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NASA NTRS2003

Lightning and Other Influences On Tropical Tropospheric Ozone: Empirical Studies of Covariation

Tropical and subtropical tropospheric ozone are important radiatively active species, with particularly large effects in the upper third of the troposphere. Temporal variability of O3 has proved difficult to simulate day by day in process models. Thus, individual roles of lightning, biomass burning, and other pollution in providing precursor NO(x), radicals, and chain carriers (CO, hydrocarbons) remain unquantified by simulation, and it is theoretically reasonable that individual roles are magnified by a joint synergy. We use wavelet analysis and Burg-algorithm maximum entropy spectral analyses to describe time-scales and correlation of ozone with proxies for processes controlling its concentration. Our empirical studies link time variations apparent in several datasets: the SHADOZ (Southern Hemisphere Additional Ozonesondes) network stations (Nairobi, Fiji), and auxiliary series with power to explain ozone-determining processes, with some interpretation based on the TTO (Tropical Tropospheric Ozone) product derived from TOMS (the Total Ozone Mapping Spectrometer). The auxiliary series are The OTD/LIS(Optical Transient Detector/Lightning Imaging Sensor) measurements of the lightning NO(x) source, the OLR (Outgoing Longwave Radiation)measurement of high-topped clouds, and standard meteorological variables from the United States NCEP (National Centers for Environmental Prediction) and Data Assimilation Office analyses. Concentrating on equatorial ozone, we compare the statistical evidence on the variability of tropospheric ozone. Important variations occur on approximately two-week, two-month (Madden-Julian Oscillation) and annual scales, and relations with OLR suggest controls associated with continental clouds. Hence we are now using the Lightning Imaging Sensor data set to indicate NO(x) sources. We report initial results defining relative roles of the process mentioned affecting O3 using their covariance properties.

Chatfield, Robert B.↗
NASA NTRS2002

Sensitivity of Assimilated Tropical Tropospheric Ozone to the Meteorological Analyses

Tropical tropospheric ozone fields from two different experiments performed with an off-line ozone assimilation system developed in NASA's Data Assimilation Office (DAO) are examined. Assimilated ozone fields from the two experiments are compared with the collocated ozone profiles from the Southern Hemispheric Additional Ozonesondes (SHADOZ) network. Results are presented for 1998. The ozone assimilation system includes a chemistry-transport model, which uses analyzed winds from the Goddard Earth Observing System (GEOS) Data Assimilation System (DAS). The two experiments use wind fields from different versions of GEOS DAS: an operational version of the GEOS-2 system and a prototype of the GEOS-4 system. While both versions of the DAS utilize the Physical-space Statistical Analysis System and use comparable observations, they use entirely different general circulation models and data insertion techniques. The shape of the annual-mean vertical profile of the assimilated ozone fields is sensitive to the meteorological analyses, with the GEOS-4-based ozone being closest to the observations. This indicates that the resolved transport in GEOS-4 is more realistic than in GEOS-2. Remaining uncertainties include quantification of the representation of sub-grid-scale processes in the transport calculations, which plays an important role in the locations and seasons where convection dominates the transport.

Hayashi, Hiroo↗
NASA NTRS2003

Validation of Envisat Ozone Data Products using Satellite and Ground Based Data

The Envisat chemistry instruments provide an opportunity to continue the ozone data sets produced by TOMS, SBUV, HALOE, and SAGE. These data sets have already been extensively validated and are assured to be of high accuracy. Continuity and consistency of data sets among the various satellite instruments as well as ground networks is essential for detecting an ozone recovery and climate change. Our objective, as part of the Envisat CaWal program, is to validate SCIAMACHY, MIPAS, and GOMOS ozone products using these heritage instruments. In addition we plan to validate SCIAMACHY Level 1 radiance using heritage satellite data and ground observations using a radiative transfer model. Ground based data included US ozonesonde profiles and a double monochromator Brewer instrument located at Goddard Space Flight Center. To date we have tested our intercomparisons algorithms using available Envisat data compared with SBW/2 and the ground based observations. We analyzed the comparisons with respect to ozone amounts and latitude and found the differences that were expected based on the initial release of Envisat data, which had known deficiencies. We will present our latest results based on the most current release of Envisat ozone data products.

