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NASA NTRS1997

Chemical Characteristics of Continental Outflow from Asia to the Troposphere Over the Western Pacific Ocean during February - March 1994: Results from PEM-West B

We present here the chemical composition of outflow from the Asian continent to the atmosphere over the western Pacific basin during the Pacific Exploratory Mission-West (PEM-West B) in February-March 1994. Comprehensive measurements of important tropospheric trace gases and aerosol particulate matter were performed from the NASA DC-8 airborne laboratory. Backward 5 day isentropic trajectories were used to partition the outflow from two major source regions- continental north (greater than 20 deg N) and continental south (less than 20 deg N). Air parcels that had not passed over continental areas for the previous 5 days were classified as originating from an aged marine source. The trajectories and the chemistry together indicated that there was extensive rapid outflow of air parcels at altitudes below 5 km, while aged marine air was rarely encountered and only at less than 20 deg N latitude. The outflow at low altitudes had enhancements in common industrial solvent vapors such as C2Cl4, CH3CCl3, and C6H6, intermixed with the combustion emission products C2H2, C2H6, CO, and NO. The mixing ratios of all species were up to tenfold greater in outflow from the continental north compared to the continental south source region, with Pb-210 concentrations reaching 38 fCi (10(exp -15) curies) per standard cubic meter. In the upper troposphere we again observed significant enhancements in combustion-derived species in the 8-10 km altitude range, but water-soluble trace gases and aerosol species were depleted. These observations suggest that ground level emissions were lofted to the upper troposphere by wet convective systems which stripped water-soluble components from these air parcels. There were good correlations between C2H2 and CO and C2H6 (r(sup 2) = 0.70 - 0.97) in these air parcels and much weaker ones between C2H2 and H2O2 or CH3OOH (r(sup 2) = 0.50). These correlations were the strongest in the continental north outflow where combustion inputs appeared to be recent (1 - 2 days old). Ozone and PAN showed general correlation in these same air parcels but not with the combustion products. It thus appears that several source inputs were intermixed in these upper tropospheric air masses, with possible contributions from European or Middle Eastern source regions. In aged marine air mixing ratios of 03 (approximately equals 20 parts per billion by volume) and PAN (less than or equal to 10 parts per trillion by volume) were nearly identical at less than 2 km and 10 - 12 km altitudes due to extensive convective uplifting of marine boundary layer air over the equatorial Pacific even in wintertime. Comparison of the Pacific Exploratory Mission-West A and PEM-West B data sets shows significantly larger mixing ratios of SO2 and H2O2 during PEM-West A. Emissions from eruption of Mount Pinatubo are a likely cause for the former, while suppressed photochemical activity in winter was probably responsible for the latter. This comparison also highlighted the twofold enhancement in C2H2, C2H6, and C3H8 in the continental north outflow during /PEM-West B. Although this could be due to reduced OH oxidation rates of these species in wintertime, we argue that increased source emissions are primarily responsible.

Talbot, R. W.↗
NASA NTRS1998

Tropical Tropospheric Ozone (TTO) Maps from Nimbus 7 and Earth-Probe TOMS by the Modified-Residual Method: Validation, Evaluation and Trends based on Atlantic Regional Time Series - 1

The well-known wave-one pattern seen in tropical total ozone [Shiotani, 1992; Ziemke et al., 1996, 1998] has been used to develop a modified-residual (MR) method for retrieving time-averaged stratospheric ozone and tropospheric ozone column amount from TOMS (Total Ozone Mapping Spectrometer) over the 14 complete calendar years of Nimbus 7 observations (1979-1992) and from TOMS on the Earth-Probe (1996-present) and ADEOS platforms (1996- 1997). Nine- to sixteen-day averaged tropical tropospheric ozone (TTO) maps, validated with ozonesondes, show a seasonality expected from dynamical and chemical influences. The maps may be viewed on a homepage: http://metosrv2.umd.edu/~tropo. Stratospheric column ozone, which is also derived by the modified-residual method, compares well with sondes (to within 6-7 DU) and with stratospheric ozone column derived from other satellites (within 8-10 DU). Validation of the TTO time-series is presently limited to ozonesonde comparisons with Atlantic stations and sites on the adjacent continents (Ascension Island, Natal, Brazil; Brazzaville); for the sounding periods, TTO at all locations agrees with the sonde record to +/-7 DU. TTO time-series and the magnitude of the wave-one pattern show ENSO signals in the strongest El Nifio periods from 1979-1998. From 12degN and 12degS, zonally averaged tropospheric ozone shows no significant trend from 1980-1990. Trends are also not significant during this period in localized regions, e.g. from just west of South America across to southern Africa. This is consistent with the ozonesonde record at Natal, Brazil (the only tropical ozone data publicly available for the 1980's), which shows a not statistically significant increase. The lack of trend in tropospheric ozone agrees with a statistical analysis based on another method for deriving TTO from TOMS, the so-called Convective-Cloud-Differential approach of Ziemke et al. [1998].

