Publications (74)45.9 Total impact
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Article: The impact of local surface changes in Borneo on atmospheric composition at wider spatial scales: coastal processes, land-use change and air quality.
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ABSTRACT: We present results from the OP3 campaign in Sabah during 2008 that allow us to study the impact of local emission changes over Borneo on atmospheric composition at the regional and wider scale. OP3 constituent data provide an important constraint on model performance. Treatment of boundary layer processes is highlighted as an important area of model uncertainty. Model studies of land-use change confirm earlier work, indicating that further changes to intensive oil palm agriculture in South East Asia, and the tropics in general, could have important impacts on air quality, with the biggest factor being the concomitant changes in NO(x) emissions. With the model scenarios used here, local increases in ozone of around 50 per cent could occur. We also report measurements of short-lived brominated compounds around Sabah suggesting that oceanic (and, especially, coastal) emission sources dominate locally. The concentration of bromine in short-lived halocarbons measured at the surface during OP3 amounted to about 7 ppt, setting an upper limit on the amount of these species that can reach the lower stratosphere.Philosophical Transactions of The Royal Society B Biological Sciences 11/2011; 366(1582):3210-24. · 6.40 Impact Factor -
Article: Representation of tropical deep convection in atmospheric models – Part 2: Tracer transport
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ABSTRACT: The tropical transport processes of 14 different models or model versions were compared, within the framework of the SCOUT-O3 (Stratospheric-Climate Links with Emphasis on the Upper Troposphere and Lower Stratosphere) project. The tested models range from the regional to the global scale, and include numerical weather prediction (NWP), chemical transport, and chemistry-climate models. Idealised tracers were used in order to prevent the model’s chemistry schemes from influencing the results substantially, so that the effects of modelled transport could be isolated. We find large differences in the vertical transport of very short-lived tracers (with a lifetime of 6 h) within the tropical troposphere. Peak convective outflow altitudes range from around 300 hPa to almost 100 hPa among the different models, and the upper tropospheric tracer mixing ratios differ by up to an order of magnitude. The timing of convective events is found to be different between the models, even among those which source their forcing data from the same NWP model (ECMWF). The differences are less pronounced for longer lived tracers, however they could have implications for modelling the halogen burden of the lowermost stratosphere through transport of species such as bromoform, or short-lived hydrocarbons into the lowermost stratosphere. The modelled tracer profiles are strongly influenced by the convective transport parameterisations, and different boundary layer mixing parameterisations also have a large impact on the modelled tracer profiles. Preferential locations for rapid transport from the surface into the upper troposphere are similar in all models, and are mostly concentrated over the western Pacific, the Maritime Continent and the Indian from around 300 hPa to almost 100 hPa among the different models, and the upper tropospheric tracer mixing ratios differ by up to an order of magnitude. The timing of convective events is found to be different between the models, even among those which source their forcing data from the same NWP model (ECMWF). The differences are less pronounced for longer lived tracers, however they could have implications for modelling the halogen burden of the lowermost stratosphere through transport of species such as bromoform, or short-lived hydrocarbons into the lowermost stratosphere. The modelled tracer profiles are strongly influenced by the convective transport parameterisations, and different boundary layer mixing parameterisations also have a large impact on the modelled tracer profiles. Preferential locations for rapid transport from the surface into the upper troposphere are similar in all models, and are mostly concentrated over the western Pacific, the Maritime Continent and the Indian Ocean. In contrast, models do not indicate that upward transport is highest over western Africa.Atmospheric Chemistry and Physics 08/2011; 11:8103-8131. · 4.88 Impact Factor -
Article: Representation of tropical deep convection in atmospheric models - Part 2: Tracer transport
