Survey
* Your assessment is very important for improving the workof artificial intelligence, which forms the content of this project
* Your assessment is very important for improving the workof artificial intelligence, which forms the content of this project
SHADOZ—A TROPICAL OZONESONDE–RADIOSONDE NETWORK FOR THE ATMOSPHERIC COMMUNITY BY ANNE M. THOMPSON, JACQUELYN C. WITTE, SAMUEL J. OLTMANS, AND FRANCIS J. SCHMIDLIN A new observing network reveals complexities of tropical ozone while providing an international model for climate-related data collection and public archiving. B ACKGROUND. The ozonesonde measurement. Although ozone-measuring satellites have been collecting data since 1970 (Heath et al. 1975), validation of profiles and total column measurements is still performed by relatively lowtechnology instruments. Total column ozone is verified with spectrophotometric data from a ground-based network (Bojkov et al. 1999). Profiles measured by balloon-borne ozonesondes are used to evaluate satellite retrievals (WMO 1998a). The ozonesonde is flown with a standard radiosonde. Designed to measure ozone concentrations from the surface to above AFFILIATIONS: THOMPSON—NASA Goddard Space Flight Center, Greenbelt, Maryland; WITTE—SSAI, Lanham, Maryland; OLTMANS— NOAA/Climate Diagnostics and Monitoring Laboratory, Boulder, Colorado; SCHMIDLIN—NASA Wallops Flight Facility, Wallops Island, Virginia CORRESPONDING AUTHOR: Anne M. Thompson, NASA Goddard Space Flight Center, Code 916, Greenbelt, MD 20771 E-mail: [email protected] DOI:10.1175/BAMS-85-10-1549 In final form 2 May 2004 ©2004 American Meteorological Society AMERICAN METEOROLOGICAL SOCIETY the ozone concentration maximum, the combined ozonesonde–radiosonde package is flown with a 1200–1500-g balloon that usually bursts at 4–8 hPa. In an electrochemical concentration cell (ECC) ozonesonde, air pumped through a pair of cells containing a potassium iodide solution initiates an electric current proportional to the amount of ozone in the atmosphere. The ozone current is transmitted back to a ground receiver and the partial pressure of ozone is recorded with the pressure–temperature– humidity (PTU) readings of the radiosonde. Figure 1 shows an ozonesonde during its preflight testing (Fig. 1a) and its assembly with the radiosonde (Fig. 1b) prior to launch. Figure 2 shows the raw data (relative humidity, temperature, and ozone pressure; left panel) and ozone amount (right panel) in volume mixing ratio, the unit most commonly used by atmospheric chemists. Note that stratospheric ozone (the “good” ozone shielding the earth from ultraviolet radiation) is present at > 1 part per million by volume (ppmv), whereas tropospheric ozone (sometimes referred to as “bad” or “smog” ozone) is counted in parts per billion by volume (ppbv). Background surface ozone ranges from 10 to 40 ppbv, depending on geographiOCTOBER 2004 | 1549 ozone measurements in the 1920s; for a review see Staehelin et al. (1998). One Dobson unit corresponds to 2.69 × 10 (16) molecules above 1 cm2 or a thickness of 0.1 mm at standard temperature. The thickness of all ozone molecules is typically 2.5–4.5 cm-atm or 250–450 Dobson units. The lower values typify a naturally thinner ozone column over the Tropics. The highest values occur near the poles, except during ozone depletion extremes when the column depth over Antarctica may drop to < 100 DU. Presently about 50 stations send ozonesonde data to the World Ozone and Ultraviolet Data Centre in Toronto, Canada (information online at www.woudc. org), an archive operated by Environment Canada. In addition to providing ground truth and climatologies for satellites (Fortuin and Kelder 1998), ozone profiles are used for the evaluation of chemical models (Logan 1999a,b; Lawrence et al. 1999; Bey et al. 2001) and the determination of ozone trends (WMO 1998a; Randel et al. 1999). Most Northern Hemisphere ozonesonde stations date from the 1960s and 1970s. The only tropical station in the Southern Hemisphere that has operated ozonesondes routinely for more than a decade is at Natal, Brazil (Logan and Kirchhoff 1986; Kirchhoff et al. 1988). FIG. 1. (a) Photo of the ECC ozonesonde instrument. Potassium iodide sensing solutions are placed in the plastic cells at the left. The inlet (blue tube at right) pulls air toward the pump; a second tube sends air into the cells. Behind the upright flat metal piece is the electronics board that transmits the current from the ozone sensor along with the radiosonde signal. The ozone current is proportional to the ozone partial pressure (Fig. 2, left box, black). (b) Assembled ozonesonde, inside its foam box, with radiosonde attached on the right. cal location. On a highly polluted day in the United States—called “code red” in some areas—surface ozone may exceed 150 ppbv. The column-integrated amount of ozone is measured in mm-atm or Dobson units (DU), which is named after G. M. B. Dobson who began routine 1550 | OCTOBER 2004 Tropical ozone and meteorological issues. Ozone column amounts in the Tropics vary over a smaller range than at higher latitudes and normally fall within 225– 300 DU (e.g., Fig. 6 in Thompson et al. 2003a). The reason is that there is less variability in the stratospheric ozone column in the Tropics compared to the extratropics. Signatures of the quasi-biennial oscillation (QBO) on ozone have been known since the 1960s, and their investigations have been greatly enhanced by satellite data (e.g., Bowman 1989; Hollandsworth et al. 1995; Bojkov and Fioletov 1996). The QBO interactions with ozone are described in many papers summarized in the Baldwin et al. (2001) review article (see below). The equatorial Total Ozone Mapping Spectrometer (TOMS) solar backscatter ultraviolet (SBUV) total ozone records show evidence of the cyclical variability attributed to the QBO (Shotani 1992; Hollandsworth et al. 1995). The Stratospheric Aerosols and Gases Experiment (SAGE) satellite captures changes in the ozone profile as it responds to shifts in midstratospheric winds (Zawodny and McCormick 1991; Randel and Wu 1996). Interannual variability in total ozone also correlates with El Niño–Southern Oscillation (ENSO). Focused attention on tropospheric