Thompson, Anne M.↗
NASA NTRS1999

Physical and Chemical Characterization of Particles in the Upper Troposphere and Lower Stratosphere: Microanalysis of Aerosol Impactor Samples

Herein is reported activities to support the characterization of the aerosol in the upper troposphere (UT) and lower stratosphere (LS) collected during the Airborne Southern Hemisphere Ozone Experiment/Measurements for Assessing the Effects of Stratospheric Aircraft (ASHOE/MAESA) missions in 1994. Through a companion proposal, another group was to measure the size distribution of aerosols in the 0.008 to 2 micrometer diameter range and to collect for us impactor samples of particles larger than about 0.02 gm. In the first year, we conducted laboratory studies related to particulate deposition patterns on our collection substrates, and have performed the analysis of many ASHOE/MAESA aerosol samples from 1994 using analytical electron microscopy (AEM). We have been building an "aerosol climatology" with these data that documents the types and relative abundances of particles observed at different latitudes and altitudes. The second year (and non-funded extension periods) saw continued analyses of impactor aerosol samples, including more ASHOE/MAESA samples, some northern hemisphere samples from the NASA Stratospheric Photochemistry Aerosols and Dynamics Expedition (SPADE) program for comparison, and a few aerosol samples from the NASA Stratospheric TRacers of Atmospheric Transport (STRAT) program. A high-resolution field emission microscope was used for the analysis and re-analysis of a number of samples to determine if this instrument was superior in performance to our conventional electron microscope. In addition, some basic laboratory studies were conducted to determine the minimum detectable and analyzable particle size for different types of aerosols. In all, 61 aerosol samples were analyzed, with a total of over 30,000 individual particle analyses. In all analyzed samples, sulfate particles comprised the major aerosol number fraction. It must be stressed that particles composed of more than one species, for example sulfate and organic carbon, were classified according to the major fraction. Thus, many of the particles classified as sulfate may have contained significant mass fractions of carbonaceous or other material. These particles for the most part did not show two physical phases, however. Nonsulfate particles were classified according to the physical and chemical characteristics of each particle, and were grouped into the major nonsulfate particle classes, including C-rich, crustal, metallic, and salts. Our UT and LS sample analyses indicate a maximum for crustal and C-rich particle abundance in the Northern Hemisphere upper troposphere, and a salt particle maximum in the Southern Hemisphere upper troposphere. Metallic particles are clearly more prevalent in the troposphere than in the stratosphere, but interhemispheric differences appear small.

Sheridan, Patrick J.↗
NASA NTRS1999

The Tropical Upper Troposphere and Lower Stratosphere in the GEOS-2 GCM

The structure of the tropical upper troposphere and lower stratosphere in the GEOS-2 General Circulation Model (GCM) is discussed. The emphasis of this study is on the reality of monthly-mean temperature and water vapor distributions in the model, compared to reasonable observational estimates. It is shown that although the zonal-mean temperature is in good agreement with observations, the GCM supports an excessive zonal asymmetry near the tropopause compared to the ECMWF Reanalyses. In reality there is a QBO-related variability in the zonally averaged lower stratospheric temperature which is not captured by the model. The observed upper tropospheric temperature and humidity fields show variations related to those in the sea surface temperature, which are not incorporated in the GCM; nevertheless, there is some interannual variability in the GCM, indicating a component arising from internal processes. The model is too moist in the middle troposphere (500 hPa) but too dry in the upper troposphere, suggesting that there is too little vertical transport or too much drying in the GCM. Transport into the stratosphere shows a pronounced annual cycle, with drier air entering the tropical stratosphere when the tropopause is coldest in northern winter; while the alternating dry and moist air masses can be traced ascending through the tropical lower stratosphere, the progression of the anomalies is too rapid.