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ABSTRACT: The tropical transport processes of 14 different models or model versions were compared, within the framework of the SCOUT-O3 (Stratospheric-Climate Links with Emphasis on the Upper Troposphere and Lower Stratosphere) project. The tested models range from the regional to the global scale, and include numerical weather prediction (NWP), chemical transport, and chemistry-climate models. Idealised tracers were used in order to prevent the model's chemistry schemes from influencing the results substantially, so that the effects of modelled transport could be isolated. We find large differences in the vertical transport of very short-lived tracers (with a lifetime of 6 h) within the tropical troposphere. Peak convective outflow altitudes range from around 300 hPa to almost 100 hPa among the different models, and the upper tropospheric tracer mixing ratios differ by up to an order of magnitude. The timing of convective events is found to be different between the models, even among those which source their forcing data from the same NWP model (ECMWF). The differences are less pronounced for longer lived tracers, however they could have implications for modelling the halogen burden of the lowermost stratosphere through transport of species such as bromoform, or short-lived hydrocarbons into the lowermost stratosphere. The modelled tracer profiles are strongly influenced by the convective transport parameterisations, and different boundary layer mixing parameterisations also have a large impact on the modelled tracer profiles. Preferential locations for rapid transport from the surface into the upper troposphere are similar in all models, and are mostly concentrated over the western Pacific, the Maritime Continent and the Indian Ocean. In contrast, models do not indicate that upward transport is highest over western Africa.ATMOSPHERIC CHEMISTRY AND PHYSICS 07/2011; 11:8103-8131. · 5.52 Impact Factor -
Article: The impact of local surface changes in Borneo on atmospheric composition at wider spatial scales: coastal processes, land use change and air quality
[show abstract] [hide abstract]
ABSTRACT: We present results from the OP3 campaign in Sabah during 2008 that allow us to study the impact of local emission changes over Borneo on atmospheric composition at the regional and wider scale. OP3 constituent data provide an important constraint on model performance. Treatment of boundary layer processes is highlighted as an important area of model uncertainty. Model studies of land-use change confirm earlier work, indicating that further changes to intensive oil palm agriculture in southeast Asia, and the tropics in general, could have important impacts on air quality, withthe biggest factor being the concomitant changes in NOx emissions. With the model scenarios used here, local increases in ozone of around 50 per cent could occur. We also report measurements of short-lived brominated compounds around Sabah suggesting that oceanic (and, especially, coastal) emission sources dominate locally. The concentration of bromine in short-lived halocarbons measured at the surface during OP3 amounted to about 7 ppt, setting an upper limit on the amount of these species that can reach the lower stratosphere.Philosophical Transactions of The Royal Society B. 01/2011; -
Article: Bromoform in the tropical boundary layer of the Maritime Continent during OP3
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ABSTRACT: We report measurements of bromoform made by gas chromatography during the OP3 campaign in 2008. Measurements were made simultaneously for a few days at the World Meteorological Organization (WMO) Global Atmospheric Watch (GAW) site in the Danum Valley, a rainforest location in Sabah, Borneo, and at a nearby coastal site at Kunak. Background values at Kunak were higher than those measured in the rainforest (2–5 ppt compared with 1 ppt) and excursions away from the background were very much higher, reaching 10 s of ppt. Measurements of C2Cl4, an industrial tracer, showed no significant difference in background at the two sites. Modelling using two different models can reproduce a number of the observed features. The data are consistent with a strong, local coastal source of bromoform in eastern Sabah and can be used to infer the strength of the source of bromoform in South East Asia. However, they provide only a very weak constraint on global emissions. The global model results highlight the difficulty for short-lived species of extrapolating limited duration, local measurements to a global source.Atmospheric Chemistry and Physics. 01/2011; -
Article: Results from the first national UK inter-laboratory calibration for very short-lived halocarbons
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ABSTRACT: Very short-lived halocarbons (VSLH) such as CH3I, CH2Br2 and CHBr3 provide an important source of reactive halogens to the atmosphere, however high spatial and seasonal variability in their ambient mixing ratios and sea-air fluxes gives rise to considerable uncertainty in global scale emission estimates. One solution to improve global flux estimates is to combine the multitude of individually published datasets to produce a database of collated global halocarbon observations. Some progress towards this has already been achieved through the HalOcAt (Halocarbons in the Ocean and Atmosphere) database initiative, however the absence of a common calibration scale for very short-lived halocarbons makes it difficult to distinguish true environmental variations from artefacts arising from differences between calibration methodologies. As such, the lack of inter-calibrations for both air and seawater measurements of very short-lived halocarbons has been identified as a major limitation to current estimations of the global scale impact of these reactive trace gases. Here we present the key findings from the first national UK inter-laboratory comparison for calibrations of the halocarbons CH3I, CH2Br2 and CHBr3. The aim of this inter-calibration was to provide transparency between halocarbon calibrations from major UK research institutions, an important step towards enabling all measurements from these institutions to be treated as one coherent integrated dataset for global source term parameterisations.Atmospheric Measurement Techniques Discussions. 01/2011; -
