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At least 235 records · Page 13

Analysis of a 7 year tropospheric ozone vertical distribution at the Observatoire de Haute Provence

A seven year (1984-90) climatology of tropospheric vertical ozone soundings, performed by electrochemical sondes at the OHP (44 deg N, 6 deg E, 700 m ASL) in Southern France, is presented. Its seasonal variation shows a broad spring/summer maximum in the troposphere. The contribution of photochemical ozone production and transport from the stratosphere to this seasonal variation are studied by a correlative analysis of ozone concentrations and meteorological variables, with emphasis on potential vorticity. This analysis shows the impact of dynamical and photochemical processes on the spatial and temporal ozone variability. In particular, a positive correlation (r = 04.0, significance greater than 99.9 percent) of ozone with potential vorticity is observed in the middle troposphere, reflecting the impact of stratosphere-troposphere exchange on the vertical ozone distribution.

Beekmann, Matthias↗

The sensitivity of tropospheric chemistry to cloud interactions

Clouds, although only occupying a relatively small fraction of the troposphere volume, can have a substantial impact on the chemistry of the troposphere. In newly formed clouds, or in clouds with air rapidly flowing through, the chemistry is expected to be far more active than in aged clouds with stagnant air. Thus, frequent cycling of air through shortlived clouds, i.e. cumulus clouds, is likely to be a much more efficient media for altering the composition of the atmosphere than an extensive cloud cover i.e. frontal cloud systems. The impact of clouds is tested out in a 2-D channel model encircling the globe in a latitudinal belt from 30 to 60 deg N. The model contains a detailed gas phase chemistry. In addition physiochemical interactions between the gas and aqueous phases are included. For species as H2O2, CH2O, O3, and SO2, Henry's law equilibria are assumed, whereas HNO3 and H2SO4 are regarded as completed dissolved in the aqueous phase. Absorption of HO2 and OH is assumed to be mass-transport limited. The chemistry of the aqueous phase is characterized by rapid cycling of odd hydrogen, (H2O2, HO2, and OH). O2(-) (produced through dissociation of HO2) reacting with dissolved O3 is a major source of OH in the aqueous phase. This reaction can be a significant sink for O3 in the troposphere. In the interstitial cloud air, odd hydrogen is depleted, whereas NO(x) remains in the gas phase, thus reducing ozone production due to the reaction between NO and HO2. Our calculations give markedly lower ozone levels when cloud interactions are included. This may in part explain the overpredictions of ozone levels often experienced in models neglecting cloud chemical interactions. In the present study, the existence of clouds, cloud types, and their lifetimes are modeled as pseudo random variables. Such pseudo random sequences are in reality deterministic and may, given the same starting values, be reproduced. The effects of cloud interactions on the overall chemistry of the troposphere are discussed. In particular, tests are performed to determine the sensitivity of cloud frequencies and cloud types.

Jonson, Jan E.↗

Climatic implications of the seasonal variation of upper troposphere water vapor

Satellite observations indicate that the humidity of the upper troposphere is higher in summer than in winter. We use general circulation model (GCM) simulations to explore the processes that maintain upper troposphere water vapor and determine its seasonal cycle. In the subtropics, drying by Hadley cell subsidence and stratiform condensation is offset primarily by moistening by eddies, with moist convection playing a minor role. Elsewhere, both mean meridional circulation and eddies moisten the upper troposphere and are balanced primarily by stratiform condensation drying. The effect of the seasonal shift of the Hadley cell is limited to latitudes equatorward of 30 deg. At higher latitudes where the largest observed summer moistening occurs, eddy moisture fluxes are primarily responsible despite the eddies being weaker in summer than winter. The same mechanism causes upper level humidity to increase in GCM climate warming simulations. The observed seasonal variation may thus be a good proxy for decadal climate change. This suggests that upper troposphere water vapor feedback is positive at all latitudes, consistent with GCM predictions.