Pawson, S.↗
NASA NTRS1998

Troposphere-to-Stratosphere Transport in the Lowermost Stratosphere from Measurements of H2O, CO2, N2O and O3

The origin of air in the lowermost stratosphere is investigated with measurements from the NASA ER-2 aircraft. Air with high water vapor mixing ratios was observed in the stratosphere at theta about 330-380 K near 40N in May 1995, indicating the influence of intrusions of tropospheric air. Assuming that observed tracer-tracer relationships reflect mixing lines between tropospheric and stratospheric air masses, we calculate mixing ratios of H2O (12-24 ppmv) and CO2 for the admixed tropospheric air at theta =352-364 K. Temperatures on the 355 K surface at 20-40 N were low enough to dehydrate air to these values. while most ER-2 CO2 data in both hemispheres are consistent with tropical or subtropical air entering the lowermost stratosphere, measurements from May 1995 for theta <362 K suggest that entry of air from the midlatitude upper troposphere can occur in conjunction with mixing processes near the tropopause.

Hintsa, E. J.↗
NASA NTRS1998

Troposphere-to-Stratosphere Transport in the Lowermost Stratosphere from Measurements of H2O, CO2, N2O and O3

The origin of air in the lowermost stratosphere is investigated with measurements from the NASA ER-2 aircraft. Air with high water vapor mixing ratios was observed in the stratosphere at theta-330-380 K near 40 N in May 1995, indicating the influence of intrusions of tropospheric air. Assuming that observed tracer-tracer relationships reflect mixing lines between tropospheric and stratospheric air masses, we calculate mixing ratios of H2O (12-24 ppmv) and CO2 for the admixed tropospheric air at theta=352-364 K. Temperatures on the 355 K surface at 20-40 N were low enough to dehydrate air to these values. While most ER-2 CO2 data in both hemispheres are consistent with tropical or subtropical air entering the lowermost stratosphere, measurements from May 1995 for theta<362 K suggest that entry of air from the midlatitude upper troposphere can occur in conjunction with mixing processes near the tropopause.

Hintsa, E. J.↗
NASA NTRS1999

HALOE Algorithm Improvements for Upper Tropospheric Sounding

This report details the ongoing efforts by GATS, Inc., in conjunction with Hampton University and University of Wyoming, in NASA's Mission to Planet Earth UARS Science Investigator Program entitled "HALOE Algorithm Improvements for Upper Tropospheric Soundings." The goal of this effort is to develop and implement major inversion and processing improvements that will extend HALOE measurements further into the troposphere. In particular, O3, H2O, and CH4 retrievals may be extended into the middle troposphere, and NO, HCl and possibly HF into the upper troposphere. Key areas of research being carried out to accomplish this include: pointing/tracking analysis; cloud identification and modeling; simultaneous multichannel retrieval capability; forward model improvements; high vertical-resolution gas filter channel retrievals; a refined temperature retrieval; robust error analyses; long-term trend reliability studies; and data validation. The current (first-year) effort concentrates on the pointer/tracker correction algorithms, cloud filtering and validation, and multi-channel retrieval development. However, these areas are all highly coupled, so progress in one area benefits from and sometimes depends on work in others.

McHugh, Martin J.↗
NASA NTRS1998

Troposphere-to-Stratosphere Transport in the Lowermost Stratosphere from Measurements of H2O, CO2, N2O, and O3

The origin of air in the lowermost stratosphere is investigated with measurements from the NASA ER-2 aircraft. Air with high water vapor mixing ratios was observed in the stratosphere at theta approximately 330-380 K near 40 N in May 1995, indicating the influence of intrusions of tropospheric air. Assuming that observed tracer-tracer relationships reflect mixing lines between tropospheric and stratospheric air masses, we calculate mixing ratios of H2O (12-24 ppmv) and CO2 for the admixed tropospheric air at theta = 352-364 K. Temperatures on the 355 K surface 20-40 N were low enough to dehydrate air to these values. While most ER-2 CO2 data in both hemispheres are consistent with tropical or subtropical air entering the lowermost stratosphere, measurements from May 1995 for theta < 362 K suggest that entry of air from the midlatitude upper troposphere can occur in conjunction with mixing processes near the tropopause.

