scholarly journals Origins and characterization of CO and O<sub>3</sub> in the African upper troposphere

2021 ◽  
Vol 21 (19) ◽  
pp. 14535-14555
Author(s):  
Victor Lannuque ◽  
Bastien Sauvage ◽  
Brice Barret ◽  
Hannah Clark ◽  
Gilles Athier ◽  
...  

Abstract. Between December 2005 and 2013, the In-service Aircraft for a Global Observing System (IAGOS) program produced almost daily in situ measurements of CO and O3 between Europe and southern Africa. IAGOS data combined with measurements from the Infrared Atmospheric Sounding Interferometer (IASI) instrument aboard the Metop-A satellite (2008–2013) are used to characterize meridional distributions and seasonality of CO and O3 in the African upper troposphere (UT). The FLEXPART particle dispersion model and the SOFT-IO model which combines the FLEXPART model with CO emission inventories are used to explore the sources and origins of the observed transects of CO and O3. We focus our analysis on two main seasons: December to March (DJFM) and June to October (JJASO). These seasons have been defined according to the position of Intertropical Convergence Zone (ITCZ), determined using in situ measurements from IAGOS. During both seasons, the UT CO meridional transects are characterized by maximum mixing ratios located 10∘ from the position of the ITCZ above the dry regions inside the hemisphere of the strongest Hadley cell (132 to 165 ppb at 0–5∘ N in DJFM and 128 to 149 ppb at 3–7∘ S in JJASO) and decreasing values southward and northward. The O3 meridional transects are characterized by mixing ratio minima of ∼42–54 ppb at the ITCZ (10–16∘ S in DJFM and 5–8∘ N in JJASO) framed by local maxima (∼53–71 ppb) coincident with the wind shear zones north and south of the ITCZ. O3 gradients are strongest in the hemisphere of the strongest Hadley cell. IASI UT O3 distributions in DJFM have revealed that the maxima are a part of a crescent-shaped O3 plume above the Atlantic Ocean around the Gulf of Guinea. CO emitted at the surface is transported towards the ITCZ by the trade winds and then convectively uplifted. Once in the upper troposphere, CO-enriched air masses are transported away from the ITCZ by the upper branches of the Hadley cells and accumulate within the zonal wind shear zones where the maximum CO mixing ratios are found. Anthropogenic and fires both contribute, by the same order of magnitude, to the CO budget of the African upper troposphere. Local fires have the highest contribution and drive the location of the observed UT CO maxima. Anthropogenic CO contribution is mostly from Africa during the entire year, with a low seasonal variability. There is also a large contribution from Asia in JJASO related to the fast convective uplift of polluted air masses in the Asian monsoon region which are further westward transported by the tropical easterly jet (TEJ) and the Asian monsoon anticyclone (AMA). O3 minima correspond to air masses that were recently uplifted from the surface where mixing ratios are low at the ITCZ. The O3 maxima correspond to old high-altitude air masses uplifted from either local or long-distance area of high O3 precursor emissions (Africa and South America during all the year, South Asia mainly in JJASO) and must be created during transport by photochemistry.

2021 ◽  
Author(s):  
Victor Lannuque ◽  
Bastien Sauvage ◽  
Brice Barret ◽  
Hannah Clark ◽  
Gilles Athier ◽  
...  