ozone at low latitudes originated in concerns about the impact of widespread biomass burning in the Tropics and in 1991), although one equatorial cruise found a number of soundings with a tropospheric column depth < 10 DU (Kley et al. 1996). Net photochemical destruction of ozone over the Pacific (Thompson et al. 1993) leads to very low surface ozone (< 5 ppbv). Convective mixing of lowozone surface air can lead to low ozone concentrations aloft (Piotrowicz et al. 1991) and a low-tropospheric ozone column. The Atlantic–Pacific difference in ozone column depth was detected by the TOMS satellite, where a FIG. 2. Typical profile from the SHADOZ Web site. (left) Data in ozone parzonal view displays a wavetial pressure, relative humidity, and temperature from radiosonde, with (right) one-like appearance (Fishman ozone volume mixing ratio determined from the ratio of the ozone and total and Larsen 1987; Shiotani atmospheric pressures. Sounding was taken on 17 Oct 2001 from Ascension 1992). The wave-one pheIsland. High ozone peaks below 10 km originate from African regions with biomass burning. nomenon refers to a variable ozone depth when the studies with satellite data in the late 1980s and 1990s. ozone column is viewed zonally. The difference beFor example, a 1980 field study characterized emis- tween the maximum (near 0∞ longitude, over the Atsions of ozone precursors (nitrogen oxides, carbon lantic) and the minimum (near 180∞) varies over the monoxide, reactive hydrocarbons) from savanna fires course of the year, ranging from ~10–25 DU. as well as their impact on ozone (Crutzen et al. 1985; Schematically, the wave is similar to the following: Chatfield and Delany 1990). In the south tropical Atlantic, a seasonal maximum in total and tropospheric ozone observed from a satellite was attributed to large-scale savanna burning (Fishman et al. 1986; 1991). Ozone soundings at Brazzaville, Congo (4∞S, 15∞E), Ascension Island (8∞S, 15∞W), and Natal (6∞S, 35∞W) confirmed that Atlantic ozone was indeed concentrated in layers trans. ported from regions of African and South American burning (Cros et al. 1992; Olson et al. 1996). During September–October, tropospheric column ozone may exceed 50 DU over Africa, South America, and the The fact that the stratospheric ozone column depth tropical Atlantic, compared to ~30 DU in April or May viewed from SAGE does not show longitudinal vari(Logan and Kirchhoff 1986; Thompson et al. 1996). ability (Fishman and Larsen 1987; Shiotani and Ozone pollution from African fires frequently crosses Hasebe 1994) suggests that there is no stratospheric the Indian and Pacific Oceans, where it has been de- wave, but this has been difficult to verify given the tected in soundings over La Réunion (Baldy et al. 1996), imprecision in lower-stratospheric ozone retrievals. Java, Indonesia (Komala et al. 1996);Tahiti; French The aforementioned observations summarize our Polynesia; Samoa; and Fiji (Oltmans et al. 2001). knowledge of tropical ozone up to 1998. Only 200– In contrast to the Atlantic, tropospheric ozone col- 300 soundings from the Tropics were available for umn amounts over the tropical Pacific were usually analysis by the scientific community. Furthermore, less than 30 DU (Komhyr et al. 1989; Fishman et al. there was no consistency in launch frequency, instruAMERICAN METEOROLOGICAL SOCIETY OCTOBER 2004 | 1551 mentation, and geographical coverage. Stations started and stopped with campaigns, so trends and mechanisms could not be determined with any reliability. Thus, more standardized and comprehensive data were required for addressing the following: • How does tropical ozone in the troposphere vary with time? Which processes are responsible? • What is the zonal structure of tropospheric ozone in the Tropics? Can it explain the standing wave-one pattern in equatorial ozone observed from satellite? • What is the best way to prescribe an ozone profile climatology for satellite retrievals? • How can typical satellite algorithms account for regional and seasonal variability in tropospheric ozone? Are new ozone products from satellites accurate—for example, the estimates of tropospheric ozone column depth? SHADOZ PROJECT AND DATA. In order to ensure that sufficient numbers of soundings are available throughout the Tropics we initiated the Southern Hemisphere Additional Ozonesondes (SHADOZ) project in 1998, putting together a network of stations according to the following criteria: • That they are operational to avoid startup costs and to leverage off local support and infrastructure; • That they contribute to a geographical distribution, spanning the entire longitude range; • That there are weekly launches, with the project sometimes supplying additional sondes (hence, the name) in exchange for all of the sonde data from the location; and • That there is unrestricted Web site access by the community to the complete SHADOZ dataset. The nine original SHADOZ stations stretched from the western Pacific and eastern Indian Oceans across to South America, Africa, and La Réunion, an island east of Madagascar. Since 1998, four more stations have joined the network, including two in the northern Tropics [Surinam and Malaysia (3∞N, 102∞E)] that displays distinct influences from the Southern Hemisphere (Peters et al. 2004). All stations are listed in Table 1. More than 2000 sonde profiles for the twelve stations (• in Fig. 3) are available at the SHADOZ Web site (online at http://croc.gsfc.nasa.gov/shadoz), including 80 profiles from several campaigns of opportunity (* in Fig. 3). Experimental details of each station and personnel contact information are given in Thompson et al. (2003a). In addition to the data and graphical display of the sounding, the air parcel history of each sounding is depicted at the SHADOZ Web site. These are based on 5-day back trajectories run with the National Aeronautics and Space Administration (NASA) Goddard kinematic trajectory model (Schoeberl and Newman 1995) at four standard pressure levels using the 2.5∞ × 2.5∞ National Centers for Environmental Prediction–National Center for Atmospheric Research (NCEP–NCAR) reanalysis dataset. For the sounding shown in Fig. 2, Fig. 4 shows the corresponding trajectories. HIGHLIGHTS OF SHADOZ OBSERVATIONS. Evaluation of sonde performance. To date, what do SHADOZ data tell us? First, by having so FIG. 3. SHADOZ sites (dots) and campaigns of opportunity (stars). Station latitude–longitude information is in Table 1. SHADOZ campaign data is as follows: Jan–Feb 1999 cruise (Thompson et al. 2000); INDOEX, Jan–Mar 1999 (data summarized in Thompson et al. 2003b); Lusaka, Zambia, Sep 2000 (Thompson et al. 2002). 