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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.↗
NASA NTRS1998

The Impact of Upper Tropospheric Humidity from Microwave Limb Sounder on the Midlatitude Greenhouse Effect

This paper presents an analysis of upper tropospheric humidity, as measured by the Microwave Limb Sounder, and the impact of the humidity on the greenhouse effect in the midlatitudes. Enhanced upper tropospheric humidity and an enhanced greenhouse effect occur over the storm tracks in the North Pacific and North Atlantic. In these areas, strong baroclinic activity and the large number of deep convective clouds transport more water vapor to the upper troposphere, and hence increase greenhouse trapping. The greenhouse effect increases with upper tropospheric humidity in areas with a moist upper troposphere (such as areas over storm tracks), but it is not sensitive to changes in upper tropospheric humidity in regions with a dry upper troposphere, clearly demonstrating that there are different mechanisms controlling the geographical distribution of the greenhouse effect in the midlatitudes.

Hu, Hua↗
NASA NTRS2000

Ozone in the Pacific Troposphere from Ozonesonde Observations

Ozone vertical profile measurements obtained from ozonesondes flown at Fiji, Samoa, Tahiti and the Galapagos are used to characterize ozone in the troposphere over the tropical Pacific. There is a significant seasonal variation at each of these sites. At sites in both the eastern and western Pacific, ozone is highest at almost all levels in the troposphere during the September-November season and lowest during, March-May. There is a relative maximum at all of the sites in the mid-troposphere during all seasons of the year (the largest amounts are usually found near the tropopause). This maximum is particularly pronounced during, the September-November season. On average, throughout the troposphere at all seasons, the Galapagos has larger ozone amounts than the western Pacific sites. A trajectory climatology is used to identify the major flow regimes that are associated with the characteristic ozone behavior at various altitudes and seasons. The enhanced ozone seen in the mid-troposphere during September-November is associated with flow from the continents. In the western Pacific this flow is usually from southern Africa (although 10-day trajectories do not always reach the continent), but also may come from Australia and Indonesia. In the Galapagos the ozone peak in the mid-troposphere is seen in flow from the South American continent and particularly from northern Brazil. The time of year and flow characteristics associated with the ozone mixing ratio peaks seen in both the western and eastern Pacific suggest that these enhanced ozone values result from biomass burning. In the upper troposphere low ozone amounts are seen with flow that originates in the convective western Pacific.

Oltmans, S. J.↗
NASA NTRS2001

Tropical Tropospheric Ozone and Smoke Interactions: Satellite Observations During the 1997 Indonesian Fires

Biomass burning generates hydrocarbons, nitrogen oxides and carbon monoxide that lead to tropospheric ozone pollution. Other combustion products form soot and various aerosol particles that make up smoke. Since early 1997 smoke and tropospheric ozone have been monitored in real-time from TOMS (Total Ozone Mapping Spectrometer) at toms.gsfc.nasa.gov (smoke aerosol) and metosrv2.umd.edu/-tropo (tropospheric ozone). The striking increase in smoke and tropospheric ozone observed during the 1997 Indonesian fires was the first extreme episode observed. During the August-November period, plumes of excess ozone and smoke coincided at times but were decoupled at other times, a phenomenon followed with trajectories. Thus, trans-boundary evolution of smoke and ozone differed greatly. The second discovery of the 1997 TOMS record was a dynamical interaction of ozone with the strong El Nino Southern Oscillation (ENSO) and Indian Ocean Dipole (IOD) that led to a jump in tropospheric ozone in March 1997 over the entire Indian Ocean, well ahead of the intense burning period. A climatology of smoke and tropospheric ozone from a 1980's TOMS instrument shows offsets in the timing of these pollutants - further evidence that factors other than biomass burning exert a strong influence on tropical tropospheric ozone.