Hilsenrath, E.↗
NASA NTRS2002

Insights into Tropical Tropospheric Ozone from the SHADOZ Network

The first view of lower stratospheric and upper tropospheric structure from sondes is provided by a 3-year, 10-site record from the Southern Hemisphere ADditional OZonesondes (SHADOZ) network: http://code9 16.gsfc.nasa.gov/Data_services/shadoz. Observations covering 1998-2000 were made over Ascension Island; Nairobi, Kenya; Irene, South Africa; La Reunion Island; Watukosek, Java; Fiji; Tahiti; American Samoa; San Cristobal, Galapagos; Natal, Brazil. Taking the UT/LS (upper troposphere-lower stratosphere) as the region between 12 and 17 km, we examine ozone variability in this region on a week-to- week and seasonal basis. The tropopause is lower in September-October-November than in March-April-May, when ozone is a minimum at most SHADOZ stations. A zonal wave-one pattern (referring to ozone mixing ratios greater over the Atlantic and adjacent continents than over the Pacific and eastern Indian Ocean), persists all year. The wave, predominantly in the troposphere and with variable magnitude, appears to be due to general circulation - with subsidence over the Atlantic and frequent deep convection over the Pacific and Indian Ocean. The variability of deep convection - most prominent at Java, Fiji, Samoa and Natal - is explored in time-vs-altitude ozone curtains. Stratospheric incursions into the troposphere are most prominent in soundings at Irene and Reunion Island.

Thompson, A. M.↗
NASA NTRS2003

Convective Lofting Links Indian Ocean Air Pollution to Paradoxical South Atlantic Ozone Maxima

We describe a broad resolution of the "Atlantic Paradox" concerning the seasonal and geographic distribution of tropical tropospheric ozone. We describe periods of significant maximum tropospheric O3 for Jan.-April, 1999, exploiting satellite estimates and SHADOZ (Southern Hemisphere Additional Ozonesondes). Trajectory analyses connecting sondes and Total Tropospheric Ozone (TTO)O3 maps suggest a complex influence from the Indian Ocean: beginning with mixed combustion sources, then low level transport, cumulonimbus venting, and finally high-level transport to the west, with possible mixing over Africa. For the Jan.- March highest column-O3 periods in the Atlantic, distinct sounding peaks trace to specific NO sources, especially lightning, while in the same episodes, recurring every 30 or 60 days, more diffuse buildups of Indian-to-Atlantic pollution make important contributions.

Chatfield, Robert B.↗
NASA NTRS2003

Estimating the Tropospheric Ozone Distribution by the Assimilation of Satellite Data

Tropospheric ozone is important to the environment, because it acts as a strong oxidant to control the concentrations of many reduced gases (methane, carbon monoxide, ... ), its radiative forcing plays a significant role in the greenhouse effect, and direct contact with ozone is harmful to human health. Tropospheric ozone, whose main sources are intrusion from the stratosphere and chemical production from source gases associated with urban pollution or biomass burning, varies on a wide range of spatial and temporal scales. Its transport and chemistry can be influenced by weather, seasonal, or multiannual variability. Despite the importance of tropospheric ozone, it contributes only about 10% of the total ozone loading in the atmosphere. Consequently, satellite instruments lose sensitivity below the stratospheric ozone peak, and provide little information about middle and lower tropospheric ozone. This talk will discuss recent modifications made to the satellite ozone data assimilation system at NASA's Data Assimilation Office (DAO) in order to provide better tropospheric ozone columns and profiles. We use a version of the system that assimilates only the data from the Solar Backscatter UltraViolet/2 (SBUV/2) instrument. The quality of the assimilated ozone in the tropical troposphere is evaluated by comparison with independent observations obtained from the Southern Hemispheric Additional Ozonesondes (SHADOZ) network. It is shown that the quality of ozone fields is sensitive to the winds used in the transport model. Increasing the vertical resolution of the model also has a beneficial impact. The assimilated ozone in the lower troposphere was substantially improved by inclusion of tropospheric ozone production, loss, and dry deposition rates from the Harvard GEOS-CHEM model. The mechanisms behind these results will be examined and the implications for our understanding of tropospheric ozone will be discussed.