Abstract. Between December 2005 and 2013, the In-service Aircraft for a Global Observing System (IAGOS) program produced almost daily in situ measurements of CO and O3 between Europe and southern Africa. IAGOS data combined with measurements from the IASI instrument onboard the Metop-A satellite (2008–2013) are used to characterize meridional distributions and seasonality of CO and O3 in the African upper troposphere (UT). The FLEXPART particle dispersion model and the SOFT-IO model which combines the FLEXPART model with CO emission inventories are used to explore the sources and origins of the observed transects of CO and O3. We focus our analysis on two main seasons: December to March (DJFM) and June to October (JJASO). These seasons have been defined according to the position of Intertropical Convergence Zone (ITCZ), determined using in situ measurements from IAGOS. During both seasons, the UT CO meridional transects are characterized by maximum mixing ratios located 10° from the position of the ITCZ above the dry regions inside the hemisphere of the strongest Hadley cell (132 to 165 ppb at 0–5° N in DJFM and 128 to 149 ppb at 3–7° S in JJASO), and decreasing values south- and north-ward. The O3 meridional transects are characterized by mixing ratio minima of ~ 42–54 ppb at the ITCZ (10–16° S in DJFM and 5–8° N in JJASO) framed by local maxima (~ 53–71 ppb) coincident with the wind shear zones North and South of the ITCZ. O3 gradients are strongest in the hemisphere of the strongest Hadley cell. IASI UT O3 distributions in DJFM have revealed that the maxima are a part of a crescent-shaped O3 plume above the Atlantic Ocean around the Gulf of Guinea. CO emitted at the surface is transported towards the ITCZ by the trade winds and then convectively uplifted. Once in the upper troposphere, CO enriched air masses are transported away from the ITCZ by the upper branches of the Hadley cells and accumulate within the zonal wind shear zones where the maximum CO mixing ratios are found. Anthropogenic and fires both contribute, by the same order of magnitude, to the CO budget of the African upper troposphere. Local fires have the highest contribution, drive the location of the observed UT CO maxima, and are related to the following transport pathway: CO emitted at the surface is transported towards the ITCZ by the trade winds and further convectively uplifted. Then UT CO enriched air masses are transported away from the ITCZ by the upper branches of the Hadley cells and accumulate within the zonal wind shear zones where the maxima are located. Anthropogenic CO contribution is mostly from Africa during the entire year, with a low seasonal variability, and is related to similar transport circulation than fire air masses. There is also a large contribution from Asia in JJASO related to the fast convective uplift of polluted air masses in the Asian monsoon region which are further westward transported by the tropical easterly jet (TEJ) and the Asian monsoon anticyclone (AMA). O3 minima correspond to air masses that were recently uplifted from the surface where mixing ratios are low at the ITCZ. The O3 maxima correspond to old high altitude air masses uplifted from either local or long distance area of high O3 precursor emissions (Africa and South America during all the year, South Asia mainly in JJASO), and must be created during transport by photochemistry. This analysis of meridional transects contribute to a better understanding of distributions of CO and O3 in the intertropical African upper troposphere and the processes which drive these distributions. Therefore, it provides a solid basis for comparison and improvement of models and satellite products in order to get the good O3 for the good reasons.


2010 ◽  
Vol 10 (7) ◽  
pp. 18063-18099
Author(s):  
M. von Hobe ◽  
J.-U. Grooß ◽  
G. Günther ◽  
P. Konopka ◽  
I. Gensch ◽  
...  

Abstract. Airborne in-situ observations of ClO in the tropics were made during the TROCCINOX (Aracatuba, Brasil, February 2005) and SCOUT-O3 (Darwin, Australia, November/December 2005) field campaigns. While during most flights significant amounts of ClO (≈10–20 parts per trillion, ppt) were present only in aged stratospheric air, instances of enhanced ClO mixing ratios of up to 40 ppt – significantly exceeding those expected from gas phase chemistry – were observed in air masses of a more tropospheric character. Most of these observations concur with low temperatures or with the presence of cirrus clouds (often both), suggesting that cirrus ice particles and/or liquid aerosol at low temperatures may promote significant heterogeneous chlorine activation in the tropical upper troposphere lower stratosphere (UTLS). In two case studies, particularly high levels of ClO observed were reproduced by chemistry simulations only under the assumption that significant denoxification had occurred in the observed air. At least for one of these flights, a significant denoxification is in contrast to the observed NO levels suggesting that the coupling of chlorine and nitrogen compounds in the tropical UTLS may not be completely understood.


2011 ◽  
Vol 11 (1) ◽  
pp. 241-256 ◽  
Author(s):  
M. von Hobe ◽  
J.-U. Grooß ◽  
G. Günther ◽  
P. Konopka ◽  
I. Gensch ◽  
...  