Del Genio, Anthony D.↗

A test of water vapor radiometer-based troposphere calibration using VLBI observations on a 21-kilometer baseline

Simultaneous very long baseline interferometry (VLBI) and water vapor radiometer (WVR) measurements on a 21 km baseline showed that calibration by WVRs removed a significant fraction of the effect of tropospheric delay fluctuations for these experiments. From comparison of the residual delay variations within scans and between scans, the total tropospheric contribution t the delay residuals for each of the three 5 to 20 hour sessions was estimated as 1, 17, and 10%, with the first value being uncertain. The observed improvement in rms residual delay from WVR calibration during these three sessions was 4, 16, and 2%, respectively. The improvement is consistent with the estimated 2 to 3 mm path delay precision of current WVRs. The VLBI measurements, of natural radio sources, were conducted in April and May 1993 at Goldstone, California. Dual-frequency (2.3 and 8.4 GHz) observations were employed to remove the effects of charged particles from the data. Measurements with co-pointed WVRs, located within 50 m of the axis of each antenna, were performed to test the ability of the WVRs to calibrate line-of-sight path delays. Factors that made WVR performance assessment difficult included (1) the fact that the level of tropospheric fluctuations was smaller than is typical for Goldstone during these experiments and (2) VLBI delay variations on longer time scales (i.e., over multiple scans) contained uncalibrated instrumental effects (probably a result of slow temperature variations in the VLBI hardware) that were larger than the tropospheric effects.

Linfield, R. P.↗

Ozone, Tropospheric

In the early part of the 20th century, ground-based and balloon-borne measurements discovered that most of atmosphere's ozone is located in the stratosphere with highest concentrations located between 15 and 30 km (9,3 and 18.6 miles). For a long time, it was believed that tropospheric ozone originated from the stratosphere and that most of it was destroyed by contact with the earth's surface. Ozone, O3, was known to be produced by the photo-dissociation of molecular oxygen, O2, a process that can only occur at wavelengths shorter than 242 nm. Because such short-wave-length radiation is present only in the stratosphere, no tropospheric ozone production is possible by this mechanism. In the 1940s, however, it became obvious that production of ozone was also taking place in the troposphere. The overall reaction mechanism was eventually identified by Arie Haagen-Smit of the California Institute of Technology, in highly polluted southern California. The copious emissions from the numerous cars driven there as a result of the mass migration to Los Angeles after World War 2 created the new unpleasant phenomenon of photochemical smog, the primary component of which is ozone. These high levels of ozone were injuring vegetable crops, causing women's nylons to run, and generating increasing respiratory and eye-irritation problems for the populace. Our knowledge of tropospheric ozone increased dramatically in the early 1950s as monitoring stations and search centers were established throughout southern California to see what could be done to combat this threat to human health and the environment.

Fishman, Jack↗

Upper-Tropospheric Winds Derived from Geostationary Satellite Water Vapor Observations

The coverage and quality of remotely sensed upper-tropospheric moisture parameters have improved considerably with the deployment of a new generation of operational geostationary meteorological satellites: GOES-8/9 and GMS-5. The GOES-8/9 water vapor imaging capabilities have increased as a result of improved radiometric sensitivity and higher spatial resolution. The addition of a water vapor sensing channel on the latest GMS permits nearly global viewing of upper-tropospheric water vapor (when joined with GOES and Meteosat) and enhances the commonality of geostationary meteorological satellite observing capabilities. Upper-tropospheric motions derived from sequential water vapor imagery provided by these satellites can be objectively extracted by automated techniques. Wind fields can be deduced in both cloudy and cloud-free environments. In addition to the spatially coherent nature of these vector fields, the GOES-8/9 multispectral water vapor sensing capabilities allow for determination of wind fields over multiple tropospheric layers in cloud-free environments. This article provides an update on the latest efforts to extract water vapor motion displacements over meteorological scales ranging from subsynoptic to global. The potential applications of these data to impact operations, numerical assimilation and prediction, and research studies are discussed.

Velden, Christopher S.↗

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.↗

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.↗

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.↗

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.↗

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.↗

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.↗

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.↗

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.↗

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↗

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.↗

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↗

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.↗