Hayashi, Hiroo↗
NASA NTRS2004

African Equatorial and Subtropical Ozone Plumes: Recurrences Timescales of the Brown Cloud Trans-African Plumes and Other Plumes

We have found repeated illustrations in the maps of Total Tropospheric Ozone (TTO) of apparent transport of ozone from the Indian Ocean to the Equatorial Atlantic Ocean. Most interesting are examples that coincide with the INDOEX observations of late northern winter, 1999. Three soundings associated with the SHADOZ (Southern Hemisphere Additional Ozonesondes) network help confirm and quantify degree of influence of pollution, lightning, and stratospheric sources, suggesting that perhaps 40% of increased Atlantic ozone could be Asian pollution during periods of maximum identified in the TTO maps. We outline recurrent periods of apparent ozone transport from Indian to Atlantic Ocean regions both during and outside the late-winter period. These are placed in the context of some general observations about factors controlling recurrence timescales for the expression of both equatorial and subtropical plumes. Low-level subtropical plumes are often controlled by frontal systems approaching the Namib coast; these direct mid-level air into either easterly equatorial plumes or westerly mid- troposphere plumes. Equatorial plumes of ozone cross Africa on an easterly path due to the occasional coincidence of two phenomena: (1) lofting of ozone to mid and upper levels, often in the Western Indian Ocean, and (2) the eastward extension of an Equatorial African easterly jet.

Chatfield, Robert B.↗
NASA NTRS2004

Brown Cloud Pollution and Smog Ozone Transport 6,000 km to the Tropical Atlantic: Mechanism and Sensing

We have found repeated illustrations in the maps of Total Tropospheric Ozone (TTO) of apparent transport of ozone from the Indian Ocean to the Equatorial Atlantic Ocean. Most interesting are examples that coincide with the INDOEX observations of late northern winter. Three soundings with the SHADOZ (Southern Hemisphere Additional Ozonesondes) network help confirm and quantify degree of influence of pollution, lightning, and stratospheric sources, suggesting that perhaps 40% of increased Atlantic ozone could be Asian pollution during periods of maximum identified in the TTO maps. This analysis also indicates a mechanism for such extended transport. We outline recurrent periods of apparent ozone transport from Indian to Atlantic Ocean regions outside the late-winter period. Clearly brown-cloud aerosol affects tropospheric ozone, both limiting its chemical production and also potentially obscuring its detection by the TOMS instrument. Introductory statistical studies will be presented, evaluating the role of tropopause meteorology, aerosol, and other factors in the modifying the relationship between true tropospheric ozone measured by SHADOZ and the TTO product, with suggestions for extending the product.

Chatfield, Robert B.↗
NASA NTRS2003

Ozone Climatological Profiles for Version 8 TOMS and SBUV Retrievals

A new altitude dependent ozone climatology has been produced for use with the latest Total Ozone Mapping Spectrometer (TOMS) and Solar Backscatter Ultraviolet (SBUV) retrieval algorithms. The climatology consists of monthly average profiles for ten degree latitude zones covering from 0 to 60 km. The climatology was formed by combining data from SAGE II (1988 to 2000) and MLS (1991-1999) with data from balloon sondes (1988-2002). Ozone below about 20 km is based on balloons sondes, while ozone above 30 km is based on satellite measurements. The profiles join smoothly between 20 and 30 km. The ozone climatology in the southern hemisphere and tropics has been greatly enhanced in recent years by the addition of balloon sonde stations under the SHADOZ (Southern Hemisphere Additional Ozonesondes) program. A major source of error in the TOMS and SBUV retrieval of total column ozone comes from their reduced sensitivity to ozone in the lower troposphere. An accurate climatology for the retrieval a priori is important for reducing this error on the average. The new climatology follows the seasonal behavior of tropospheric ozone and reflects its hemispheric asymmetry. Comparisons of TOMS version 8 ozone with ground stations show an improvement due in part to the new climatology.