Abstract. Airborne in-situ observations of ClO in the tropics were made during the TROCCINOX (Aracatuba, Brazil, February 2005) and SCOUT-O3 (Darwin, Australia, November/December 2005) field campaigns. While during most flights significant amounts of ClO (≈10–20 parts per trillion, ppt) were present only in aged stratospheric air, instances of enhanced ClO mixing ratios of up to 40 ppt – significantly exceeding those expected from gas phase chemistry – were observed in air masses of a more tropospheric character. Most of these observations are associated with low temperatures or with the presence of cirrus clouds (often both), suggesting that cirrus ice particles and/or liquid aerosol at low temperatures may promote significant heterogeneous chlorine activation in the tropical upper troposphere lower stratosphere (UTLS). In two case studies, particularly high levels of ClO observed were reproduced by chemistry simulations only under the assumption that significant denoxification had occurred in the observed air. However, to reproduce the ClO observations in these simulations, O3 mixing ratios higher than observed had to be assumed, and at least for one of these flights, a significant denoxification is in contrast to the observed NO levels, suggesting that the coupling of chlorine and nitrogen compounds in the tropical UTLS may not be completely understood.


2020 ◽  
Author(s):  
Ralf Weigel ◽  
Christoph Mahnke ◽  
Manuel Baumgartner ◽  
Antonis Dragoneas ◽  
Bärbel Vogel ◽  
...  

Abstract. During the monsoon season of the year 2017 the airborne StratoClim mission took place in Kathmandu, Nepal with eight mission flights of the M-55 Geophysica in the upper troposphere/lower stratosphere (UT/LS) of the Asian Monsoon Anticyclone (AMA) over northern India, Nepal and Bangladesh. More than hundred events of New Particle Formation (NPF) were observed. In total, more than two hours of flight time were spent under NPF conditions as indicated by the abundant presence of ultrafine aerosols, i.e. with particle diameters dp smaller than 15 nm, which were in-situ detected by means of condensation nuclei counting techniques. Mixing ratios of ultrafine particles (nuf) of up to ~ 50000 mg−1 were measured at heights of 15–16 km (θ ≈ 370 K). NPF was most frequently observed at ~ 12–16 km altitude (θ ≈ 355–380 K) and mainly below the tropopause , but nuf remained elevated (~ 300–2000 mg−1) up to altitudes of ~ 17.5 km (θ ≈ 400 K) while under NPF conditions the fraction (f) of submicrometre-sized non-volatile particle residues (dp > 10 nm) remained below 50 %. At ~ 12–14 km (θ ≈ 355–365 K) the minimum of f (


2015 ◽  
Vol 8 (6) ◽  
pp. 2473-2489 ◽  
Author(s):  
J. Ungermann ◽  
J. Blank ◽  
M. Dick ◽  
A. Ebersoldt ◽  
F. Friedl-Vallon ◽  
...  

Abstract. The Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) is an airborne infrared limb imager combining a two-dimensional infrared detector with a Fourier transform spectrometer. It was operated aboard the new German Gulfstream G550 High Altitude LOng Range (HALO) research aircraft during the Transport And Composition in the upper Troposphere/lowermost Stratosphere (TACTS) and Earth System Model Validation (ESMVAL) campaigns in summer 2012. This paper describes the retrieval of temperature and trace gas (H2O, O3, HNO3) volume mixing ratios from GLORIA dynamics mode spectra that are spectrally sampled every 0.625 cm−1. A total of 26 integrated spectral windows are employed in a joint fit to retrieve seven targets using consecutively a fast and an accurate tabulated radiative transfer model. Typical diagnostic quantities are provided including effects of uncertainties in the calibration and horizontal resolution along the line of sight. Simultaneous in situ observations by the Basic Halo Measurement and Sensor System (BAHAMAS), the Fast In-situ Stratospheric Hygrometer (FISH), an ozone detector named Fairo, and the Atmospheric chemical Ionization Mass Spectrometer (AIMS) allow a validation of retrieved values for three flights in the upper troposphere/lowermost stratosphere region spanning polar and sub-tropical latitudes. A high correlation is achieved between the remote sensing and the in situ trace gas data, and discrepancies can to a large extent be attributed to differences in the probed air masses caused by different sampling characteristics of the instruments. This 1-D processing of GLORIA dynamics mode spectra provides the basis for future tomographic inversions from circular and linear flight paths to better understand selected dynamical processes of the upper troposphere and lowermost stratosphere.