Thompson, A. M.↗
NASA NTRS2001

SHADOZ (Southern Hemisphere ADditional Ozonesondes): A Look at the First Three Years' (1998-2000) Tropospheric Ozone Data

The first climatological overview of total, stratospheric and tropospheric ozone in the southern hemisphere tropical and subtropics is based on ozone sounding data from 10 sites comprising the Southern Hemisphere ADditional OZonesondes (SHADOZ) network. The period covered is 1998-2000. Observations were made over: Ascension Island; Nairobi, Kenya; Irene, South Africa; RCunion Island; Watukosek, Java; Fiji; Tahiti; American Samoa; San Cristobal, Galapagos; Natai, Brazil. Campaign data were collected on a trans-Atlantic oceanographic cruise and during SAFARI-2000 in Zambia. The ozone data, with simultaneous temperature profiles to approx. 7 hPa and relative humidity to approx. 200 hPa, reside at an open archive: . SHADOZ ozone time-series and profiles give a perspective on tropical total, stratospheric and tropospheric ozone in 1998-2000. Prominent features are highly variable tropospheric ozone, a zonal wave-one pattern in total (and tropospheric) column ozone, and signatures of the Quasi-Biennial Oscillation (QBO) in stratospheric ozone. Total, stratospheric and tropospheric column ozone amounts peak between August and November and are lowest between March and May. Tropospheric ozone variability over the Indian and Pacific Ocean displays influences of the Indian Ocean Dipole, ENSO, and Madden-Julian circulation on convective mixing. Pollution transport from Africa, South American and the Maritime Continent is a seasonal feature. Tropospheric ozone seasonality over the Atlantic Basin shows effects of regional subsidence and recirculation as well as biomass burning. Dynamical and chemical influences appear to be of comparable magnitude.

Thompson, Anne M.↗
NASA NTRS2002

SHADOZ (Southern Hemisphere ADditional Ozonesondes): What Have We Learned About Tropical Tropospheric Ozone from the First Three Years' (1998-2000) Data?

The first climatological overview of total, stratospheric and tropospheric ozone in the southern hemisphere tropical and subtropics is based on ozone sounding data from 10 sites comprising the Southern Hemisphere Additional OZonesondes (SHADOZ) network. The period covered is 1998-2000. Observations were made over: Ascension Island; Nairobi, Kenya; Irene, South Africa; RCunion Island; Watukosek, Java; Fiji; Tahiti; American Samoa; San Cristobal, Galapagos; Natal, Brazil. Campaign data were collected on a trans-Atlantic oceanographic cruise and during SAFARI-2000 in Zambia. The ozone data, with simultaneous temperature profiles to approx. 7 hPa and relative humidity to approx. 200 hPa, reside at: . SHADOZ ozone time-series and profiles give a perspective on tropical total, stratospheric and tropospheric ozone in 1998-2000. Prominent features are highly variable tropospheric ozone, a zonal wave-one pattern in total (and tropospheric) column ozone, and signatures of the Quasi-Biennial Oscillation (QBO) in stratospheric ozone. Total, stratospheric and tropospheric column ozone amounts peak between August and November and are lowest between March and May. Tropospheric ozone variability over the Indian and Pacific Ocean displays influences of the Indian Ocean Dipole, and convective mixing. Pollution transport from Africa, South American and the Maritime Continent is a seasonal feature. Tropospheric ozone seasonality over the Atlantic Basin shows effects of regional subsidence and recirculation as well as biomass burning. Dynamical and chemical influences appear to be of comparable magnitude though model studies are needed to quantify this.