Hintsa, E. J.↗
NASA NTRS1999

Remote Sensing of Tropical Tropospheric Ozone: Validation on the R/V R. H. Brown and the SHADOZ (Southern Hemisphere Additional Ozonesondes) Project

This talk will give background on tropical tropospheric ozone studies in the field and from space from the TOMS (Total Ozone Mapping Spectrometer) satellite instrument. Background will be given on why tropospheric ozone in the tropics is of interest to people studying global change and its role in measurements on the R/V R H Brown 1999 Aerosols cruise. The new modified-residual method (Hudson and Thompson, 1998; Thompson and Hudson, 1999) for determining column depth of tropospheric ozone from TOMS will be described. Examples of modified-residual TTO (tropical tropospheric ozone) maps will be shown. These include Earth-Probe TOMS maps of ozone from the 1997 Indonesian fires as well as 14 years of twice-monthly maps from which seasonal and trends behavior can be deduced. The need for validation data for TTO maps has led to establishment of the NASA/NOAA-sponsored SHADOZ network in which 9 tropical nations are participating (Ascension Is., Brazil, Kenya, Indonesia, Fiji, Tahiti, Galapagos, Am. Samoa, Reunion Is. [France]). Some of the R/V Brown ozonesonde data, collected from daily launches on board the ship, from mid-January through mid-february 1999, will be shown.

Thompson, Anne↗
NASA NTRS1999

Tropical Tropospheric Ozone: New Insights from Remote Sensing, Sondes and Field Studies

This talk will summarize our recent research in tropical tropospheric ozone studies in the field and from space. New tropospheric ozone and aerosol products from the TOMS (Total Ozone Mapping Spectrometer) satellite instrument will be highlighted (Hudson and Thompson, 1998; Thompson and Hudson, 1999). These are suitable for studying processes like ozone pollution resulting from biomass fires, seasonal and interannual variations and trends. Archived maps of tropospheric ozone over the tropics, from the Nimbus 7 observing period (1979-1992) are available in digital form at our website: http://metosrv2.umd.edu/-tropo. Real-time processing of TOMS data has produced images of tropical tropospheric ozone (TTO) since early 1997, using Earth-Probe TOMS; these maps are also available on the homepage. The need for validation data for TTO maps has led to establishment of the NASA/NOAA-sponsored SHADOZ (Southern Hemisphere Additional Ozonesondes) network, from which a 2-year record of high-quality ozonesonde data can be obtained: (http://hyperion.gsfc.nasa.gov/Data-services/Shadoz/shadoz-hmpg2.htrnl). Examples will be shown, along with ozonesondes from the January-February 1999 Aerosols-99 cruise of the R/V Ronald H Brown from Virginia to Cape Town, South Africa.

Thompson, Anne M.↗
NASA NTRS1999

Tropical Tropospheric Ozone: New Insights from Remote Sensing and Field Studies

This talk will summarize our recent research in tropical tropospheric ozone studies in the field and from space. New tropospheric ozone and aerosol products from the TOMS (Total Ozone Mapping Spectrometer) satellite instrument will be highlighted (Hudson and Thompson, 1998; Thompson and Hudson, 1999). These are suitable for studying processes like ozone pollution resulting from biomass fires, seasonal and interannual variations and trends. Archived maps of tropospheric ozone over the tropics, from the Nimbus 7 observing period (1979-1992) are available in digital form at our website. Real-time processing of TOMS data has produced images of tropical tropospheric ozone (TTO) since early 1997, using Earth-Probe TOMS; these maps are also available on the homepage.