2011 ◽  
Vol 11 (7) ◽  
pp. 3067-3091 ◽  
Author(s):  
C. Córdoba-Jabonero ◽  
M. Sorribas ◽  
J. L. Guerrero-Rascado ◽  
J. A. Adame ◽  
Y. Hernández ◽  
...  

Abstract. The synergetic use of meteorological information, remote sensing both ground-based active (lidar) and passive (sun-photometry) techniques together with backtrajectory analysis and in-situ measurements is devoted to the characterization of dust intrusions. A case study of air masses advected from the Saharan region to the Canary Islands and the Iberian Peninsula, located relatively close and far away from the dust sources, respectively, was considered for this purpose. The observations were performed over three Spanish geographically strategic stations within the dust-influenced area along a common dust plume pathway monitored from 11 to 19 of March 2008. A 4-day long dust event (13–16 March) over the Santa Cruz de Tenerife Observatory (SCO), and a linked short 1-day dust episode (14 March) in the Southern Iberian Peninsula over the Atmospheric Sounding Station "El Arenosillo" (ARN) and the Granada station (GRA) were detected. Meteorological conditions favoured the dust plume transport over the area under study. Backtrajectory analysis clearly revealed the Saharan region as the source of the dust intrusion. Under the Saharan air masses influence, AERONET Aerosol Optical Depth at 500 nm (AOD500) ranged from 0.3 to 0.6 and Ångström Exponent at 440/675 nm wavelength pair (AE440/675) was lower than 0.5, indicating a high loading and predominance of coarse particles during those dusty events. Lidar observations characterized their vertical layering structure, identifying different aerosol contributions depending on altitude. In particular, the 3-km height dust layer transported from the Saharan region and observed over SCO site was later on detected at ARN and GRA stations. No significant differences were found in the lidar (extinction-to-backscatter) ratio (LR) estimation for that dust plume over all stations when a suitable aerosol scenario for lidar data retrieval is selected. Lidar-retrieved LR values of 60–70 sr were obtained during the main dust episodes. These similar LR values found in all the stations suggest that dust properties were kept nearly unchanged in the course of its medium-range transport. In addition, the potential impact on surface of that Saharan dust intrusion over the Iberian Peninsula was evaluated by means of ground-level in-situ measurements for particle deposition assessment together with backtrajectory analysis. However, no connection between those dust plumes and the particle sedimentation registered at ground level is found. Differences on particle deposition processes observed in both Southern Iberian Peninsula sites are due to the particular dust transport pattern occurred over each station. Discrepancies between columnar-integrated and ground-level in-situ measurements show a clear dependence on height of the dust particle size distribution. Then, further vertical size-resolved observations are needed for evaluation of the impact on surface of the Saharan dust arrival to the Iberian Peninsula.


2009 ◽  
Vol 9 (13) ◽  
pp. 4407-4417 ◽  
Author(s):  
S. Lossow ◽  
M. Khaplanov ◽  
J. Gumbel ◽  
J. Stegman ◽  
G. Witt ◽  
...  

Abstract. The Hygrosonde-2 campaign took place on 16 December 2001 at Esrange/Sweden (68° N, 21° E) with the aim to investigate the small scale distribution of water vapour in the middle atmosphere in the vicinity of the Arctic polar vortex. In situ balloon and rocket-borne measurements of water vapour were performed by means of OH fluorescence hygrometry. The combined measurements yielded a high resolution water vapour profile up to an altitude of 75 km. Using the characteristic of water vapour being a dynamical tracer it was possible to directly relate the water vapour data to the location of the polar vortex edge, which separates air masses of different character inside and outside the polar vortex. The measurements probed extra-vortex air in the altitude range between 45 km and 60 km and vortex air elsewhere. Transitions between vortex and extra-vortex usually coincided with wind shears caused by gravity waves which advect air masses with different water vapour volume mixing ratios. From the combination of the results from the Hygrosonde-2 campaign and the first flight of the optical hygrometer in 1994 (Hygrosonde-1) a clear picture of the characteristic water vapour distribution inside and outside the polar vortex can be drawn. Systematic differences in the water vapour concentration between the inside and outside of the polar vortex can be observed all the way up into the mesosphere. It is also evident that in situ measurements with high spatial resolution are needed to fully account for the small-scale exchange processes in the polar winter middle atmosphere.


