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NASA NTRS2000

Model Study of the Sources of Upper Tropospheric Ozone Over The Atlantic, with Emphasis on Interhemispheric Asymmetries

Measurements of ozone and aerosols from ships transecting the Atlantic Ocean reveal considerable interhemispheric asymmetries in the vertical structure of the ozone distribution. There is much more upper tropospheric ozone to the South of the Equator than in the northern hemisphere. These profiles suggest that the air in the southern hemispheric tropics and subtropics has a source in the stratosphere, while that in the northern hemisphere originates in the boundary layer. A model experiment designed to investigate this problem will be discussed. They are based on a new general circulation model, based on a Finite-Volume dynamical core and the physical parametrizations from the Community Climate Model at the National Center for Atmospheric Research (NCAR). The model simulates a climatological state in reasonable agreement with observations, comparable to other contemporary climate models, but has a much more accurate transport capability than most other present-day models. The experiment involves using a suite of tracers, designed to highlight air from different source regions. Some of these (water vapor and ozone) represent real atmospheric quantities, while others are markers which indicate whether the air originates in the stratosphere, the boundary layer, or has traversed regions of convection (for example). The experiments were run for periods of up to one month, initialized from snapshots from a long climate integration of the model. A sample of results will be presented, chosen to illustrate the different sources of air in the upper troposphere and the physical mechanisms by which these air parcels arrived there.

Pawson, Steven↗

NASA NTRS2000

Dominant Presence of Oxygenated Organic Species in the Remote Southern Hemisphere Troposphere

Oxygenated organic species are intimately involved with the fate of nitrogen oxides (NO(sub x)) and hydrogen oxides (HO(sub x)), which are necessary for tropospheric ozone formation. A recent airborne experiment (March-April, 1999) focused over the southern hemisphere (SH) Pacific Ocean (PEM-tropics-B) provided a first opportunity for a detailed characterization of the oxygenated organic composition of the remote southern hemisphere troposphere. Three co-located multi-channel airborne instruments measured a dozen key oxygenated species (carbonyls, alcohols, organic nitrates, organic pernitrates, peroxides) along with a comprehensive suite of C2-C8 Nonmethane hydrocarbons (NMHC). These measurements reveal that in the tropical SH (0-30 deg south), oxygenated chemical abundances are extremely large and collectively are nearly five times those of NMHC. Even in the NH remote atmospheres their burden is equal to or greater than that of NMHC. The relatively uniform global distribution oxygenates (EPSILON Ox-org) is indicative of the presence of large natural and distributed sources. A global 3-D model, reflecting the present state of science, is unable to correctly simulate the atmospheric distribution and variability of several of these species.

Singh, H.↗

NASA NTRS2000

Compendium of NASA Data Base for the Global Tropospheric Experiment's Pacific Exploratory Mission-Tropics B (PEM-Tropics B): DC-8 - Volume 1

This report provides a compendium of NASA aircraft data that are available from NASA's Global Tropospheric Experiment's (GTE) Pacific Exploratory Mission-Tropics B (PEM-Tropics B) conducted in March and April 1999. PEM-Tropics B was conducted during the southern-tropical wet season when the influence from biomass burning observed in PEM-Tropics A was minimal. Major deployment sites were Hawaii, Kiritimati (Christmas Island), Tahiti, Fiji, and Easter Island. The broad goals of PEM-Tropics B were to improved understanding of the oxidizing power of the atmosphere and the processes controlling sulfur aerosol formation and to establish baseline values for chemical species that are directly coupled to the oxidizing power and aerosol loading of the troposphere. The purpose of this document is to provide a representation of aircraft data that will be available in archived format via NASA Langley's Distributed Active Archive Center (DAAC) or are available through the GTE Project Office archive. The data format is not intended to support original research/analysis, but to assist the reader in identifying data that are of interest.