1552 | OCTOBER 2004 The precision of the ozonesonde instrument deduced from SHADOZ may be better than previous evaluations (WMO 1998b) because SHADOZ samples are taken in a fairly uniform meteorological regime and with a similar technique. AMERICAN METEOROLOGICAL SOCIETY –0.92 San Cristóbal, Galapagos Islands OCTOBER 2004 –7.60 Watukosek, Java, Indonesia *positive for North, negative for South latitudes. **positive for East, negative for West longitudes. –18.13 –21.06 La Réunion Suva, Fiji –1.27 Nairobi, Kenya –25.25 Irene, South Africa –2.99 –7.98 Ascension Island Malindi, Kenya –5.42 Natal, Brazil 5.81 –18.00 Papeete, Tahiti, French Polynesia Paramaribo, Surinam –14.23* Latitude (∞∞) Pago, Pago, American Samoa Station 178.40 112.70 55.48 36.80 40.19 28.22 –14.42 –35.38 –55.21 89.60 149.00 170.56** Longitude (∞∞) NOAA/CMDL; S. J. Oltmans NASDA; T. Ogawa, S. Kawakami; and Kyoto University; M. Shiotani, M. Fujiwara CNRS/University of Réunion; F. Posny Méteosuisse; B. Hoegger, B. Calpini, G. Levrat University of Rome; G. Laneve South Africa Weather Service (SAWS); G. J. R. Coetzee NASA/Wallops; F. J. Schmidlin NASA/Wallops; F. J. Schmidlin KNMI; H. M. Kelder NOAA/CMDL; S. J. Oltmans, H. Vömel NOAA/CMDL; S. J. Oltmans NOAA/Climate Modeling and Diagnostics Laboratory (CMDL); S. J. Oltmans Sponsor; Coinvestigator University of the Pacific; K. Koshy LAPAN; S. Saraspriya, N. Komala University of Réunion; F. Posny, J-M. Metzger Kenya Meteorological Department; W. Kimani, W. Ayoma Project San Marco, M. A. C. Mwasaha SAWS; N. A. Phahlane, D. Esterhuyse U.S. Air Force INPE, V. W. J. H. Kirchhoff, F. da Silva Meteorological Service of Surinam; C. R. Becker National Institute of Hydrology and Meteorology of Ecuador (INAMHI); M. V. A. Reyes MéteoFrance; P. Simon NOAA/CMDL Operating Agency; Station Manager • The precision of the total ozone column measured by a single sounding device is 5%, realizing that each sonde launched is essentially a new instrument (this figure refers to the reproducibility of an individual sounding). • Comparison with groundbased instruments (four Dobson spectrophotometers and one Brewer spectrometer) showed agreement between integrated total ozone from the sondes ranging from 2% to 7%, with the best agreement at the African stations of Irene (near Pretoria, South Africa) and Nairobi, Kenya. • Comparison with total ozone from the TOMS satellite (version-7 data) shows a greater degree of variability (2%–11%) among stations, with the satellite measurement always higher. The new TOMS version-8 algorithm improves the sonde–satellite total column agreement by only 1%–2%. TABLE 1. SHADOZ stations; further technical details given in Table A1 in Thompson et al. (2003a). many data points taken under mostly tropical conditions, we have learned something about the ozonesonde measurement (Thompson et al. 2003a). Statistics from the first large set of tropical ozone soundings show the following: | 1553 QUASI-BIENNIAL OSCILLATION. Prior to SHADOZ, sounding data were neither frequent enough nor close enough to the equator (where the QBO effect is most pronounced) to fully document the ozone response to the QBO. In the stratosphere, near the ozone partial pressure maximum (25–27 km), the QBO variation is evident in many SHADOZ profiles (Logan et al. 2003). The QBO, a downward-propagating oscillation between easterly and westerly winds, has a period of about 28 months FIG. 4. Five-day back trajectories, initialized at pressure levels shown with color (Reed 1964). In the first half code, created by the GSFC kinematic trajectory model (Schoeberl and of 1998 the winds above Newman 1995), initialized with NCEP winds at the pressure levels indicated; + marks each 24-h transit segment. 30 hPa (~24 km) are easterly; throughout the year Although the SHADOZ PTU soundings have not there is a shift to westerly winds that causes the ozone been used as widely as ozone observations, the archive to increase at that pressure, over and above the noroffers a unique set of radiosondes (sample profiles are mal seasonal increase. Examples of profile changes for in Fig. 2). Temperature measurements from both a re- 1998 appear in Fig. 5. The reader is referred to Logan sistive-type (VIZ/Sippican) and capacitive-type et al. (2003) for a complete discussion of the QBO and (Vaisala) thermistor are used in SHADOZ. The two ozone using SHADOZ sondes and concurrent sateltypes of sensors do not provide identical values lite data. (Schmidlin 1988; Nash and Schmidlin 1987); differences in the stratosphere can exceed 1∞–1.5∞. Capacitive thermistor data are corrected in the sonde software at each station. Resistive thermistor measurements are not corrected at the station but may be when used by analysis centers, for example, NCEP. Ozone variability and meteorology. With unprecedented coverage, the principal accomplishment of SHADOZ has been to provide striking examples of the links among tropical meteorology, ozone, and pollution (Thompson et al. 2003b). We illustrate this with several examples. 1554 | OCTOBER 2004 FIG. 5. Profiles from Nairobi, Kenya, illustrate stratospheric ozone increases under the influence of the QBO in 1998 (a) Feb relative to (b) Oct. In 1999 there was not a noticeable difference in Feb–Oct phases. Profiles in 2001 (not shown) were similar to those for 1998. ZONAL WAVE-ONE PATTERN IN OZONE. As mentioned above, satellites like TOMS detect a standing wave-one pattern in the total ozone column at the equator (Fishman and Larsen 1987; Shiotani 1992; Shiotani and Hasebe 1994; Kim et al. 1996; Newchurch et al. 2001). Researchers have attempted to resolve the issue: is the wave-one pattern due to more ozone over the Atlantic in the troposphere, the lower stratosphere, or both? The ozone measurement from profiling satellites is least accurate in the lower stratosphere so it has been difficult to anFIG. 