Article: μ Dirac: an autonomous instrument for halocarbon measurements
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ABSTRACT: We describe a new instrument ( μ Dirac) capable of measuring halocarbons in the atmosphere. Portability, power efficiency and autonomy were critical design requirements and the resulting instrument can be readily deployed unattended on a range of platforms: long duration balloon, aircraft, ship and ground-based stations. The instrument is a temperature programmed gas chromatograph with electron capture detector (GC-ECD). The design requirements led to μ Dirac being built in-house with several novel features. It currently measures a range of halocarbons (including short-lived tracers having biogenic and anthropogenic sources) with measurement precision relative standard deviations ranging from ± 1% (CCl<sub>4</sub>) to ± 9% (CH<sub>3</sub>I). The prototype instrument was first tested in 2005 and the instrument has been proved in the field on technically challenging aircraft and ground-based campaigns. Results from an aircraft and a ground-based deployment are described.Atmospheric Measurement Techniques. 01/2010; -
Article: μDirac: an autonomous instrument for halocarbon measurements
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ABSTRACT: We describe a new instrument (μDirac) capable of measuring halocarbons in the atmosphere. Portability, power efficiency and autonomy were critical design requirements and the resulting instrument can be readily deployed unattended on a range of platforms: long duration balloon, aircraft, ship and ground-based stations. The instrument is a temperature programmed gas chromatograph with electron capture detector (GC-ECD). The design requirements led to μDirac being built in-house with several novel features. It currently measures a range of halocarbons (including short-lived tracers having biogenic and anthropogenic sources) with measurement precision relative standard deviations ranging from ± 1% (CCl4) to ± 9% (CH3I). The prototype instrument was first tested in 2005 and the instrument has been proved in the field on technically challenging aircraft and ground-based campaigns. Results from an aircraft and a ground-based deployment are described.Atmospheric Measurement Techniques 01/2010; 3:507-521. · 3.34 Impact Factor -
Article: Bromoform in the tropical boundary layer of the Maritime Continent during OP3: the contrast between coast and rainforest
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ABSTRACT: We report measurements of bromoform made by gas chromatography during the OP3 campaign in 2008. Measurements were made simultaneously for a few days at the World Meteorological Organization (WMO) Global Atmospheric Watch (GAW) site in the Danum Valley, a rainforest location in Sabah, Borneo, and at a nearby coastal site at Kunak. Background values at Kunak were higher than those measured in the rainforest (2–5 ppt compared with 1 ppt) and excursions away from the background were very much higher, reaching 10s of ppt. Measurements of C2Cl4, an industrial tracer, showed no significant difference in background at the two sites. The data are consistent with a strong, local coastal source of bromoform in eastern Sabah. Modelling using two different models can reproduce many of the observed features. The bromoform data are consistent with a lower global source (190 Gg Br yr−1) than indicated by our recent measurements on Cape Verde (O'Brien et al., 2009) and point to the difficulty for short-lived species of extrapolating local measurements to a global source.Atmospheric Chemistry and Physics Discussions. 01/2010; -
Article: A closer look at Arctic ozone loss and polar stratospheric clouds
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ABSTRACT: The empirical relationship found between column-integrated Arctic ozone loss and the potential volume of polar stratospheric clouds inferred from meteorological analyses is recalculated in a self-consistent manner using the ERA Interim reanalyses. The relationship is found to hold at different altitudes as well as in the column. The use of a PSC formation threshold based on temperature dependent cold aerosol formation makes little difference to the original, empirical relationship. Analysis of the photochemistry leading to the ozone loss shows that activation is limited by the photolysis of nitric acid. This step produces nitrogen dioxide which is converted to chlorine nitrate which in turn reacts with hydrogen chloride on any polar stratospheric clouds to form active chlorine. The rate-limiting step is the photolysis of nitric acid: this occurs at the same rate every year and so the interannual variation in the ozone loss is caused by the extent and persistence of the polar stratospheric clouds. In early spring the ozone loss rate increases as the solar insolation increases the photolysis of the chlorine monoxide dimer in the near ultraviolet. However the length of the ozone loss period is determined by the photolysis of nitric acid which also occurs in the near ultraviolet. As a result of these compensating effects, the amount of the ozone loss is principally limited by the extent of original activation rather than its timing. In addition a number of factors, including the vertical changes in pressure and total inorganic chlorine as well as denitrification and renitrification, offset each other. As a result the extent of original activation is the most important factor influencing ozone loss. These results indicate that relatively simple parameterisations of Arctic ozone loss could be developed for use in coupled chemistry climate models.Atmospheric Chemistry and Physics. 