Thompson, Anne↗
NASA NTRS1999

Biomass Burning Influences on the Composition of the Remote South Pacific Troposphere: Analysis Based on Observations from PEM Tropics-A

Airborne, in-situ measurements from PEM-Tropics-A (September/October 1996) are analyzed to show the presence of distinct pollution plumes in the middle-tropical troposphere of the remote South Pacific (10-30degS). These elevated plumes cause a relative maximum at about 5-7km attitude in the vertical distribution of primary and secondary species characteristic of fuel combustion and biomass burning (CO, C2H2, C2H6, CH3Cl, PAN, O3). Similar plumes were also observed at mid-latitudes in the middle troposphere during three flights east of New Zealand (40-45degS). In all, pollution plumes with CO larger than 100 ppb were observed 24 times on 7 separate flight days south of the equator. The observed plumes were generally embedded in very dry air. Ten-day back trajectory analysis supports the view that these originated from the biomass burning regions of South Africa (and South America) and were transported to the South Pacific along long-distance subsiding trajectories. The chemical composition of the southern Pacific troposphere analyzed from the PEM-Tropics-A data is compared with data from the tropical regions of the northern Pacific (PEM-West-A) and southern Atlantic (TRACE-A) during the same Sept/Oct time period. Sizable perturbations in the abundance of ozone and its key precursors, resulting from the transport of pollution originating from biomass burning sources, are observed in much of the Southern Hemispheric troposphere.

Singh, H. B.↗
NASA NTRS2000

Troposphere-Stratosphere Connections in Recent Northern Winters in NASA GEOS Assimilated Datasets

The northern winter stratosphere displays a wide range of interannual variability, much of which is believed to result from the response to the damping of upward-propagating waves. However, there is considerable (growing) evidence that the stratospheric state can also impact the tropospheric circulation. This issue will be examined using datasets generated in the Data Assimilation Office (DAO) at NASA's Goddard Space Flight Center. Just as the tropospheric circulation in each of these years was dominated by differing synoptic-scale structures, the stratospheric polar vortex also displayed different evolutions. The two extremes are the winter 1998/1999, when the stratosphere underwent a series of warming events (including two major warmings), and the winter 1999/2000, which was dominated by a persistent, cold polar vortex, often distorted by a dominant blocking pattern in the troposphere. This study will examine several operational and research-level versions of the DAO's systems. The 70-level-TRMM-system with a resolution of 2-by-2.5 degrees and the 48-level, 1-by-l-degree resolution ''Terra'' system were operational in 1998/1999 and 1999/2000, respectively. Research versions of the system used a 48-level, 2-by-2.5-degree configuration, which facilitates studies of the impact of vertical resolution. The study includes checks against independent datasets and error analyses, as well as the main issue of troposphere-stratosphere interactions.

Pawson, Steven↗
NASA NTRS2000

Tropospheric Chemistry from Space

Measuring tropospheric chemical constituents from space has been only of the "Holy Grails" of remote sensing. Tropospheric remote sensing has been done in two phases, extracting troposheric constituent information from satellite instruments designed for other purposes and constituent measurements with instruments optimized for tropospheric detection. Examples from the first phase, tropospheric ozone and aerosols from Total Ozone Mapping Spectrometer (TOMS) and Global Ozone Monitoring Experiment (GOME) will be presented. Expected results from upcoming instruments and missions, Atmospheric Ultraviolet Radiance Analyzer (AURA), Ozone Monitoring Instrument (OMI), GOME2, and Scanning Imaging Spectrometer for Atmospheric Chartography (SCIAMACHY) will be presented.

Gleason, James↗
NASA NTRS2000

The Evolution of Tropospheric Temperature Field and its Relationship With The Onset of Asian Summer Monsoon

The mean state and year-to-year variations of the tropospheric temperature fields and their relationship with the establishment of the summertime East Asian monsoon (EAM) and the Indian monsoon (INM) are studied using the NCEP reanalysis data of 15 years (1982-1996). The results show that the seasonal shift of the South Asian High in the upper troposphere and the establishment of the EAM and the INM are closely related to the seasonal warming which causes a reversal of the meridional gradient of upper tropospheric mean temperature over the monsoon regions. On the average of 15 years, the reversal time of the temperature gradient in the EAM region (INM region) is concurrent with (one pentad earlier than) the onset time of the summer monsoon. In most years of the 15-year period, the reversal of temperature gradient coincides or precedes the onset time of the summer monsoon in both the EAM region and the INM region. The results suggest an important role of thermal processes on the establishment of the Asian monsoon. The contributors to the upper tropospheric warming over the EAM region are the strong horizontal warm advection and the diabetic heating against the adiabatic cooling due to upward motion. In the INM region, strong adiabatic heating by subsidence and the diabetic heating are major warming processes against the strong horizontal cold advection related to the persistent northwestlies to the southwestern periphery of the Tibetan Plateau. It appears that the early or late establishment of the Asian summer monsoon is not directly related to the differential warming near the surface.