Scott, A. Donald, Jr.↗

NASA NTRS2000

Compendium of NASA Data Base for the Global Tropospheric Experiment's Pacific Exploratory Mission - Tropics B (PEM-Tropics B): P-3B - Volume 2

Scott, A. Donald, Jr.↗

NASA NTRS2000

Evaluation of Upper-Tropospheric and Lower-Stratospheric Ozone Profiles from a Global Ozone Data Assimilation System

The Data Assimilation Office at NASA's Goddard Space Flight Center provides global 3D ozone fields at six-hour time intervals. Data from Total Ozone Mapping Spectrometer (TOMS) and the Solar Backscatter Ultraviolet (SBUV) instrument are used in the assimilation. TOMS provides total column information and SBUV provides profile information, primarily above the ozone peak. Information below the ozone peak comes from the model. This paper will explore the realism of the assimilated ozone in the upper troposphere and lower stratosphere through validation with ozonesondes, Halogen Occultation Experiment (HALOE), and Polar Ozone and Aerosol Measurement (POAM) observations. This work is in preparation of using the assimilated ozone in the radiative calculation for the meteorological assimilation as well as in the derivation of tropospheric ozone.

Rood, Richard B.↗

NASA NTRS2001

Investigation of the Physical Processes Governing Large-Scale Tracer Transport in the Stratosphere and Troposphere

This report summarizes work conducted from January 1996 through April 1999 on a program of research to investigate the physical mechanisms that underlie the transport of trace constituents in the stratosphere-troposphere system. The primary scientific goal of the research has been to identify the processes which transport air masses within the lower stratosphere, particularly between the tropics and middle latitudes. This research was conducted in collaboration with the Subsonic Assessment (SASS) of the NASA Atmospheric Effects of Radiation Program (AEAP) and the Upper Atmospheric Research Program (UARP). The SASS program sought to understand the impact of the present and future fleets of conventional jet traffic on the upper troposphere and lower stratosphere, while complementary airborne observations under UARP seek to understand the complex interactions of dynamical and chemical processes that affect the ozone layer. The present investigation contributed to the goals of each of these by diagnosing the history of air parcels intercepted by NASA research aircraft in UARP and AEAP campaigns. This was done by means of a blend of trajectory analyses and tracer correlation techniques.

Selkirk, Henry B.↗

NASA NTRS2001

Troposphere-Stratosphere Dynamic Coupling Under Strong and Weak Polar Vortex Conditions

The relationship between Northern Hemisphere (NH) tropospheric and stratospheric wave-like anomalies of spherical zonal wave number (ZWN) 1 is studied by applying Canonical Correlation Analysis (CCA). A lag-correlation technique is used with 10-day lowpass filtered daily time series of 50- and 500-hPa geopotential heights. Generally stratospheric circulation is determined by ultralong tropospheric planetary waves. During winter seasons characterized either by any anomalously strong or weak polar winter vortex different propagation characteristics for waves of ZWN 1 are observed. The non-linear perspective of the results have implications for medium range weather forecast and climate sensitivity experiments.

Perlwitz, Judith↗

NASA NTRS1999

On the Accuracy of In Situ Water Vapor Measurements in the Troposphere and Lower Stratosphere with the Harvard Lyman-Alpha Hygrometer

In an effort to better constrain atmospheric water vapor mixing ratios and to understand the discrepancies between different measurements of water vapor in the stratosphere and troposphere, we have carefully examined data from the Harvard Lyman-alpha photofragment fluorescence hygrometer, which has flown on the NASA ER-2 aircraft from 1992 through 1998. The instrument is calibrated in the laboratory before and after each deployment, and the calibration is checked by direct absorption measurements in the troposphere. On certain flights, the ER-2 flew level tracks during which water vapor varied by up to 80 ppmv, under nearly constant atmospheric conditions. These flights provide a stringent test of our calibration via direct absorption and indicate agreement to within 3%. During the 1997 Photochemistry of Ozone Loss in the Arctic Region In Summer (POLARIS) mission, our Lyman-alpha instrument was compared with a new diode laser hygrometer from the Jet Propulsion Laboratory. Overall agreement was 5% during the June/July deployment and 1% for potential temperatures of 490 to 540 K. The accuracy of our instrument is shown to be +/-5 %, with an additional offset of at most 0.1 ppmv. Data from this instrument, combined with simultaneous measurements of CH4, and H2, are therefore ideal for studies of the hydrogen budget of the lower stratosphere.

Hintsa, Eric J.↗

NASA NTRS2001

Tropospheric Formaldehyde Measurements from the ESA GOME Instrument

The Global Ozone Monitoring Experiment (GOME) was launched on the European Space Agency's ERS-2 satellite on April 20, 1995. GOME measures the Earth's atmosphere in the nadir geometry, using a set of spectrometers that cover the UV and visible (240-790 nm) at moderate resolution (0.2 nm in the UV, 0.4 nm in the visible), employing silicon diode array detectors. GOME takes some 30,000 spectra per day, obtaining full global coverage in three days. We directly fit GOME radiance spectra using nonlinear least-squares analysis to obtain column amounts of several trace species with significant tropospheric concentrations, including ozone (O3), nitrogen dioxide (NO2), sulfur dioxide (SO2), and formaldehyde (HCHO). Measurements of HCHO due to biogenic activity in the troposphere are presented here.