01/2010; -
Article: Tropical deep convection and its impact on composition in global and mesoscale models – Part 2: Tracer transport
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ABSTRACT: The tropical transport processes of 14 different models or model versions were compared, within the framework of the SCOUT-O3 (Stratospheric-Climate Links with Emphasis on the Upper Troposphere and Lower Stratosphere) project. The tested models range from the regional to the global scale, and include numerical weather prediction (NWP), chemistry transport, and climate chemistry models. Idealised tracers were used in order to prevent the model's chemistry schemes from influencing the results substantially, so that the effects of modelled transport could be isolated. We find large differences in the vertical transport of very short lived tracers (with a lifetime of 6 hours) within the tropical troposphere. Peak convective outflow altitudes range from around 300 hPa to almost 100 hPa among the different models, and the upper tropospheric tracer mixing ratios differ by up to an order of magnitude. The timing of convective events is found to differ between the models, even among those which source their forcing data from the same NWP model (ECMWF). The differences are less pronounced for longer lived tracers, however they could have implications for the modelling of the halogen burden of the lowermost stratosphere through species such as bromoform, or for the transport of short lived hydrocarbons into the lowermost stratosphere. The modelled tracer profiles are found to be strongly influenced by the convective transport parameterisations, and boundary layer mixing parameterisations of the models. The location of rapid transport into the upper troposphere is similar among the models, and is mostly concentrated over the western Pacific, the Maritime Continent and the Indian Ocean. In contrast, none of the models indicates significant enhancement in upward transport over western Africa. The mean mixing ratios of an idealised CO like tracer in the upper tropical troposphere are found to be sensitive to the surface CO mixing ratios in the regions with the most active convection, revealing the importance of correctly modelling both the location of convective transport and the geographical pollutant emission patterns.Atmospheric Chemistry and Physics Discussions. 01/2010; -
Article: An introduction to the SCOUT-AMMA stratospheric aircraft, balloons and sondes campaign in West Africa, August 2006: rationale and roadmap
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ABSTRACT: A multi-platform field measurement campaign involving aircraft and balloons took place over West Africa between 26 July and 25 August 2006, in the frame of the concomitant AMMA Special Observing Period and SCOUT-O3 African tropical activities. Specifically aiming at sampling the upper troposphere and lower stratosphere, the high-altitude research aircraft M55 Geophysica was deployed in Ouagadougou (12.3° N, 1.7° W), Burkina Faso, in conjunction with the German D-20 Falcon, while a series of stratospheric balloon and sonde flights were conducted from Niamey (13.5° N, 2.0° E), Niger. The stratospheric aircraft and balloon flights intended to gather experimental evidence for a better understanding of large scale transport, assessing the effect of lightning on NOx production, and studying the impact of intense mesoscale convective systems on water, aerosol, dust and chemical species in the upper troposphere and lower stratosphere. The M55 Geophysica carried out five local and four transfer flights between southern Europe and the Sahel and back, while eight stratospheric balloons and twenty-nine sondes were flown from Niamey. These experiments allowed a characterization of the tropopause and lower stratosphere of the region. We provide here an overview of the campaign activities together with a description of the general meteorological situation during the flights and a summary of the observations accomplished.Atmospheric Chemistry and Physics. 01/2010; 10(2010):2237-2256. -
Article: Bromocarbons in the tropical marine boundary layer at the Cape Verde Observatory – measurements and modelling