Thompson, Anne M.↗
NASA NTRS2002

SHADOZ (Southern Hemisphere ADditional Ozonesondes}: What Have We Learned About Tropical Tropospheric Ozone from the First Three Years (1998-2000) Data

The first climatological overview of total, stratospheric and tropospheric ozone in the southern hemisphere tropical and subtropics is based on ozone sounding data from 10 sites comprising the Southern Hemisphere Additional OZonesondes (SHADOZ) network. The period covered is 1998-2000. Observations were made over: Ascension Island; Nairobi, Kenya; Irene, South Africa; Reunion Island; Watukosek, Java; Fiji; Tahiti; American Samoa; San Cristobal, Galapagos; Natal, Brazil. Campaign data were collected on an Trans-Atlantic oceanographic cruise and during SAFARI-2000 in Zambia. The ozone data, with simultaneous temperature profiles to approximately 7 hPa and relative humidity to approximately 200 hPa, reside at: . SHADOZ ozone time-series and profiles give a perspective on tropical total, stratospheric and tropospheric ozone in 1998-2000. Prominent features are highly variable tropospheric ozone, a zonal wave-one pattern in total (and tropospheric) column ozone, and signatures of the Quasi-Biennial Oscillation (QBO) in stratospheric ozone. Total, stratospheric and tropospheric column ozone amounts peak between August and November and are lowest between March and May. Tropospheric ozone variability over the Indian and Pacific Ocean displays influences of the Indian Ocean Dipole, and convective mixing. Pollution transport from Africa, South American and the Maritime Continent is a seasonal feature. Tropospheric ozone seasonality over the Atlantic Basin shows effects of regional subsidence and recirculation as well as biomass burning. Dynamical and chemical influences appear to be of comparable magnitude though model studies are needed to quantify this.

Thompson, Anne M.↗
NASA NTRS2002

Tropical Tropospheric Ozone from SHADOZ (Southern Hemisphere ADditional Ozonesondes) Network: A Project for Satellite Research, Process Studies, Education

The first climatological overview of total, stratospheric and tropospheric ozone in the southern hemisphere tropical and subtropics is based on ozone sounding data from 10 sites comprising the Southern Hemisphere Additional OZonesondes (SHADOZ) network. The period covered is 1998-2000. Observations were made over: Ascension Island; Nairobi, Kenya; Irene, South Africa; Reunion Island; Watukosek, Java; Fiji; Tahiti; American Samoa; San Cristobal, Galapagos; Natal, Brazil. Campaign data were collected on a trans-Atlantic oceanographic cruise and during SAFARI-2000 in Zambia. The ozone data, with simultaneous temperature profiles to approx. 7 hPa and relative humidity to approx. 200 hPa, reside at: . SHADOZ ozone time-series and profiles give a perspective on tropical total, stratospheric and tropospheric ozone. Prominent features are highly variable tropospheric ozone and a zonal wave-one pattern in total (and tropospheric) column ozone. Total, stratospheric and tropospheric column ozone amounts peak between August and November and are lowest between March and May. Tropospheric ozone variability over the Indian and Pacific Ocean displays influences of the Indian Ocean Dipole and convective mixing. Pollution transport from Africa and South America is a seasonal feature. Tropospheric ozone seasonality over the Atlantic Basin shows effects of regional subsidence and recirculation as well as biomass burning. Dynamical and chemical influences appear to be of comparable magnitude though model studies are needed to quantify this.

Thompson, Anne M.↗
NASA NTRS2004

Characterization of Transport Errors in Chemical Forecasts from a Global Tropospheric Chemical Transport Model