6. The structure of the zonal wave one in tropospheric ozone based on swer the question with suf0.25-km mean mixing ratios from all SHADOZ stations (except Irene), 1998– ficient precision in the ab2002. Between eastern South America and the western Indian Ocean, ozone sence of in situ ozone data and sources of photoreactive ozone precursors are more concentrated durin the Tropics. Given the ing biomass burning and lightning episodes. Further enrichment of ozone over the Atlantic is a consequence of a tendency for ozone to subside in that relongitudinal and temporal gion, compared to more active convection over the central Pacific. Thus, more coverage of the SHADOZ tropospheric ozone appears from ~50∞∞ W to 100∞∞ E than at other longitudes, data, it is possible to examgiving a wavelike appearance to the integrated ozone column (Figs. 13 and 14 ine the wave pattern for the in Thompson et al. 2003a). first time. The sonde record confirms the amplitude of the wave—10–25 DU, depending on time of year— 1996; Moxim and Levy 2000; Martin et al. 2002; Peters and shows that it is predominantly, if not completely, et al. 2002). Furthermore, subsidence is prevalent over in the troposphere. The structure is summarized in the south tropical Atlantic where midtropospheric Fig. 6, where a cross-sectional view of the ozone mix- ozone accumulates (Krishnamurti et al. 1996). It aping ratio (annually averaged) in the troposphere and pears that northern tropical ozone adds to the south lower stratosphere is illustrated. Details of the wave Atlantic ozone burden at times of the year when vary over the course of a year but the basic appear- southwesterly flows are followed by interhemispheric transport (Thompson et al. 2000; Edwards et al. 2003; ance remains similar to Fig. 6. How does the wave come about? It apparently re- Jenkins et al. 2003). The high-ozone feature over the sults from photochemical activity, dynamical patterns, Atlantic is enhanced by a persistent recirculation of and the general circulation. Photochemical reactions ozone pollution in an anticyclonic high pressure sysinvolve free-radical processes that form and destroy tem over southern Africa (Garstang et al. 1996; Tyson ozone at rates determined by local conditions: UV et al. 1997). Figure 7 shows the resulting gyre with arradiation, temperature, source species, and loss pro- rows indicating where ozone pollution heads west cesses, including removal at the surface. At any point toward the Atlantic. Ozone pollution also heads east in the atmosphere the ozone concentration is in an from Africa toward La Réunion (arrows in Fig. 7). equilibrium fixed by the net rate of formation or loss Over the eastern Indian and Pacific Oceans and net transport. Above the boundary layer, ozone (Watukosek, Java, and Fiji–Samoa–Tahiti), freein the Tropics is most concentrated over eastern South tropospheric ozone is at a minimum because convecAmerica, the Atlantic, Africa, and the Indian Ocean tion brings clean, lower-tropospheric ozone to the (40∞W–90∞E). In this region, photochemical sources middle and upper troposphere (Fig. 6). Similar patterns to those seen in SHADOZ sondes (biogenic, from biomass burning, lightning formation of ozone precursors) are abundant (Pickering et al. prevailed over the tropical Atlantic Ocean during the AMERICAN METEOROLOGICAL SOCIETY OCTOBER 2004 | 1555 Convective activity at La Réunion, most pronounced in February–March, is indicated by the appearance of relatively lower levels of ozone in the troposphere above 5 km. Convective influence is more pronounced at Natal (Fig. 8b) and Fiji (Fig. 8c) than at La Réunion (Fig. 8a). Signified by a local minimum in the middle– upper troposphere (within the 35 ppbv contour), the impact of convection is strongest at Natal during the February–April period. Fiji (Fig. 8c), in the South Pacific convergence zone, shows signatures of convective mixing throughout the year (Pickering et al. 2001). FIG. 7. Schematic representation of flows and processes contributing to the At all three stations, during persistent zonal ozone maximum observed over the south tropical Atlantic. the period from August to Besides biomass fires, lightning-derived nitric oxide, biogenic sources of nitric oxide, and nonmethane hydrocarbons provide the precursor gases that lead the end of the year, there is to photochemical ozone formation. The dynamic patterns all operate at some a localized ozone maxipoint in an annual cycle. mum between 5 and 10 km. Analysis of the ozone peaks Southern African Fire Atmospheric Research Initia- contributing to these features shows origins over retive (SAFARI)/Transport and Atmospheric Chemis- gions of biomass burning, mostly from Africa. try near the Equator—Atlantic (TRACE-A) field camPerhaps the most surprising result of SHADOZ is paigns (Fishman et al. 1996) in September–October the extent of week-to-week variability in ozone 1992. During that mission, aircraft and sonde sam- throughout the troposphere. Because most SHADOZ pling showed that the south Atlantic ozone maximum stations are remote from sources, the ozone vertical is due to elevated ozone mixing ratios (> 40 ppbv) that structure versus time (curtain graphs, Fig. 9) essenare most concentrated in the free troposphere (2– tially reflects short-term meteorological change. In 8 km) where the photochemical lifetime of ozone is many cases, advection of pollution alternates with 1 month. From Ascension Island ozonesondes and convection. Pollution leads to high ozone mixing raback trajectories, it was inferred that tropical Atlan- tios in the midtroposphere at Nairobi (green and yeltic ozone was composed roughly equally of a “back- low , Fig. 9a) and convection brings up low-ozone air ground ozone” amount and imported pollution, each and cleans it out. The convective signature is corrobo25 DU in column amount. Two-thirds of the pollu- rated by variations in relative humidity (Fig. 9b), tion originated over Africa, the remainder was from where the higher relative humidity, green-red above South America (Thompson et al. 1996). 