Chance, K.↗

NASA NTRS1994

Acetone in theGlobal Troposphere: Its Possible Role as a Global Source of PAN

Oxygenated hydrocarbons are thought to be important components of the atmosphere but, with the exception of formaldehyde, very little about their distribution and fate is known. Aircraft measurements of acetone (CH3COCH3), PAN (CH3CO3NO2) and other organic species (e. g. acetaldehyde, methanol and ethanol) have been performed over the Pacific, the southern Atlantic, and the subarctic atmospheres. Sampled areas extended from 0 to 12 km altitude over latitudes of 70 deg N to 40 deg S. All measurements are based on real time in-situ analysis of cryogenically preconcentrated air samples. Substantial concentrations of these oxygenated species (10-2000 ppt) have been observed at all altitudes and geographical locations in the troposphere. Important sources include, emissions from biomass burning, plant and vegetation, secondary oxidation of primary non-methane hydrocarbons, and man-made emissions. Direct measurements within smoke plumes have been used to estimate the biomass burning source. Photochemistry studies are used to suggest that acetone could provide a major source of peroxyacetyl radicals in the atmosphere and play an important role in sequestering reactive nitrogen. Model calculations show that acetone photolysis contributes significantly to PAN formation in the middle and upper troposphere.

Singh, H. B.↗

NASA NTRS2000

Factors Controlling Upper-Troposphere Water Vapor

The seasonal changes of the upper-tropospheric humidity are studied with the water vapor data from the Microwave Limb Sounder on the National Aeronautics and Space Administration's Upper Atmosphere Research Satellite and the winds and vertical velocity data obtained from the European Centre for Medium-Range Weather Forecasts. Using the same algorithm for vertical transport as that used for horizontal transport (by Zhu and Newell), the authors find that the moisture in the tropical upper troposphere may be increased mainly by intensified local convection in a small portion, less than 10%, of the whole area between 40 degrees S and 40 degrees N. The contribution of large-scale background circulations and divergence of horizontal transport is relatively small in these regions. These dynamic processes cannot be revealed by the traditional analyses of moisture fluxes. The negative response suggested by Lindzen, with enhanced convection in the Tropics being accompanied by subsidence drying in the subtropics, also exists, but the latter does not apparently dominate in the moisture budget.

Zhu, Yong↗

NASA NTRS2002

In-Situ Measurements of HCN and CH3CN in the Pacific Troposphere: Sources, Sinks, and Comparisons with Spectroscopic Observations

We report the first in-situ measurements of hydrogen cyanide (HCN) and acetonitrile (CH3CN) from the Pacific troposphere (0-12 km) obtained during the NASA/Trace-P mission (Feb.-April, 2001). Mean HCN and CH3CN mixing ratios of 243 (+/-118) ppt and 149 (+/-56) ppt respectively, were measured. The in-situ observations correspond to a total HCN column of 4.4-4.9 x 10(exp 15) molec. cm(exp -2) and a CH3CN column of 2.8-3.0 x 10(exp 15) molec. cm(exp -2). This HCN column is in good agreement with available spectroscopic observations. The atmospheric concentrations of HCN and CH3CN were greatly influenced by outflow of pollution from Asia. There is a linear relationship between the mixing ratios of HCN and CH3CN, and in turn these are well correlated with tracers of biomass combustion (e.g. CH3Cl, CO). Relative enhancements with respect to known tracers of biomass combustion within selected plumes in the free troposphere, and pollution episodes in the boundary layer allow an estimation of a global biomass burning source of 0.8+/-0.4 Tg (N)/y for HCN and 0.4+/-0.1 Tg (N)/y for CH3CN. In comparison, emissions from automobiles and industry are quite small (<0.05 Tg (N)/y). The vertical structure of HCN and CH3CN indicated reduced mixing ratios in the MBL (Marine Boundary Layer). Using, a simple box model, the observed gradients across the top of the MBL are used to derive an oceanic flux of 6.7 x 10(exp -15) g (N) cm(exp -2)/s for HCN and 4.8 x 10(exp -15) g (N) cm(exp -2)/s for CH3CN. An air-sea exchange model is used to conclude that this flux can be maintained if the oceans are under-saturated in HCN and CH3CN by 23% and 17%, respectively. It is inferred that oceanic loss is a dominant sink for these nitrites, and they deposit some 1.3 Tg (N) of nitrogen annually to the oceans. Assuming reaction with OH radicals and loss to the oceans as the major removal processes, a mean atmospheric residence time of 4.7 months for HCN and 5.1 months for CH3CN is calculated. A global budget analysis shows that the sources and sinks of HCN and CH3CN are roughly in balance. There are indications that biogenic sources may also be present. Mechanisms involved in nitrate formation during combustion and removal in the oceans are poorly understood.