We propose a new methodology to characterize errors in the representation of transport processes in chemical transport models. We constrain the evaluation of a global three-dimensional chemical transport model (GEOS-CHEM) with an extended dataset of carbon monoxide (CO) concentrations obtained during the Transport and Chemical Evolution over the Pacific (TRACE-P) aircraft campaign. The TRACEP mission took place over the western Pacific, a region frequently impacted by continental outflow associated with different synoptic-scale weather systems (such as cold fronts) and deep convection, and thus provides a valuable dataset. for our analysis. Model simulations using both forecast and assimilated meteorology are examined. Background CO concentrations are computed as a function of latitude and altitude and subsequently subtracted from both the observed and the model datasets to focus on the ability of the model to simulate variability on a synoptic scale. Different sampling strategies (i.e., spatial displacement and smoothing) are applied along the flight tracks to search for systematic model biases. Statistical quantities such as correlation coefficient and centered root-mean-square difference are computed between the simulated and the observed fields and are further inter-compared using Taylor diagrams. We find no systematic bias in the model for the TRACE-P region when we consider the entire dataset (i.e., from the surface to 12 km ). This result indicates that the transport error in our model is globally unbiased, which has important implications for using the model to conduct inverse modeling studies. Using the First-Look assimilated meteorology only provides little improvement of the correlation, in comparison with the forecast meteorology. These general statements can be refined when the entire dataset is divided into different vertical domains, i.e., the lower troposphere (less than 2 km), the middle troposphere (2-6 km), and the upper troposphere (greater than 6 km). The best agreement between the observations and the model is found in the lower and middle troposphere. Downward displacements in the lower troposphere provide a better fit with the observed value, which could indicate a problem in the representation of boundary layer height in the model. Significant improvement is also found for downward and southward displacements in the upper troposphere. There are several potential sources of errors in our simulation of the continental outflow in the upper troposphere which could lead to such biases, including the location and/or the strength of deep convective cells as well as that of wildfires in Southeast Asia.

Bey, I.↗
NASA NTRS2007

Reactive Nitrogen Distribution and Partitioning in the North American Troposphere and Lowermost Stratosphere

A comprehensive group of reactive nitrogen species (NO, NO2, HNO3, HO2NO2, PANs, alkyl nitrates, and aerosol-NO3) were measured in the troposphere and lowermost stratosphere over North America and the Atlantic during July/August 2004 (INTEX-A) from the NASA DC-8 platform (0.1-12 km). Less reactive nitrogen species (HCN and CH3CN), that are also unique tracers of biomass combustion, were also measured along with a host of other gaseous (CO, VOC, OVOC, halocarbon) and aerosol tracers. Clean background air as well as air with influences from biogenic emissions, anthropogenic pollution, biomass combustion, and stratosphere was sampled both over continental U. S., Atlantic and Pacific. The North American upper troposphere was found to be greatly influenced by both lightning NO(x) and surface pollution lofted via convection and contained elevated concentrations of PAN, ozone, hydrocarbons, and NO(x). Under polluted conditions PAN was a dominant carrier of reactive nitrogen in the upper troposphere while nitric acid dominated in the lower troposphere. Peroxynitric acid (HO2NO2) was present in sizable concentrations always peaking at around 8 km. Aerosol nitrate appeared to be mostly contained in large soil based particles in the lower troposphere. Plumes from Alaskan fires contained large amounts of PAN and very little enhancement in ozone. Observational data suggest that lightning was a far greater contributor to NO(x) in the upper troposphere than previously believed. NO(x) and NO(y) reservoir appeared to be in steady state only in the middle troposphere where NO(x)/NO(y) was independent of air mass age. A first comparison of observed data with simulations from four 3-D models shows significant differences between observations and models as well as among models. These uncertainties likely propagate themselves in satellites derived NOx data. Observed data are interpreted to suggest that soil sinks of HCN/CH3CN are at best very small. We investigate the partitioning and interplay of the reactive nitrogen species within characteristic air masses and further examine their role in ozone formation.

Singh, H. B.↗
NASA NTRS2004

Climate Response to the Increase in Tropospheric Ozone since Preindustrial Times: A Comparison between Ozone and Equivalent CO2 Forcings