8–10 km, shows vertical redistribution of ozone from the surface. Variability, pollution, convection, and long-range transport. There are two practical consequences of the variSeasonal variability in tropospheric ozone at three ability of ozone at SHADOZ sites. First, simple averSHADOZ sites, based on monthly averaged data from aged profiles, often used for analysis of trends, may 5 yr, is illustrated in Fig. 8. The chemical tropopause not be statistically robust. In Figs. 10a and 10b, sea(100 ppbv) is lower at La Réunion (Fig. 8a) than at sonally averaged [March–April–May (MAM) and the other two stations shown. In all three cases, the September–October–November (SON)] mean ozone tropopause is at its greatest altitude between February profiles at Nairobi, based on 4 yr of data, are shown and April, and is lowest in August through October. along with the individual profiles that comprise the 1556 | OCTOBER 2004 mean. The distribution of mixing ratios at a typical altitude (Fig. 10c) is so broad that the mean represents a relatively small fraction of the observations. The statistics are fairly similar during the two periods, although when tropospheric ozone column amounts are analyzed, the highest and lowest 20% occur, respectively, in the second half and first half of the year. Trends might be manifested in a modified distribution, particularly at the extremes. In an intriguing classification of ozone profiles from aircraft ascents and descents (surface–11 km) over one African location, Diab et al. (2003) showed ozone distributions correlating with a half-dozen prototypical synoptic situations. A second implication of the variability observed in SHADOZ data concerns the nature of ozone fluctuations that satellites and models are attempting to capture. For example, simulation of convective episodes apparently detected in SHADOZ ozone may challenge convective parameterizations in models. Similarly, convection, pollution, and stratospheric– tropospheric exchange episodes observed in SHADOZ are not resolved in satellite ozone data that are often available as monthly averages (Martin et al. 2002). Daily (or better, continuous) satellite data are required to track regional and intercontinental ozone transport (see, e.g., Thompson et al. 2001). One approach to obtain more accurate ozone retrievals could be to combine SHADOZ data with an assimilation model that includes photochemistry and appropriately resolved sources and transport. SHADOZ PARTICIPATION IN CAMPAIGNS. To give greater tropical coverage, SHADOZ station data have been augmented with ozone launches from field campaigns in which the interaction of ozone chemistry and meteorological processes has been studied. The campaign data are also available at the SHADOZ Web site. Aerosols99 and INDOEX campaigns. An Atlantic cruise on the National Oceanic and Atmospheric Administration (NOAA) R/V Ronald H. Brown in January and February 1999 (Fig. 3 gives the cruise track) showed that tropical tropospheric ozone profiles north of the ITCZ may be very different from south of the ITCZ. The shipboard measurements showed convective influence north of the ITCZ, and an ozone column 4– 5 DU lower than south of the ITCZ where ozone accumulated in descending air. In Fig. 11, the convection is signified by better mixing and more uniform ozone and humidity profiles (solid lines); the higher ozone with drier air (dashed lines) represents conditions south of the ITCZ. Satellite data showed AMERICAN METEOROLOGICAL SOCIETY FIG. 8. Tropospheric ozone variability, on an annually averaged basis at three SHADOZ stations, representative of the (a) subtropical Indian (La Réunion), (b) Atlantic (Natal, Brazil), and (c) Pacific (Samoa) Oceans. Based on data from 1998 to 2002. that the hemispheric ozone contrast was characteristic of the entire tropical Atlantic. Because biomass burning added pollution north of the ITCZ, the expectation had been that the greater ozone column OCTOBER 2004 | 1557 FIG. 9. Week-to-week tropospheric variability at Nairobi, indicated in altitude vs time graphs of the (a) ozone mixing ratio and (b) relative humidity for 1998–2001. Means of 0.25 km are used. Nairobi uses a capacitive-type temperature sensor (temperature profiles also available at SHADOZ Web site) for which corrections are incorporated into the reduction software. would be to the north. Instead, greater column ozone is south of the ITCZ, a phenomenon referred to as the “tropical Atlantic ozone paradox” (Thompson et al. 2000; Edwards et al. 2003; Jenkins et al. 2003). The Aerosols99 cruise coincided with the beginning of the Indian Ocean Experiment (INDOEX) 1558 | OCTOBER 2004 campaign (Zachariasse et al. 2001) during which soundings were taken for SHADOZ on Male Island (Kaashidhoo Observatory, 5∞N, 73∞E) in the Maldives. In Chatfield et al. (2004), SHADOZ soundings and daily tropospheric ozone satellite maps were used with trajectories and corroborative data [e.g., outgoing longwave radiation, fire, and lightning counts from the Tropical Rainfall Measuring Mission (TRMM) satellite, smoke aerosol from TOMS] to trace individual high-ozone layers to lightning and African and South American biomass fires. Ozone in the Kaashidhoo observatory sondes (35 DU) was similar to the TOMS measurement over the Indian Ocean downwind of southern Asia in late February 1999. Some of this ozone was lofted above 9 km, then transported over Africa to the region of Atlantic subsidence (Fig. 7). Signatures of Indian Ocean ozone were detected in the 3 March 1999 Nairobi sounding and at Ascension Island on 11 March 1999 (Fig. 12). Not only are individual pollution layers at Ascension Island traceable to transport from the Indian Ocean, a gradual increase in background ozone at Ascension Island during February–March 1999 is attributed to pollution from south Asia (Chatfield et al. 2004). SAFARI-2000. A campaign at Lusaka, Zambia, during SAFARI-2000 (Swap et al. 2003) confirmed the vertical stability of pollution layers during the southern African dry season, a phenomenon first characterized during the 1992 SAFARI(92)/TRACE-A (Garstang et al. 1996). Recirculation of pollution layers over south-central Africa produced very high tropospheric ozone throughout the free troposphere, in