McPeters, R. D.↗
NASA NTRS2004

Variability in Tropical Tropospheric Ozone as Observed by SHADOZ

The SHADOZ (Southern Hemisphere Additional Ozonesondes) ozone sounding network was initiated in 1998 to improve the coverage of tropical in-situ ozone measurements for satellite validation, algorithm development and related process studies. Over 2000 soundings have been archived at the central website, , for 12 stations: Ascension Island; Nairobi and Malindi, Kenya; Irene, South Africa; Reunion Island; Watukosek, Java; Fiji; Tahiti; American Samoa; San Cristobal, Galapagos; Natal, Brazil; Paramaribo, Surinam. Some results to date indicate reliability of the measurement and highly variable interactions between ozone and tropical meteorology. For example: 1. By using ECC sondes with similar procedures, 5-10% accuracy and precision (1-sigma) of the sonde total ozone measurement was achieved [Thompson et al., 2003al; 2. Week-to-week variability in tropospheric ozone is so great that statistics are frequently not Gaussian and most stations vary up to a factor of 3 in column amount over the course of a year [Thompson et al., 2002b]. 3. Longitudinal variability in tropospheric ozone profiles is a consistent feature, with a 10- 15 DU column-integrated difference between Atlantic and Pacific sites; this is the cause of the zonal wave-one feature in total ozone [Shiotani, 1992]. The ozone record from Paramaribo, Surinam (6N, 55W) is a marked contrast to southern tropical ozone because Surinam is often north of the Intertropical Convergence Zone. Interpretations of SHADOZ time-series and approaches to classification suggested by SHADOZ data over Africa and the Indian Ocean will be described.

Thompson, Anne M.↗
NASA NTRS2004

Tropospheric Ozone Climatology over Irene, South Africa, From 1990-1994 and 1998-2002

This paper describes ozone profiles from sonde data during the period of NASA s TRACE-A and the more recent SHADOZ (Southern Hemisphere Additional Ozonesondes) period. The data were taken by the South African Weather Service at the Irene (25 deg.54 min S; 28 deg. 13 min. E) station near Pretoria, South Africa, an area that is a unique mixture of local industry, heavy biofuels use and importation of biomass burning ozone from neighboring countries to the north. The main findings are: (1) With its geographical position at the edge of the subtropical transition zone, mid- latitude dynamical influences are evident at Irene, predominantly in winter when upper tropospheric ozone is enhanced as a result of stratospheric-tropospheric exchange. (2) There has been an increase in the near-surface ozone amount between the early 1990s and a decade later, presumably due to an influx of rural population toward the Johannesburg-Pretoria area, as well as with industrial growth and development. (3) Most significant for developing approaches for satellite ozone profile climatologies, cluster analysis has enabled the delineation of a background and "most polluted" profile. Enhancements of at least 30% occur throughout the troposphere in spring and in certain layers increases of 100 % are observed.

Diab, R. D.↗
NASA NTRS2004

Perspectives on African Ozone from Sondes, Dobson and Aircraft Measurements

We have been studying variability in ozone over Africa using data from ozonesondes (vertical profiles from surface to stratosphere), aircraft (the MOZAIC dataset with cruise altitude and landing/takeoff profiles) and the ground (Dobson spectrophotometer total ozone column measurement). The following may give context for ozone investigations during AMMA: 1. Total ozone measurements since 1989 show considerable variability in mean value among the African stations in Algeria, Kenya, Egypt, South Africa, as well as in seasonal cycles and year-to-year. Trends are not evident. 2. The impacts of convection, stratospheric injection, biomass burning and lightning appear in ozone sounding profile data. Time-series analysis and case studies point to periodic influences of long-range interactions with the Atlantic ("ozone paradox," wave-one") and Indian Oceans. 3. Tropospheric ozone variations, observed in tropospheric profiles and integrated column amount, follow general seasonal patterns but short- term variability is so strong that simple averages are inadequate for describing "climatology" and statistical classification approaches may be required.

Thompson, A. M.↗
NASA NTRS2004

Can Assimilation of Satellite Ozone Data Contribute to the Understanding of the Lower Stratospheric Ozone?