We examine the characteristics of the climate response to anthropogenic changes in tropospheric ozone. Using a general circulation model, we have carried out a pair of equilibrium climate simulations with realistic present-day and preindustrial ozone distributions. We find that the instantaneous radiative forcing of 0.49 W m(sup -2) due to the increase in tropospheric ozone since preindustrial times results in an increase in global mean surface temperature of 0.28 C. The increase is nearly 0.4 C in the Northern Hemisphere and about 0.2 C in the Southern Hemisphere. The largest increases (greater than 0.8 C) are downwind of Europe and Asia and over the North American interior in summer. In the lower stratosphere, global mean temperatures decrease by about 0.2 C due to the diminished upward flux of radiation at 9.6 micrometers. The largest stratospheric cooling, up to 1.0 C, occurs over high northern latitudes in winter, with possibly important implications for the formation of polar stratospheric clouds. To identify the characteristics of climate forcing unique to tropospheric ozone, we have conducted two additional climate equilibrium simulations: one in which preindustrial tropospheric ozone concentrations were increased everywhere by 18 ppb, producing the same global radiative forcing as present-day ozone but without the heterogeneity; and one in which CO2 was decreased by 25 ppm relative to present day, with ozone at present-day values, to again produce the same global radiative forcing but with the spectral signature of CO2 rather than ozone. In the first simulation (uniform increase of ozone), the global mean surface temperature increases by 0.25 C, with an interhemispheric difference of only 0.03 C, as compared with nearly 0.2 C for the heterogeneous ozone increase. In the second simulation (equivalent CO2), the global mean surface temperature increases by 0.36 C, 30% higher than the increase from tropospheric ozone. The stronger surface warming from CO2 is in part because CO2 forcing (obscured by water vapor) is shifted relatively poleward where the positive ice-albedo feedback amplifies the climate response and in part because the magnitude of the CO2 forcing in the mid-troposphere is double that of ozone. However, we find that CO2 is far less effective than tropospheric ozone in driving lower stratospheric cooling at high northern latitudes in winter.

Mickley L. J.↗
NASA NTRS2013

Software for Generating Troposphere Corrections for InSAR Using GPS and Weather Model Data

Atmospheric errors due to the troposphere are a limiting error source for spaceborne interferometric synthetic aperture radar (InSAR) imaging. This software generates tropospheric delay maps that can be used to correct atmospheric artifacts in InSAR data. The software automatically acquires all needed GPS (Global Positioning System), weather, and Digital Elevation Map data, and generates a tropospheric correction map using a novel algorithm for combining GPS and weather information while accounting for terrain. Existing JPL software was prototypical in nature, required a MATLAB license, required additional steps to acquire and ingest needed GPS and weather data, and did not account for topography in interpolation. Previous software did not achieve a level of automation suitable for integration in a Web portal. This software overcomes these issues. GPS estimates of tropospheric delay are a source of corrections that can be used to form correction maps to be applied to InSAR data, but the spacing of GPS stations is insufficient to remove short-wavelength tropospheric artifacts. This software combines interpolated GPS delay with weather model precipitable water vapor (PWV) and a digital elevation model to account for terrain, increasing the spatial resolution of the tropospheric correction maps and thus removing short wavelength tropospheric artifacts to a greater extent. It will be integrated into a Web portal request system, allowing use in a future L-band SAR Earth radar mission data system. This will be a significant contribution to its technology readiness, building on existing investments in in situ space geodetic networks, and improving timeliness, quality, and science value of the collected data

Moore, Angelyn W.↗
NASA NTRS2014

Global Free Tropospheric NO2 Abundances Derived Using a Cloud Slicing Technique Applied to Satellite Observations from the Aura Ozone Monitoring Instrument (OMI)