contrast to relatively clean profiles often found at fixed SHADOZ sites. Biomass burning over Angola, Namibia, Zimbabwe, and Mozambique, as well as South Africa and Zambia, itself contributed to a layer of pollution ozone > 100 ppbv over Lusaka (Thompson et al. 2002). Figure 13 shows a curtain graph of the ozone mixing ratio, averaged in 1-km layers, for nine soundings in the 2000 SAFARI (2000) campaign. A localized disturbance, following the fifth sounding, cleaned out the boundary layer and reduced ozone aloft, but a thinner stable layer at 2–3 km remained intact. In addition to the pollution aloft, boundary layer ozone during the first four SAFARI-2000 launches exceeded 90 ppbv, the highest level yet measured over southern Africa. Up to one-half of this pollution appeared to be from local vehicles and urban burning practices (Thompson et al. 2002). FIG. 10. Nairobi seasonal mean profile (a) MAM, and (b) SON to 20 km, based on 4-yr data, with individual profiles contributing to mean. (c) Histogram of ozone mixing ratios from Nairobi soundings, binned at 5 ppbv intervals, at 450 hPa (between 5 and 6 km). AMERICAN METEOROLOGICAL SOCIETY OCTOBER 2004 | 1559 FIG. 11. Mean profiles of ozone and relative humidity, taken north (solid) and south (dashed), respectively, of the ITCZ on the Aerosols99 cruise of the R/V Ronald H. Brown during a Jan–Feb 1999 Atlantic transect from Virginia to Cape Town, South Africa (Thompson et al. 2000). Sounding data reside in SHADOZ archive (online at http://croc.gsfc.nasa.gov/shadoz). JOSIE. SHADOZ is a vital part of several international efforts sponsored by the United Nations and several International Council of Scientific Unions (ICSU) bodies to assure integrated (satellite, airborne, balloon, ground-based) observing strategies to detect global change. The World Meteorological Organization (WMO) is developing a standard procedure for ozonesonde operations to be used at Global Atmospheric Watch (GAW) stations. It turns out that although all SHADOZ stations use the ECC sonde, small variations in instrument type (manufacturer) and preparation procedures may affect the ozone measurement. Thus, SHADOZ data and techniques are being used to evaluate details of sonde operations and data handling. In September 2000, SHADOZ investigators participated in the 2000 Jülich Ozonesonde Intercomparison Experiment (JOSIE) under WMO sponsorship (WMO 1998b). All of the methods used in SHADOZ were tested against a calibrated spectroscopic instrument in chamber tests conducted in September 2000 at the Forschungszentrum in Jülich, Germany (information online at 1560 | OCTOBER 2004 FIG. 12. A sequence of soundings taken during INDOEX (1999) in which ozone pollution originating over south Asia is detected successively at the Maldives (Kaashidhoo Observatory), Nairobi (East Africa), and Ascension Island in the Atlantic. Black arrow points to progression of pollution from Indian Ocean over Africa then adding to the background ozone over Ascension in early March 1999. www.fz-juelich.de/icg/icg2/forschung/Josie). Preliminary analysis of results shows that instrument properties (manufacturer and concentration of the chemical solution) affect the ozone measurement and may account for small variations seen among SHADOZ stations when sonde total ozone is compared to a ground-based or satellite total ozone column (Thompson et al. 2003a). A WMO-sponsored field comparison of sondes was made in April 2004 in the Balloon Experiment on Standards for Ozone Sondes (BESOS; online at http://croc.gsfc.nasa. gov/besos). A large balloon was flown with a UV spectrophotometer and several types of sonde instruments. WMO’s GAW seeks to increase the number of ozonesonde stations in developing countries. Several SHADOZ stations provide a model for GAW’s “twinning” concept. Station operations, infrastructure, and gases are provided by the country in which the station is located. A partner country initiates sonde launches with a local agency, either a meteorological department or a space institute. Training, expend- ful launch of NASA’s Aura spacecraft, SHADOZ is well poised for validation of the four ozone sensors on board. ACKNOWLEDGMENTS. SHADOZ is supported by NASA’s Atmospheric Chemistry Modeling and Analysis Program (ACMAP) and the TOMS project. It would not exist without the generous and enthusiastic participation of the following: NASA’s Wallops Flight Facility, NOAA, National Space Development Agency of Japan (NASDA), Lembaga Penerbangan dan Antariksa Nasional (LAPAN, the National Institute of Aeronautics and Space of Indonesia), Instituto Nacional de Pesquisas Espaciais (INPE, the National Space Agency of Brazil), the South African Weather Service, the Swiss MeFIG. 13. Succession of nine soundings, 1-km mean mixing ratio, taken from teorological Agency, the Kenyan 6 to 11 Sep 2000, over Lusaka, Zambia (15.5∞∞ S, 28∞∞ E). Launches were made Meteorological Department, the during SAFARI-2000 campaign (Thompson et al. 2002); the data reside Royal Dutch Meteorological Inin the SHADOZ archive. A stable ozone pollution layer from 2 to 5 km stitute (KNMI), the University of coincides in most of these soundings with a double temperature inversion. the South Pacific (Suva, Fiji), Below the stable layer is the mixed layer. Five kilometers is a typical height CNRS, and the University of of a capping layer of tropical fair-weather cumulus. Réunion (France). We are grateful to the WMO Global Atmoables, and data processing are provided by the out- spheric Watch project for the opportunity to participate in side sponsor. In this manner the National Aeronau- the JOSIE intercomparison activity. Thanks to the BAMS tics and Space Administration (NASA) and the Bra- Atmospheric Chemistry Editor, two anonymous reviewers, zilian Space Agency (INPE) started the first tropical and B. N. Duncan (UMBC/GEST and GSFC) for their soundings in 1978 when the Nimbus-7 TOMS satel- comments. lite instrument was launched. Twinning between the Swiss Meteorological Agency and the Kenyan Meteorological Department led to the start of Nairobi sonde launches in 1996. Other examples in SHADOZ are the Japanese and Indonesian Space Agency operation on Java and the meteorological