We study the quality of lower stratospheric ozone fields from a three- dimensional global ozone assimilation system. Ozone in this region is important for the forcing of climate, but its global distribution is not fully known because of its large temporal and vertical variability. Modeled fields often have biases due to the inaccurate representation of transport processes in this region with strong gradients. Accurate ozonesonde or satellite occultation measurements have very limited coverage. Nadir measurements, such as those from the Solar Backscatter Ultraviolet/2 (SBUV/2) instrument that provide wide latitudinal coverage, lack the vertical resolution needed to represent sharp vertical features. Limb measurements, such as those from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), provide a finer vertical resolution. We show that assimilation of MIPAS data in addition to SBUV/2 data leads to better estimates of ozone in comparison with independent high quality satellite, aircraft, and ozone sonde measurements. Other modifications to the statistical analysis that have an impact on the lower stratospheric ozone will be mentioned: error covariance modeling and data selection. Direct and indirect impacts of transport and chemistry models will be discussed. Implications for multi-year analyses and short-tern prediction will be addressed.

Stajner, I.↗
NASA NTRS2004

Tropical Tropospheric Ozone Climatology: Approaches Based on SHADOZ Observations

The SHADOZ (Southern Hemisphere Additional Ozonesondes) ozone sounding network was initiated in 1998 to improve the coverage of tropical in-situ ozone measurements for satellite validation, algorithm development and related process studies. Over 2000 soundings have been archived at the central website, , for 12 stations that span the entire equatorial zone [Thompson et al., JGR, 108,8238, 2003]. The most striking features of tropospheric ozone profiles in SHADOZ are: (1) persistent longitudinal variability in tropospheric ozone profiles, with a 10-15 DU column-integrated difference between Atlantic and Pacific sites; (2) intense short-term variability triggered by changing meteorological conditions and advection of pollution. The implications of these results for profile climatologies and trends are described along with several approaches to classifying ozone profiles: 1) Seasonal means during MAM (March-April-May) and SON (September-October-November); 2) Maxima and minima, identified through correlation of TOMS-derived TTO (tropical tropospheric ozone) column depth with the sonde integrated tropospheric ozone column; and 3) Meteorological regimes, a technique that is effective in the subtropics where tropical and mid-latitude conditions alternate.

Thompson, Anne M.↗
NASA NTRS2004

Ozone Measurements and a 3D Chemical Transport Model

We have used our three-dimensional chemical transport model (CTM) to calculate the expected reponse of stratospheric composition over the past 30 years to forcing by chlorine and bromine compounds, solar ultraviolet, and volcanic aerosols. The CTM uses off-line winds and temperatures fiom a 50-year run of the finite volume general circulation model (FVGCM). We compare the total column ozone and the ozone profile fiom the CTM output to a variety of data sources. These include a merged total ozone data set from TOMS and SBUV using the new version 8 algorithm. Total ozone fiom the CTM are compared to ground-station measurements of total ozone at specific locations. Ozone profiles are compared to satellite meausrements fiom SBUV, SAGE, and HALOE. Profiles are also compared to ozonesondes over several locations. The results of the comparisons are quantified by using a time-series statistical analysis to determine trends, solar cycle, and volcanic reponse in both the model and in the data. Initial results indicate that the model responds to forcings in a way that is similar to the observed atmospheric response. The model does seem to be more sensitive to the chlorine and bromine perturbation ihan is the data. Further details and comparisons wiii be discussed.

Stolarski, Richard S.↗
NASA NTRS2001

Global Modeling of Tropospheric Chemistry with Assimilated Meteorology: Model Description and Evaluation