He, H.↗
NASA NTRS2000

Tropospheric Ozone Profile Information Derived From "Cloud Slicing"

This study introduces a new approach to obtain ozone vertical profile information given coincident satellite measurements of both cloud-top pressure and above-cloud column ozone. This method is denoted "cloud slicing". In this study information of cloud-top pressure is derived from Geostationary Orbital Earth Satellite (GOES) infrared data, while above-cloud column ozone is obtained from the Earth Probe total ozone mapping spectrometer (TOMS) instrument. Several case examples are presented showing the feasibility of this technique as well as providing new geophysical results. Because the TOMS instrument measures backscattered UV radiation, it does detect ozone lying below dense water vapor clouds. This opaque property of TOMS can be used directly in conjunction with co-located cloud-top pressure data to derive ozone profile information in the troposphere. The cloud slicing method is an extension of the "Convective Cloud Differential" (CCD) method. In the CCD method, tropospheric column ozone (i.e., the total vertical column of ozone lying in the troposphere) is computed by taking total column ozone with low reflectivity (R less than 0.2) and subtracting from this a nearby measurement of above-cloud column ozone amount under conditions of high reflectivity (R greater than 0.9). (High reflectivity away from snow/ice conditions coincides with strong convection and tropopause-level clouds). The key element in determining tropospheric ozone profile information from the cloud slicing method is to have simultaneous and co-located measurements of both above-cloud column ozone and cloud-top pressure.

Ziemke, Jerald R.↗
NASA NTRS1998

Troposphere-to-Stratosphere Transport in the Lowermost Stratosphere from Measurements of H2O, CO2, N2O and O3

The origin of air in the lowermost stratosphere is investigated with measurements from the NASA ER-2 aircraft. Air with high water vapor mixing ratios was observed in the stratosphere at theta = 330-380 K near 40 N in May 1995, indicating the influence of intrusions of tropospheric air. Assuming that observed tracer-tracer relationships reflect mixing lines between tropospheric and stratospheric air masses, we calculate mixing ratios of H2O (12-24 ppmv) and CO2 for the admixed tropospheric air at theta = 352-364 K. Temperatures on the 355 K surface at 20-40 N were low enough to dehydrate air to these values. While most ER-2 CO2 data in both hemispheres are consistent with tropical or subtropical air entering the lowermost stratosphere, measurements from May 1995 for theta < 362 K suggest that entry of air from the midlatitude upper troposphere can occur in conjunction with mixing processes near the tropopause.

Hintsa, E. J.↗
NASA NTRS2001

Global Distribution and Sources of Volatile and Nonvolatile Aerosol In the Remote Troposphere

Airborne measurements of aerosol (Condensation Nuclei, CN) and selected trace gases made in the areas of the North Atlantic Ocean during SONEX (October/November 1997), and the south tropical Pacific Ocean during PEM-Tropics A (September/October 1996) and PEM-Tropics B (March/April 1999) have been analyzed. Emphasis is on the interpretations of variations in the number densities of the fine (>17 nm) and ultrafine (>8 nm) CN in the upper troposphere (8-12 km). These data suggest that large number densities of highly volatile CN (10(exp 4)-10(exp 5)/cu cm) are present in the clean upper troposphere with highest values over the tropical1subtropical region. Through marine convection and long-distance horizontal transport, volatile CN originating from the tropical/subtropical regions can frequently impact the abundance of aerosol in the middle and upper troposphere at mid to high latitudes. Nonvolatile aerosol particles behave in a manner similar to tracers of combustion (CO) and photochemical pollution (PAN), implying a source from continental pollution of industrial or biomass burning origin. In the upper troposphere, we find that volatile and nonvolatile partials number densities are inversely correlated. An aerosol microphysical model is used to suggest that coagulation of fine volatile particles with fewer larger nonvolatile particles provides one possible mechanism for this relationship. It appears that nonvolatile particles, of principally anthropogenic origin,provide a highly efficient removal process for the fine volatile aerosol.

Singh, Hanwant B.↗