services of the Netherlands and Surinam at Paramaribo, Surinam. SUMMARY. More than 2000 ozone and PTU profiles archived between 1998 and 2003 are now at the SHADOZ Web site (online at http://croc.gsfc.nasa.gov/ shadoz). SHADOZ data have been used to improve the profile climatology for models and satellite algorithms, elucidate the structure of the zonal wave one in tropospheric ozone, and delineate characteristics of the ozone response to the QBO. With the successAMERICAN METEOROLOGICAL SOCIETY REFERENCES Baldwin, M. P., and Coauthors, 2001: The quasi-biennial oscillation. Rev. Geophys., 39, 179–229. Baldy, S., G. Ancellet, M. Bessafi, A. Badr, and D. Lan Sun Luk, 1996: Field observations of tropospheric vertical distribution of tropical ozone at a remote marine site in the southern hemisphere. J. Geophys. Res., 101, 23 835–23 849. Bey, I., D. J. Jacob, J. A. Logan, and R. M. Yantosca, 2001: Global modeling of tropospheric chemistry with assimilated meteorology: Model description and evaluation. J. Geophys. Res., 106, 23 073-23 095. Bojkov, R. D., and V. E. Fioletov, 1996: Total ozone variations in the tropical belt: An application for OCTOBER 2004 | 1561 quality of ground-based measurements. Meteor. Atmos. Phys., 58, 223–240. ——, and R. D. Hudson, L. Bishop, V. Fioletov, J. M. Russell III, R. S. Stolarski, O. Uchino, and C. S. Zerefos, 1999: Ozone variability and trends. WMO Global Ozone Research and Monitoring Project— Report No. 44: Scientific Assessment of Ozone Depletion. 1998, WMO. Bowman, K. P., 1989: Global patterns of the quasi-biennial oscillation in total ozone. J. Atmos. Sci., 46, 3328– 3343. Chatfield, R. B., and A. C. Delany, 1990: Convection links biomass burning to increased tropical ozone: However, models will tend to overpredict O 3. J. Geophys. Res., 95, 18 473–18 488. ——, H. Guan, A. M. Thompson, and J. C. Witte, 2004: Convective lofting links Indian Ocean air pollution to paradoxical south Atlantic ozone maxima. Geophys. Res. Lett., 31, L06103, doi:10.1029/ 2003GL018866. Cros, B., D. Nganga, A. Minga, J. Fishman, and V. Brackett, 1992: Distribution of tropospheric ozone at Brazzaville, Congo, determined from ozonesonde measurements. J. Geophys. Res., 97, 12 869–12 875. Crutzen, P. J., and Coauthors, 1985: Tropospheric chemical composition measurements in Brazil during the dry season. J. Atmos. Chem., 2, 233–256. Diab, R. D., A. Raghunandan, A. M. Thompson, and V. Thouret, 2003: Classification of tropospheric ozone profiles based on MOZAIC aircraft data. Atmos. Chem. Phys., 3, 705–732. Edwards, D. P., and Coauthors, 2003: Tropospheric ozone over the Atlantic: A satellite perspective. J. Geophys. Res., 108, 4237, doi:10.1029/2002JD002927. Fishman, J., and J. C. Larsen, 1987: Distribution of total ozone and stratospheric ozone in the tropics—Implications for the distribution of tropospheric ozone. J. Geophys. Res., 92, 6227–6634. ——, P. Minnis, and H. G. Reichle, 1986: Use of satellite data to study tropospheric ozone in the tropics. J. Geophys. Res., 91, 14 451–14 465. ——, K. Fakhruzzaman, B. Cros, and D. Nganga, 1991: Identification of widespread pollution in the southern hemisphere deduced from satellite analyses. Science, 252, 1693–1696. ——, J. M. Hoell, R. D. Bendura, R. J. McNeal, and V. W. J. H. Kirchhoff, 1996: NASA GTE TRACE A Experiment (September–October 1992): Overview. J. Geophys. Res., 101, 23 865–23 879. Fortuin, J. P. F., and H. Kelder, 1998: An ozone climatology based on ozonesonde and satellite measurements. J. Geophys. Res., 103, 31 709–31 734. 1562 | OCTOBER 2004 Garstang, M., P. D. Tyson, R. J. Swap, M. Edwards, P. Kållberg, and J. A. Lindesay, 1996: Horizontal and vertical transport of air over southern Africa. J. Geophys. Res., 101, 23 721–23 736. Heath, D. F., A. J. Krueger, H. A. Roeder, and B. D. Henderson, 1975: The solar back-scatter ultraviolet and total ozone mapping spectrometer (SBUV/ TOMS) for Nimbus G. Opt. Eng., 14, 323–331. Hollandsworth, S. M., K. P. Bowman, and R. D. McPeters, 1995: Observational study of the quasi-biennial oscillation in ozone. J. Geophys. Res., 100, 7347–7361. Jenkins, G. S., J.-H., Ryu, A. M. Thompson, and J. C. Witte, 2003: Linking horizontal and vertical transport of biomass fire emissions to the tropical Atlantic Ozone Paradox during the Northern hemisphere winter season: 1999. J. Geophys. Res., 108, 4745, doi:10.1029/2002JD003297. Kim, J.-H., R. D. Hudson, and A. M. Thompson, 1996: A new method of deriving time-averaged tropospheric column ozone over the tropics using TOMS radiances: Intercomparison and analysis. J. Geophys. Res., 101, 24 317–24 330. Kirchhoff, V. W. J. H., E. V. Browell, and G. L. Gregory, 1988: Ozone measurements in the troposphere of an Amazonian rainforest environment. J. Geophys. Res., 93, 15 850–15 860. Kley, D., P. J. Crutzen, H. G. J. Smit, H. Vömel, S. J. Oltmans, H. Grassl, and V. Ramanathan, 1996: Observations of near-zero ozone concentrations over the convective Pacific: Effects on air chemistry. Science, 274, 230–233. Komala, N., S. Saraspriya, K. Kita, and T. Ogawa, 1996: Tropospheric ozone behavior observed in Indonesia. Atmos. Environ., 30, 1851–1856. Komhyr, W., S. J. Oltmans, P. P. Franchois, W. F. J. Evans, and W. A. Mathews, 1989: The latitudinal distribution of ozone to 35 km altitude from ECC ozonesonde observations, 1985–1987. Ozone in the Atmosphere, R. D. Bojkov and P. Fabian, Eds., 147–150. Krishnamurti, T. N., M. C. Sinha, M. Kanamitsu, D. Oosterhof, H. Fuelberg, R. Chatfield, D. J. Jacob, and J. Logan, 1996: Passive tracer transport relevant to the TRACE-A experiment. J. Geophys. Res., 101, 23 889–23 907. Lawrence, M. G., P. J. Crutzen, P. J. Rasch, B. E. Eaton, and N. M. Mahowald, 1999: A model for studies of tropospheric photochemistry: Description, global distributions, and evaluation. J. Geophys. Res., 104, 26 245–26 277. Logan, J. A., 1999a: An analysis of ozonesonde data for the lower stratosphere. J. Geophys. Res., 104, 16 151– 16 170. ——, 1999b: An analysis of ozonesonde data for the troposphere: Recommendations for testing 3-D models and development of a gridded climatology for tropospheric ozone. J. Geophys. Res., 104, 16 115–16 149. ——, and V. W. J. H. Kirchhoff, 1986: Seasonal-variations of tropospheric ozone at Natal, Brazil. J. Geophys. Res., 91, 7875–7881. ——, and Coauthors, 2003: The quasibiennial oscillation in equatorial ozone as revealed by ozonesonde and satellite data. J. Geophys. Res., 108, 4244, doi:10.1029/ 2002JD002170. Martin, R. V., and Coauthors, 2002: Global model analysis of TOMS and in-situ observations of tropical tropospheric ozone. J. Geophys. Res., 107, 4437, doi:10.1029/2001JD001027. Moxim, W. J., and H. Levy, 2000: A model analysis of the tropical South Atlantic Ocean tropospheric ozone maximum: The interaction of transport and chemistry. J. Geophys. Res., 27, 2229–2232. Nash, J., and F. J. Schmidlin, 1987: Final report of the WMO International Radiosonde Intercomparison. WMO Instruments and Observing Systems Rep. 30, 123 pp. Newchurch, M. J., D. Sun, and J.