2014 ◽  
Vol 7 (3) ◽  
pp. 743-755 ◽  
Author(s):  
C. Dyroff ◽  
A. Zahn ◽  
S. Sanati ◽  
E. Christner ◽  
A. Rauthe-Schöch ◽  
...  

Abstract. A laser spectrometer for automated monthly measurements of methane (CH4) mixing ratios aboard the CARIBIC passenger aircraft is presented. The instrument is based on a commercial Fast Greenhouse Gas Analyser (FGGA, Los Gatos Res.), which was adapted to meet the requirements imposed by unattended airborne operation. It was characterised in the laboratory with respect to instrument stability, precision, cross sensitivity to H2O, and accuracy. For airborne operation, a calibration strategy is described that utilises CH4 measurements obtained from flask samples taken during the same flights. The precision of airborne measurements is 2 ppb for 10 s averages. The accuracy at aircraft cruising altitude is 3.85 ppb. During aircraft ascent and descent, where no flask samples were obtained, instrumental drifts can be less accurately determined and the uncertainty is estimated to be 12.4 ppb. A linear humidity bias correction was applied to the CH4 measurements, which was most important in the lower troposphere. On average, the correction bias was around 6.5 ppb at an altitude of 2 km, and negligible at cruising flight level. Observations from 103 long-distance flights are presented that span a large part of the northern hemispheric upper troposphere and lowermost stratosphere (UT/LMS), with occasional crossing of the tropics on flights to southern Africa. These accurate data mark the largest UT/LMS in-situ CH4 dataset worldwide. An example of a tracer-tracer correlation study with ozone is given, highlighting the possibility for accurate cross-tropopause transport analyses.


2002 ◽  
Vol 107 (D5) ◽  
pp. SOL 47-1-SOL 47-6 ◽  
Author(s):  
A. A. Viggiano ◽  
D. E. Hunton ◽  
Thomas M. Miller ◽  
John O. Ballenthin

2008 ◽  
Vol 8 (12) ◽  
pp. 3231-3246 ◽  
Author(s):  
B. Barret ◽  
P. Ricaud ◽  
C. Mari ◽  
J.-L. Attié ◽  
N. Bousserez ◽  
...  

Abstract. The transport pathways of carbon monoxide (CO) in the African Upper Troposphere (UT) during the West African Monsoon (WAM) is investigated through the assimilation of CO observations by the Aura Microwave Limb Sounder (MLS) in the MOCAGE Chemistry Transport Model (CTM). The assimilation setup, based on a 3-D First Guess at Assimilation Time (3-D-FGAT) variational method is described. Comparisons between the assimilated CO fields and in situ airborne observations from the MOZAIC program between Europe and both Southern Africa and Southeast Asia show an overall good agreement around the lowermost pressure level sampled by MLS (~215 hPa). The 4-D assimilated fields averaged over the month of July 2006 have been used to determine the main dynamical processes responsible for the transport of CO in the African UT. The studied period corresponds to the second AMMA (African Monsoon Multidisciplinary Analyses) aircraft campaign. At 220 hPa, the CO distribution is characterized by a latitudinal maximum around 5° N mostly driven by convective uplift of air masses impacted by biomass burning from Southern Africa, uplifted within the WAM region and vented predominantly southward by the upper branch of the winter hemisphere Hadley cell. Above 150 hPa, the African CO distribution is characterized by a broad maximum over northern Africa. This maximum is mostly controlled by the large scale UT circulation driven by the Asian Summer Monsoon (ASM) and characterized by the Asian Monsoon Anticyclone (AMA) centered at 30° N and the Tropical Easterly Jet (TEJ) on the southern flank of the anticyclone. Asian pollution uplifted to the UT over large region of Southeast Asia is trapped within the AMA and transported by the anticyclonic circulation over Northeast Africa. South of the AMA, the TEJ is responsible for the tranport of CO-enriched air masses from India and Southeast Asia over Africa. Using the high time resolution provided by the 4-D assimilated fields, we give evidence that the variability of the African CO distribution above 150 hPa and north of the WAM region is mainly driven by the synoptic dynamical variability of both the AMA and the TEJ.


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