Singh, Hanwant B.↗

NASA NTRS2002

Derivation of Tropospheric Ozone Climatology and Trends from TOMS Data

This research addresses the following three objectives: (1) Derive tropospheric ozone columns from the TOMS instruments by computing the difference between total-ozone columns over cloudy areas and over clear areas in the tropics; (2) Compute secular trends in Nimbus-7 derived tropospheric Ozone column amounts and associated potential trends in the decadal-scale tropical cloud climatology; (3) Explain the occurrence of anomalously high ozone retrievals over high ice clouds.

Newchurch, Michael J.↗

NASA NTRS2003

A Climatology of Tropospheric CO over the Central and Southeastern United States and the Southwestern Pacific Ocean Derived from Space, Air, and Ground-based Infrared Interferometer Spectra

This final report summarizes all research activities and publications undertaken as part of NASA Atmospheric Chemistry and Modeling Analysis Program (ACMAP) Grant NAG-1-2022, 'A Climatology of Tropospheric CO over the Central and Southeastern United States and the Southwestern Pacific Ocean Derived from Space, Air, and Ground-based Infrared Interferometer Spectra'. Major project accomplishments include: (1) analysis of more than 300,000 AERI spectra from the ARM SGP site yielding a 5-year (1998-2002) timeseries of CO retrievals from the Lamont, OK AERI; (2) development of a prototype CO profile retrieval algorithm for AERI spectra; (3) validation and publication of the first CO retrievals from the Scanning High-resolution Interferometer Sounder (SHIS); and (4) development of a prototype AERI tropospheric O3 retrieval algorithm. Compilation and publication of the 5-year Lamont, OK timeseries is underway including a new collaboration with scientists at the Lawrence Berkeley National Laboratory. Public access to this data will be provided upon article submission. A comprehensive CO analysis of the archive of HIS spectra of remains as the only originally proposed activity with little progress. The greatest challenge faced in this project was motivating the University of Wisconsin Co-Investigators to deliver their archived HIS and AERIOO data along with the requisite temperature and water vapor profiles in a timely manner. Part of the supplied HIS dataset from ASHOE may be analyzed as part of a Master s Thesis under a separate project. Our success with the SAFARI 2000 SHIS CO analysis demonstrates the utility of such aircraft remote sensing data given the proper support from the instrument investigators. In addition to the PI and Co-I s, personnel involved in this CO climatology project include one Post Doctoral Fellow, one Research Scientist, two graduate students, and two undergraduate students. A total of fifteen presentations regarding research related to this project were delivered at eleven different scientific meetings. Thus far, three publications have resulted from this project with another five in preparation. No subject inventions resulted from this research project.

McMillian, W. Wallace↗

NASA NTRS2003

The Role of Wave Cyclones in Transporting Boundary Layer Air to the Free Troposphere During the Spring 2001 NASA / TRACE-P Experiment

Transport of boundary layer air to the free troposphere by cyclones during NASA's Transport and Chemical Evolution over the Pacific (TRACE-P) experiment is investigated. Airstreams responsible for boundary layer venting are diagnosed using results from a high-resolution meteorological model (MM5) together with in situ and remotely sensed chemical data. Hourly wind data from the MM5 are used to calculate three-dimensional grids of backward air trajectories. A reverse domain filling (RDF) technique then is employed to examine the characteristics of airstreams over the computational domain, and to isolate airstreams ascending from the boundary layer to the free troposphere during the previous 36 hours. Two cases are examined in detail. Results show that airstreams responsible for venting the boundary layer differ considerably from those described by classic conceptual models and in the recent literature. In addition, airstreams sampled by the TRACE-P aircraft are found to exhibit large variability in chemical concentrations. This variability is due to differences in the boundary layer histories of individual airstreams with respect to anthropogenic sources over continental Asia and Japan. Complex interactions between successive wave cyclones also are found to be important in determining the chemical composition of the airstreams. Particularly important is the process of post-cold frontal boundary layer air being rapidly transported offshore and recirculated into ascending airstreams of upstream cyclones.

