern hemisphere during the study period.

Kim, J. H.↗

NASA NTRS1998

NO(x) Concentrations in the Upper Troposphere as a Result of Lightning

Upper tropospheric NO(x) controls, in part, the distribution of ozone in this greenhouse-sensitive region of the atmosphere. Many factors control NO(x) in this region. As a result it is difficult to assess uncertainties in anthropogenic perturbations to NO from aircraft, for example, without understanding the role of the other major NO(x) sources in the upper troposphere. These include in situ sources (lightning, aircraft), convection from the surface (biomass burning, fossil fuels, soils), stratospheric intrusions, and photochemical recycling from HNO3. This work examines the separate contribution to upper tropospheric "primary" NO(x) from each source category and uses two different chemical transport models (CTMS) to represent a range of possible atmospheric transport. Because aircraft emissions are tied to particular pressure altitudes, it is important to understand whether those emissions are placed in the model stratosphere or troposphere and to assess whether the models can adequately differentiate stratospheric air from tropospheric air. We examine these issues by defining a point-by-point "tracer tropopause" in order to differentiate stratosphere from troposphere in terms of NO(x) perturbations. Both models predict similar zonal average peak enhancements of primary NO(x) due to aircraft (approx. = 10-20 parts per trillion by volume (pptv) in both January and July); however, the placement of this peak is primarily in a region of large stratospheric influence in one model and centered near the level evaluated as the tracer tropopause in the second. Below the tracer tropopause, both models show negligible NO(x) derived directly from the stratospheric source. Also, they predict a typically low background of 1 - 20 pptv NO(x) when tropospheric HNO3 is constrained to be 100 pptv of HNO3. The two models calculate large differences in the total background NO(x) (defined as the source of NO(x) from lightning + stratosphere + surface + HNO3) when using identical loss frequencies for NO(x). This difference is primarily due to differing treatments of vertical transport. An improved diagnosis of this transport that is relevant to NO(x) requires either measurements of a surface-based tracer with a substantially shorter lifetime than Rn-222 or diagnosis and mapping of tracer correlations with different source signatures. Because of differences in transport by the two models we cannot constrain the source of NO(x) from lightning through comparison of average model concentrations with observations of NO(x).

Penner, Joyce E.↗