We derive free-tropospheric NO2 volume mixing ratios (VMRs) and stratospheric column amounts of NO2 by applying a cloud slicing technique to data from the Ozone Monitoring Instrument (OMI) on the Aura satellite. In the cloud-slicing approach, the slope of the above-cloud NO2 column versus the cloud scene pressure is proportional to the NO2 VMR. In this work, we use a sample of nearby OMI pixel data from a single orbit for the linear fit. The OMI data include cloud scene pressures from the rotational-Raman algorithm and above-cloud NO2 vertical column density (VCD) (defined as the NO2 column from the cloud scene pressure to the top-of-the-atmosphere) from a differential optical absorption spectroscopy (DOAS) algorithm. Estimates of stratospheric column NO2 are obtained by extrapolating the linear fits to the tropopause. We compare OMI-derived NO2 VMRs with in situ aircraft profiles measured during the NASA Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign in 2006. The agreement is generally within the estimated uncertainties when appropriate data screening is applied. We then derive a global seasonal climatology of free-tropospheric NO2 VMR in cloudy conditions. Enhanced NO2 in the free troposphere commonly appears near polluted urban locations where NO2 produced in the boundary layer may be transported vertically out of the boundary layer and then horizontally away from the source. Signatures of lightning NO2 are also shown throughout low and middle latitude regions in summer months. A profile analysis of our cloud slicing data indicates signatures of uplifted and transported anthropogenic NO2 in the middle troposphere as well as lightning-generated NO2 in the upper troposphere. Comparison of the climatology with simulations from the Global Modeling Initiative (GMI) for cloudy conditions (cloud optical thicknesses > 10) shows similarities in the spatial patterns of continental pollution outflow. However, there are also some differences in the seasonal variation of free-tropospheric NO2 VMRs near highly populated regions and in areas affected by lightning-generated NOx. Stratospheric column NO2 obtained from cloud slicing agrees well with other independently-generated estimates, providing further confidence in the free-tropospheric results.

NO2↗
NASA NTRS2020

Global-scale distribution of ozone in the remote troposphere from ATom and HIPPO airborne field missions

Ozone is a key constituent of the troposphere, where it drives photochemical processes, impacts air quality, and acts as a climate forcer. Large-scale in situ observations of ozone commensurate with the grid resolution of current Earth system models are necessary to validate model outputs and satellite retrievals. In this paper, we examine measurements from the Atmospheric Tomography (ATom; four deployments in 2016–2018) and the HIAPER Pole-to-Pole Observations (HIPPO; five deployments in 2009–2011) experiments, two global-scale airborne campaigns covering the Pacific and Atlantic basins. ATom and HIPPO represent the first global-scale, vertically resolved measurements of O3 distributions throughout the troposphere, with HIPPO sampling the atmosphere over the Pacific and ATom sampling both the Pacific and Atlantic. Given the relatively limited temporal resolution of these two campaigns, we first compare ATom and HIPPO ozone data to longer-term observational records to establish the representativeness of our dataset. We show that these two airborne campaigns captured on average 53 %, 54 %, and 38 % of the ozone variability in the marine boundary layer, free troposphere, and upper troposphere–lower stratosphere (UTLS), respectively, at nine well-established ozonesonde sites. Additionally, ATom captured the most frequent ozone concentrations measured by regular commercial aircraft flights in the northern Atlantic UTLS. We then use the repeated vertical profiles from these two campaigns to confirm and extend the existing knowledge of tropospheric ozone spatial and vertical distributions throughout the remote troposphere. We highlight a clear hemispheric gradient, with greater ozone in the Northern Hemisphere, consistent with greater precursor emissions and consistent with previous modeling and satellite studies. We also show that the ozone distribution below 8 km was similar in the extra-tropics of the Atlantic and Pacific basins, likely due to zonal circulation patterns. However, twice as much ozone was found in the tropical Atlantic as in the tropical Pacific, due to well-documented dynamical patterns transporting continental air masses over the Atlantic. Finally, we show that the seasonal variability of tropospheric ozone over the Pacific and the Atlantic basins is driven year-round by transported continental plumes and photochemistry, and the vertical distribution is driven by photochemistry and mixing with stratospheric air. This new dataset provides additional constraints for global climate and chemistry models to improve our understanding of both ozone production and loss processes in remote regions, as well as the influence of anthropogenic emissions on baseline ozone.