-J. Kim, 2001: Zonal wave-1 structure in TOMS tropical stratospheric ozone. Geophys. Res. Lett., 28, 3151–3154. Olson, J. R., J. Fishman, V. W. J. H. Kirchhoff, D. Nganga, and B. Cros, 1996: An analysis of the distribution of O3 over the southern Atlantic region. J. Geophys. Res., 101, 24 083–24 094. Oltmans, S. J., and Coauthors, 2001: Ozone in the Pacific tropical troposphere from ozonesonde observations. J. Geophys. Res., 106, 32 503–32 526. Peters, W., M. Krol, F. Dentener, A. Thompson, and J. Lelieveld, 2002: Chemistry-transport modeling of the satellite observed distribution of tropical tropospheric ozone. Atmos. Chem. Phys., 2, 103–120. ——, ——, J. P. F. Fortuin, H. M. Kelder, C. R. Becker, A. M. Thompson, J. Lelieveld, and P. J. Crutzen, 2004: Tropospheric ozone over a tropical Atlantic station in the Northern Hemisphere: Paramaribo, Surinam (6N, 55W). Tellus, 56B, 21–34. Pickering, K. E., and Coauthors, 1996: Convective transport of biomass burning emissions over Brazil during TRACE. A. J. Geophys. Res., 101, 23 993–24 012. ——, and Coauthors, 2001: Trace gas transport and scavenging in PEM-Tropics B South Pacific convergence zone convection. J. Geophys. Res., 106, 32 591– 32 607. Piotrowicz, S. R., H. F. Bezdek, G. R. Harvey, M. Springer-Young, and K. J. Hanson, 1991: On the ozone minimum over the equatorial Pacific Ocean. J. Geophys. Res., 96, 18 679–18 687. AMERICAN METEOROLOGICAL SOCIETY Randel, W. J., and F. Wu, 1996: Isolation of the ozone QBO in SAGE II data by singular-value decomposition. J. Atmos. Sci., 53, 2546–2559. ——, R. S. Stolarski, D. M. Cunnold, J. A. Logan, M. J. Newchurch, and J. M. Zawodny, 1999: Trends in the vertical distribution of ozone. Science, 285, 1689– 1692. Reed, R. J., 1964: A tentative model of the 26-month oscillation in tropical latitudes. Quart. J. Roy. Meteor. Soc., 90, 441–446. Schmidlin, F. J., 1988: WMO International Radiosonde Intercomparison, Phase II, 1985: Wallops Island, Virginia USA. WMO Instruments and Observing Systems Rep. 29, 113 pp. Schoeberl, M. R., and P. A. Newman, 1995: A multiplelevel trajectory analysis of vortex filaments. J. Geophys. Res., 100, 25 801–25 815. Shiotani, M., 1992: Annual, quasi-biennial and El NinoSouthern Oscillation (ENSO) time-scale variations in Equatorial total ozone. J. Geophys. Res., 97, 7625– 7634. ——, and F. Hasebe, 1994: Stratospheric ozone variations in the equatorial region as seen in stratospheric aerosols and gas experiment data. J. Geophys. Res., 99, 14 575–14 584. Staehelin, J., A. Renaud, J. Bader, R. McPeters, P. Viatte, B. Hoegger, V. Bugnion, M. Giroud, and H. Schill, 1998: Total ozone series at Arosa (Switzerland): Homogenization and data comparison. J. Geophys. Res., 103, 5827–5841. Swap, R. J., H. J. Annegarn, J. T. Suttles, M. D. King, S. Platnick, J. L. Privette, and R. J. Scholes, 2003: Africa burning: A thematic analysis of the Southern African Regional Science Initiative (SAFARI-2000). J. Geophys. Res., 108, 8465, doi:10.1029/2002JD003747. Thompson, A. M., and Coauthors, 1993: SAGA-3 ozone observations and a photochemical model analysis of the marine boundary layer during SAGA-3. J. Geophys. Res., 98, 16 955–16 968. ——, and Coauthors, 1996: Where did tropospheric ozone over southern Africa and the tropical Atlantic come from in October 1992? Insights from TOMS, GTE/TRACE-A and SAFARI-92. J. Geophys. Res., 101, 24 251–24 278. ——, and Coauthors, 2000: A tropical Atlantic ozone paradox: Shipboard and satellite views of a tropospheric ozone maximum and wave-one in January– February 1999. Geophys. Res. Lett., 27, 3317–3320. ——, J. C. Witte, R. D. Hudson, H. Guo, J. R. Herman, and M. Fujiwara, 2001: Tropical tropospheric ozone and biomass burning. Science, 291, 2128–2132. ——, ——, M. T. Freiman, N. A. Phahlane, and G. J. R. Coetzee, 2002: Lusaka, Zambia (15.5S, 28E) during OCTOBER 2004 | 1563 SAFARI-2000: Convergence of local and imported ozone pollution. Geophys. Res. Lett., 29, 1976, doi:10.1029/2002GL015399. ——, and Coauthors, 2003a: Southern Hemisphere Additional Ozonesondes (SHADOZ) 1998–2000 tropical ozone climatology. 1. Comparison with TOMS and ground-based measurements. J. Geophys. Res., 108, 8238, doi:10.1029/2001JD000967. ——, and Coauthors, 2003b: Southern Hemisphere Additional Ozonesondes (SHADOZ) 1998-2000 tropical ozone climatology. 2. Tropospheric ozone variability and the zonal wave-one. J. Geophys. Res., 108, 8241, doi:10.1029/2002JD002241. Tyson, P. D., M. Garstang, A. M. Thompson, P. D’Abreton, R. D. Diab, and E. V. Browell, 1997: Atmospheric transport and photochemistry of ozone over central Southern Africa during the Southern 1564 | OCTOBER 2004 Africa Fire-Atmosphere Research Initiative. J. Geophys. Res., 102, 10 623–10 635. WMO, 1998a: SPARC/IOC/GAW assessment of trends in the vertical distribution of ozone. SPARC Rep. 1, WMO Global Ozone Research and Monitoring Project Rep. 43, 279 pp. ——, 1998b: JOSIE. Rep. 130, WMO Global Ozone Research and Monitoring Project Rep. TD926, 109 pp. Zachariasse, M., H. G. J. Smit, P. van Velthoven, and H. M. Kelder, 2001: Cross-tropopause exchange and interhemispheric transports into the tropical free troposphere over the Indian Ocean. J. Geophys. Res., 106, 28 441–28 452. Zawodny, J. M., and M. P. McCormick, 1991: Stratospheric Aerosol and Gas Experiment—II Measurements of the quasi-biennial oscillations in ozone and nitrogen dioxide. J. Geophys. Res., 96, 9371–9377.