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ABSTRACT: A new gas chromatograph was used to make measurements of halocarbons at the Cape Verde observatory during late May and early June 2007. The instrument demonstrated its potential for long-term autonomous measurements. Bromoform (CHBr3) exhibits the most variability of all the halocarbons observed, ranging from a background concentration of about 4 ppt to a maximum of >40 ppt during the course of the measurement period. Dibromomethane (CH2Br2) correlates well with CHBr3, suggesting a common regional source. Methyl iodide (CH3I) does not correlate with these bromocarbons, with base levels of around 1–2 ppt and some periods of much higher mixing ratios. Model studies with published bromocarbon emission rates do not reproduce the observations. Local emission magnitudes and CHBr3:CH2Br2 ratios must be increased more in line with the recent observations of Yokouchi et al. (2005) to improve the model to measurement comparison. Even when the model reproduces the observed bromocarbons, modelled BrO is much less than recent tropical observations (Read et al., 2008). A sea salt source seems the likely explanation. When high BrO is reproduced, the model agrees much better with the observed ozone changes, including diurnal variation, during the measurement period but it is suggested that a representation of iodine chemistry in the model is also required.Atmospheric Chemistry and Physics Discussions. 01/2009; -
Article: The SCOUT-O3 Darwin Aircraft Campaign: rationale and meteorology
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ABSTRACT: An aircraft measurement campaign involving the Russian high-altitude aircraft M55 Geophysica and the German DLR Falcon was conducted in Darwin, Australia in November and December 2005 as part of the European integrated project SCOUT-O3. The overall objectives of the campaign were to study the transport of trace gases through the tropical tropopause layer (TTL), mechanisms of dehydration close to the tropopause, and the role of deep convection in these processes. In this paper a detailed roadmap of the campaign is presented, including rationales for each flight, and an analysis of the local and large-scale meteorological context in which they were embedded. The campaign took place during the pre-monsoon season which is characterized by a pronounced diurnal evolution of deep convection including a mesoscale system over the Tiwi Islands north of Darwin known as "Hector". This allowed studying in detail the role of deep convection in structuring the tropical tropopause region, in situ sampling convective overshoots above storm anvils, and probing the structure of anvils and cirrus clouds by Lidar and a suite of in situ instruments onboard the two aircraft. The large-scale flow during the first half of the campaign was such that local flights, away from convection, sampled air masses downstream of the "cold trap" region over Indonesia. Abundant cirrus clouds enabled the study of active dehydration, in particular during two TTL survey flights. The campaign period also encompassed a Rossby wave breaking event transporting stratospheric air to the tropical middle troposphere and an equatorial Kelvin wave modulating tropopause temperatures and hence the conditions for dehydration.Atmospheric Chemistry and Physics 01/2009; · 4.88 Impact Factor -
Article: An overview of the SCOUT-AMMA stratospheric aircraft, balloons and sondes campaign in West Africa, August 2006: rationale, roadmap and highlights
[show abstract] [hide abstract]
ABSTRACT: A multi-platform field measurement campaign involving aircraft and balloons took place over West Africa between 26 July and 25 August 2006, in the frame of the concomitant AMMA Special Observing Period and SCOUT-O3 African tropical activities. Specifically aiming at sampling the upper troposphere and lower stratosphere, the high-altitude research aircraft M55 Geophysica was deployed in Ouagadougou (12.3° N, 1.7° W), Burkina Faso, in conjunction with the German D-20 Falcon, while a series of stratospheric balloon and sonde flights were conducted from Niamey (13.5° N, 2.0° E), Niger. The stratospheric aircraft and balloon flights intended to gather experimental evidence for a better understanding of large scale transport, assessing the effect of lightning on NOx production, and studying the impact of intense mesoscale convective systems on water, aerosol, dust and chemical species in the upper troposphere and lower stratosphere. The M55 Geophysica carried out five local and four transfer flights between southern Europe and the Sahel and back, while eight stratospheric balloons and twenty-nine sondes were flown from Niamey. These experiments allowed a characterization of the tropopause and lower stratosphere of the region. We provide here an overview of the campaign activities together with a description of the general meteorological situation during the flights and a summary of the observations accomplished.Atmospheric Chemistry and Physics Discussions. 01/2009; -
Article: μDirac: an autonomous instrument for halocarbon measurements
[show abstract] [hide abstract]
ABSTRACT: We describe a new instrument (μDirac) capable of measuring halocarbons in the atmosphere. Portability, power efficiency and autonomy were critical requirements in the design, and the resulting instrument can be readily deployed unattended on a range of platforms: long duration balloon, aircraft, ship and ground based stations. The instrument is a temperature programmed gas chromatograph with electron capture detector (GC-ECD). The design requirements led to μDirac being built in-house with several novel features. It currently measures a range of halocarbons (CFCs and shorter-lived halocarbons having biogenic and anthropogenic sources) with measurement precisions ranging from ∼1% sd (CCl4) to ∼9% sd (CH3I). Since the prototype instrument was first tested in 2005 the instrument has been proved in the field on technically challenging aircraft and ground based campaigns. Results from one aircraft and two ground-based deployments are described.Atmospheric Measurement Techniques Discussions. 01/2009; -