Fuelberg, Henry E.↗

NASA NTRS2003

The Correlation Between Tropical Convection and Upper Tropospheric Momentum Flux Convergence

In this study, the relationship between tropical convection and the meridional convergence of zonal momentum flux in the tropical upper troposphere is investigated using NOAA interpolated outgoing longwave radiation data and NCEP-NCAR reanalysis wind data. In particular, a variety of correlation coefficients are calculated between the data sets, both of which are filtered to isolate disturbances with frequencies and wavenumbers consistent with the Madden-Julian oscillation. The results show regions of significant correlation during each season, with the magnitude and area covered by significant correlation coefficients varying with season. Furthermore, it is found that the correlation structures look very similar to theoretical calculations of the atmospheric response to a region of tropical heating. This result suggests that tropical waves, in particular mixed Rossby-gravity waves, play an important role in the meridional transport zonal momentum into the deep tropical upper troposphere. Finally, these findings have implications to the generation of rising motion near the tropical tropopause, which in turn has ramifications for vertical moisture transport and tropopause cirrus formation.

O'CStarr, David↗

NASA NTRS2003

SPARC-IGAC Symposium on Climate-Chemistry Interactions. Climate Feedback by Water Vapor in the Tropical Upper Troposphere

The strong greenhouse forcing by atmospheric water vapor is expected to play an important role in shaping the direction of any future changes in climate. We present calculations that provide a new perspective on the sensitivity of upper tropospheric water vapor to changes in surface temperature. Equilibrium states of our atmospheric model show unambiguously that as the surface warms, changes in the vertical distribution and temperature of detraining air parcels from tropical convection lead to higher water vapor mixing ratios in the upper troposphere. However, the increase in mixing ratio is not as large as the increase in saturation mixing ratio due to warmer environmental temperatures, so that the relative humidity decreases. Our analysis suggests that models that maintain a fixed relative humidity are likely overestimating the magnitude of the water vapor feedback.

Dessler, A. E.↗

NASA NTRS2003

Sensitivity of Middle Atmospheric Temperature and Circulation in the UIUC Mesosphere-Stratosphere-Troposphere GCM to the Treatment of Subgrid-Scale Gravity-Wave Breaking

The sensitivity of the middle atmospheric temperature and circulation to the treatment of mean- flow forcing due to breaking gravity waves was investigated using the University of Illinois at Urbana-Champaign 40-layer Mesosphere-Stratosphere-Troposphere General Circulation Model (MST-GCM). Three GCM experiments were performed. The gravity-wave forcing was represented first by Rayleigh friction, and then by the Alexander and Dunkerton (AD) parameterization with weak and strong breaking effects of gravity waves. In all experiments, the Palmer et al. parameterization was included to treat the breaking of topographic gravity waves in the troposphere and lower stratosphere. Overall, the experiment with the strong breaking effect simulates best the middle atmospheric temperature and circulation. With Rayleigh friction and the weak breaking effect, a large warm bias of up to 60 C was found in the summer upper mesosphere and lower thermosphere. This warm bias was linked to the inability of the GCM to simulate the reversal of the zonal winds from easterly to westerly crossing the mesopause in the summer hemisphere. With the strong breaking effect, the GCM was able to simulate this reversal, and essentially eliminated the warm bias. This improvement was the result of a much stronger meridional transport circulation that possesses a strong vertical ascending branch in the summer upper mesosphere, and hence large adiabatic cooling. Budget analysis indicates that 'in the middle atmosphere the forces that act to maintain a steady zonal-mean zonal wind are primarily those associated with the meridional transport circulation and breaking gravity waves. Contributions from the interaction of the model-resolved eddies with the mean flow are small. To obtain a transport circulation in the mesosphere of the UIUC MST-GCM that is strong enough to produce the observed cold summer mesopause, gravity-wave forcing larger than 100 m/s/day in magnitude is required near the summer mesopause. In the tropics, only with the AD parameterization can the model produce realistic semiannual oscillations.

Yang, Fanglin↗