ATom, aircraft profiles, Atlantic pollution, ozone↗
NASA NTRS2023

Arctic Tropospheric Ozone: Assessment of Current Knowledge and Model Performance

As the third most important greenhouse gas (GHG) after carbon dioxide (CO2) and methane (CH4), tropospheric ozone (O3) is also an air pollutant causing damage to human health and ecosystems. This study brings together recent research on observations and modeling of tropospheric O3 in the Arctic, a rapidly warming and sensitive environment. At different locations in the Arctic, the observed surface O3 seasonal cycles are quite different. Coastal Arctic locations, for example, have a minimum in the springtime due to O3 depletion events resulting from surface bromine chemistry. In contrast, other Arctic locations have a maximum in the spring. The 12 state-of-the-art models used in this study lack the surface halogen chemistry needed to simulate coastal Arctic surface O3 depletion in the springtime; however, the multi-model median (MMM) has accurate seasonal cycles at non-coastal Arctic locations. There is a large amount of variability among models, which has been previously reported, and we show that there continues to be no convergence among models or improved accuracy in simulating tropospheric O3 and its precursor species. The MMM underestimates Arctic surface O3 by 5 % to 15 % depending on the location. The vertical distribution of tropospheric O3 is studied from recent ozonesonde measurements and the models. The models are highly variable, simulating free-tropospheric O3 within a range of ±50 % depending on the model and the altitude. The MMM performs best, within ±8 % for most locations and seasons. However, nearly all models overestimate O3 near the tropopause (∼300 hPa or ∼8 km), likely due to ongoing issues with underestimating the altitude of the tropopause and excessive downward transport of stratospheric O3 at high latitudes. For example, the MMM is biased high by about 20 % at Eureka. Observed and simulated O3 precursors (CO, NOx, and reservoir PAN) are evaluated throughout the troposphere. Models underestimate wintertime CO everywhere, likely due to a combination of underestimating CO emissions and possibly overestimating OH. Throughout the vertical profile (compared to aircraft measurements), the MMM underestimates both CO and NOx but overestimates PAN. Perhaps as a result of competing deficiencies, the MMM O3 matches the observed O3 reasonably well. Our findings suggest that despite model updates over the last decade, model results are as highly variable as ever and have not increased in accuracy for representing Arctic tropospheric O3.

Arctic↗
NASA NTRS2008

Impact of Surface Emissions to the Zonal Variability of Tropical Tropospheric Ozone and Carbon Monoxide for November 2004

The chemical and dynamical processes governing the zonal variability of tropical tropospheric ozone and carbon monoxide are investigated for November 2004 using satellite observations, in-situ measurements, and chemical transport models in conjunction with inverse-estimated surface emissions. Vertical ozone profile estimates from the Tropospheric Emission Spectrometer (TES) and ozone sonde measurements from the Southern Hemisphere Additional Ozonesondes (SHADOZ) network show the so called zonal 'wave-one' pattern, which is characterized by peak ozone concentrations (70-80 ppb) centered over the Atlantic, as well as elevated concentrations of ozone over Indonesia and Australia (60-70 ppb) in the lower troposphere. Observational evidence from TES CO vertical profiles and Ozone Monitoring Instrument (OMI) NO2 columns point to regional surface emissions as an important contributor to the elevated ozone over Indonesia. This contribution is investigated with the GEOS-Chem chemistry and transport model using surface emission estimates derived from an optimal inverse model, which was constrained by TES and Measurements Of Pollution In The Troposphere (MOPITT) CO profiles (Jones et al., 2007). These a posteriori estimates, which were over a factor of 2 greater than climatological emissions, reduced differences between GEOS-Chem and TES ozone observations by 30-40% and led to changes in GEOS-Chem upper tropospheric ozone of up to 40% over Indonesia. The remaining residual differences can be explained in part by upper tropospheric ozone produced from lightning NOx in the South Atlantic. Furthermore, model simulations from GEOS-Chem indicate that ozone over Indonesian/Australian is more sensitive to changes in surface emissions of NOx than ozone over the tropical Atlantic.

tropical tropospheric ozone↗