Article: Ozone trends at northern mid- and high latitudes – a European perspective
Annales Geophysicae 01/2008; 26(5):1207-1220. · 1.84 Impact Factor -
Article: Observations of an atmospheric chemical equator and its implications for the tropical warm pool region
Journal of Geophysical Research-Atmospheres. 01/2008; 113(D20). -
Article: Seasonal and inter-annual variations in troposphere-to-stratosphere transport from the tropical tropopause layer
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ABSTRACT: In an earlier study of troposphere-to-stratosphere transport (TST) via the tropical tropopause layer (TTL), we found that the vast majority of air parcels undergoing TST from the base of the TTL enter the extratropical lowermost stratosphere quasi-horizontally and show little or no regional preference with regards to origin in the TTL or entry into the stratosphere. We have since repeated the trajectory calculations – originally limited to a single Northern Hemisphere winter period – in a variety of months and years to assess how robust our earlier findings are to change of timing. To first order, we find that the main conclusions hold, irrespective of the season, year and phase of the El Niño Southern Oscillation (ENSO). We also explore: the distribution of TST between the Northern and Southern Hemispheres; the sensitivity of modelled TST to the definition of the tropopause; and the routes by which air parcels undergo transport exclusively to the stratospheric overworld. Subject to a dynamical definition of the tropopause, we identify a strong bias towards TST in the Southern Hemisphere, particularly during the Northern Hemisphere summer. The thermal tropopause, defined according to the World Meteorological Organization, lies above the dynamical tropopause throughout the extratropics. Inevitably, on switching to the thermal definition, we calculate much less transport across the tropopause, particularly in the subtropics, which could be important with regards to interpretation of processes affecting ozone chemistry in the extratropical lowermost stratosphere (ELS). In contrast to the rather homogeneous nature of TST into the ELS, we find that transport to the overworld takes place from relatively well-defined regions of the TTL, predominantly above the West Pacific and Indonesia, except for an El Niño period in which most transport takes place from regions above the East Pacific and South America.Atmospheric Chemistry and Physics. 01/2008; -
Article: An overview of the HIBISCUS campaign
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ABSTRACT: HIBISCUS was a field campaign for investigating the impact of deep convection on the Tropical Tropopause Layer (TTL) and the Lower Stratosphere, which took place during the Southern Hemisphere summer in February–March 2004 in the State of São Paulo, Brazil. Its objective was to provide a set of new observational data on meteorology, tracers of horizontal and vertical transport, water vapour, clouds, and chemistry in the tropical UT/LS from balloon observations at local scale over a land convective area, as well as at global scale using circumnavigating long-duration balloons. Overall, the composition of the TTL, the region between 14 and 19 km of intermediate lapse rate between the almost adiabatic upper troposphere and the stable stratosphere, appears highly variable. Tracers and ozone measurements performed at both the local and the global scale indicate a strong quasi-horizontal isentropic exchange with the lowermost mid-latitude stratosphere suggesting that the barrier associated to the tropical jet is highly permeable at these levels in summer. But the project also provides clear indications of strong episodic updraught of cold air, short-lived tracers, low ozone, humidity and ice particles across the lapse rate tropopause at about 15 km, up to 18 or 19 km at 420–440 K potential levels in the lower stratosphere, suggesting that, in contrast to oceanic convection penetrating little the stratosphere, fast daytime developing land convective systems could be a major mechanism in the troposphere-stratosphere exchange at the global scale. The present overview is meant to provide the background of the project, as well as overall information on the instrumental tools available, on the way they have been used within the highly convective context of the South Atlantic Convergence Zone, and a brief summary of the results, which will be detailed in several other papers of this special issue.Atmospheric Chemistry and Physics Discussions. 01/2007;
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2000–2006
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University of Cambridge
- • Centre for Atmospheric Science
- • Department of Chemistry
Cambridge, ENG, United Kingdom
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