We present a first description and evaluation of GEOS-CHEM, a global three-dimensional (3-D) model of tropospheric chemistry driven by assimilated meteorological observations from the Goddard Earth Observing System (GEOS) of the NASA Data Assimilation Office (DAO). The model is applied to a 1-year simulation of tropospheric ozone-NOx-hydrocarbon chemistry for 1994, and is evaluated with observations both for 1994 and for other years. It reproduces usually to within 10 ppb the concentrations of ozone observed from the worldwide ozonesonde data network. It simulates correctly the seasonal phases and amplitudes of ozone concentrations for different regions and altitudes, but tends to underestimate the seasonal amplitude at northern midlatitudes. Observed concentrations of NO and peroxyacetylnitrate (PAN) observed in aircraft campaigns are generally reproduced to within a factor of 2 and often much better. Concentrations of HNO3 in the remote troposphere are overestimated typically by a factor of 2-3, a common problem in global models that may reflect a combination of insufficient precipitation scavenging and gas-aerosol partitioning not resolved by the model. The model yields an atmospheric lifetime of methylchloroform (proxy for global OH) of 5.1 years, as compared to a best estimate from observations of 5.5 plus or minus 0.8 years, and simulates H2O2 concentrations observed from aircraft with significant regional disagreements but no global bias. The OH concentrations are approximately 20% higher than in our previous global 3-D model which included an UV-absorbing aerosol. Concentrations of CO tend to be underestimated by the model, often by 10-30 ppb, which could reflect a combination of excessive OH (a 20% decrease in model OH could be accommodated by the methylchloroform constraint) and an underestimate of CO sources (particularly biogenic). The model underestimates observed acetone concentrations over the South Pacific in fall by a factor of 3; a missing source from the ocean may be implicated.

Bey, Isabelle↗
NASA NTRS2004

Vertical Profiling of Air Pollution at RAPCD

The interaction between local and regional pollution levels occurs at the interface of the Planetary Boundary Layer and the Free Troposphere. Measuring the vertical distribution of ozone, aerosols, and winds with high temporal and vertical resolution is essential to diagnose the nature of this interchange and ultimately for accurately forecasting ozone and aerosol pollution levels. The Regional Atmospheric Profiling Center for Discovery, RAPCD, was built and instrumented to address this critical issue. The ozone W DIAL lidar, Nd:YAG aerosol lidar, and 2.1 micron Doppler wind lidar, along with balloon- borne ECC ozonesondes form the core of the W C D instrumentation for addressing this problem. Instrumentation in the associated Mobile Integrated Profiling (MIPS) laboratory includes 91 5Mhz profiler, sodar, and ceilometer. The collocated Applied particle Optics and Radiometry (ApOR) laboratory hosts an FTIR along with MOUDI and optical particle counters. With MODELS-3 analysis by colleagues in the National Space Science and Technology Center on the UAH campus and the co- located National Weather Service Forecasting Office in Huntsville, AL we are developing a unique facility for advancing the state of the science of pollution forecasting.

Newchurch, Michael J.↗
NASA NTRS2004

New Perspectives from Satellite and Profile Observations on Tropospheric Ozone over Africa and the Adjacent Oceans: An Indian-Atlantic Ocean Link to tbe "Ozone Paradox"

In the past few years, tropospheric ozone observations of Africa and its adjacent ocenas have been greatly enhanced by high resolution (spatial and temporal) satellite measurements and profile data from aircraft (MOZAIC) and balloon-borne (SHADOZ) soundings. These views have demonstrated for the first time the complexity of chemical-dynamical interactions over the African continent and the Indian and Atlantic Oceans. The tropical Atlantic "ozone paradax" refers to the observation that during the season of maximum biomass burning in west Africa north of the Intertropical Convergence Zone (ITCZ), the highest tropospheric ozone total column occurs south of the ITCZ over the tropical Atlantic. The longitudinal view of tropospheric ozone in the southern tropics from SHADOZ (Southern Hemisphere Additional Ozonesondes) soundings shown the persistence of a "zonal-wave one" pattern that reinforces the "ozone paradox". These ozone features interact with dynamics over southern and northern Africa where anthropogenic sources include the industrial regions of the South African Highveld and Mideastern-Mediterranean influences, respectively. Our newest studies with satellites and soundings show that up to half the ozone pollution over the Atlantic in the January-March "paradox" period may originate from south Asian pollution. Individual patches of pollurion over the Indian Ocean are transported upward by convective mixing and are enriched by pyrogenic, biogenic sources and lightning as they cross Africa and descend over the Atlantic. In summary, local sources, intercontinental import and export and unique regional transport patterns put Africa at a crossroads of troposheric ozone influences.

Thompson, Anne M.↗