scholarly journals Pollution trace gas distributions and their transport in the Asian monsoon upper troposphere and lowermost stratosphere during the StratoClim campaign 2017

2020 ◽  
Author(s):  
Sören Johansson ◽  
Michael Höpfner ◽  
Oliver Kirner ◽  
Ingo Wohltmann ◽  
Silvia Bucci ◽  
...  
Keyword(s):  
Large Scale ◽  
Asian Summer Monsoon ◽  
Trace Gases ◽  
Local Maximum ◽  
Horizontal Resolution ◽  
Convective Transport ◽  
Trace Gas ◽  
Air Masses ◽  
Upper Troposphere ◽  
Simulation Results

Abstract. We present the first high resolution measurements of pollutant trace gases in the Asian Summer Monsoon Upper Troposphere and Lowermost Stratosphere (UTLS) from the Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) during the StratoClim (Stratospheric and upper tropospheric processes for better climate predictions) campaign with base in Kathamandu, Nepal, 2017. Measurements of peroxyacetyl nitrate (PAN), acetylene (C2H2), and formic acid (HCOOH) show strong local enhancements up to altitudes of 16 km. More than 500 pptv of PAN, more than 200 pptv of C2H2, and more than 200 pptv of HCOOH are observed. An observed local maximum of PAN and C2H2 at altitudes up to 18 km, reaching to the lowermost stratosphere, instead has been transported for a longer time. A local minimum of HCOOH is correlated with a maximum of ammonia (NH3), which suggests different wash out efficiencies of these species in the same air masses. To study the influence of convective transport to the measured pollution trace gas occurrences in detail, a trajectory analysis of the models ATLAS and TRACZILLA examined backward trajectories, starting at geolocations of GLORIA measurements with enhanced pollution trace gases. Both trajectory schemes implemented advanced techniques for detection of convective events. These convective events along trajectories leading to GLORIA measurements with enhanced pollutants are located close to regions, where satellite measurements by OMI show enhanced tropospheric columns of nitrogen dioxide (NO2) in the days prior to the observation. As an application of these highly resolved measurements, a comparison to the atmospheric models CAMS and EMAC is performed. It is demonstrated that these simulation results are able to reproduce large scale structures of the pollution trace gas distributions if the convective influence on the measured air masses is captured by the meteorological fields used by these simulations. Both models do not have sufficient horizontal resolution to capture all the convective events that are necessary to reproduce the fine structures measured by GLORIA. To investigate the influence of the strength of non-methane volatile organic compounds (NMVOCs) emissions in the EMAC model, sensitivity studies with artificially enhanced NMVOC emissions are performed. With these enhanced emissions, the simulation results succeed to reproduce the measured peak values of the pollutants, but do not improve the comparison of spatial distributions.

scholarly journals Pollution trace gas distributions and their transport in the Asian monsoon upper troposphere and lowermost stratosphere during the StratoClim campaign 2017

2020 ◽  
Vol 20 (23) ◽  
pp. 14695-14715
Author(s):  
Sören Johansson ◽  
Michael Höpfner ◽  
Oliver Kirner ◽  
Ingo Wohltmann ◽  
Silvia Bucci ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Large Scale ◽  
Trajectory Analysis ◽  
Asian Summer Monsoon ◽  
Trace Gas ◽  
Ozone Monitoring Instrument ◽  
Air Masses ◽  
Upper Troposphere ◽  
Mixing Ratios ◽  
Monitoring Service

Abstract. We present the first high-resolution measurements of pollutant trace gases in the Asian summer monsoon upper troposphere and lowermost stratosphere (UTLS) from the Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) during the StratoClim (Stratospheric and upper tropospheric processes for better climate predictions) campaign based in Kathmandu, Nepal, 2017. Measurements of peroxyacetyl nitrate (PAN), acetylene (C2H2), and formic acid (HCOOH) show strong local enhancements up to altitudes of 16 km. More than 500 pptv of PAN, more than 200 pptv of C2H2, and more than 200 pptv of HCOOH are observed. Air masses with increased volume mixing ratios of PAN and C2H2 at altitudes up to 18 km, reaching to the lowermost stratosphere, were present at these altitudes for more than 10 d, as indicated by trajectory analysis. A local minimum of HCOOH is correlated with a previously reported maximum of ammonia (NH3), which suggests different washout efficiencies of these species in the same air masses. A backward trajectory analysis based on the models Alfred Wegener InsTitute LAgrangian Chemistry/Transport System (ATLAS) and TRACZILLA, using advanced techniques for detection of convective events, and starting at geolocations of GLORIA measurements with enhanced pollution trace gas concentrations, has been performed. The analysis shows that convective events along trajectories leading to GLORIA measurements with enhanced pollutants are located close to regions where satellite measurements by the Ozone Monitoring Instrument (OMI) indicate enhanced tropospheric columns of nitrogen dioxide (NO2) in the days prior to the observation. A comparison to the global atmospheric models Copernicus Atmosphere Monitoring Service (CAMS) and ECHAM/MESSy Atmospheric Chemistry (EMAC) has been performed. It is shown that these models are able to reproduce large-scale structures of the pollution trace gas distributions for one part of the flight, while the other part of the flight reveals large discrepancies between models and measurement. These discrepancies possibly result from convective events that are not resolved or parameterized in the models, uncertainties in the emissions of source gases, and uncertainties in the rate constants of chemical reactions.

Trace gases and organic aerosol at a rural site in Vietnam during large scale biomass burning

2021 ◽  
Author(s):  
Simone M. Pieber ◽  
Dac-Loc Nguyen ◽  
Hendryk Czech ◽  
Stephan Henne ◽  
Nicolas Bukowiecki ◽  
...  
Keyword(s):  
Air Quality ◽  
Chemical Composition ◽  
Biomass Burning ◽  
Large Scale ◽  
Trace Gases ◽  
Organic Aerosol ◽  
Trace Gas ◽  
Rural Site ◽  
Air Masses ◽  
Mixing Ratios

<p>Open biomass burning (BB) is a globally widespread phenomenon. The fires release pollutants, which are harmful for human and ecosystem health and alter the Earth's radiative balance. Yet, the impact of various types of BB on the global radiative forcing remains poorly constrained concerning greenhouse gas emissions, BB organic aerosol (OA) chemical composition and related light absorbing properties. Fire emissions composition is influenced by multiple factors (e.g., fuel and thereby vegetation-type, fuel moisture, fire temperature, available oxygen). Due to regional variations in these parameters, studies in different world regions are needed. Here we investigate the influence of seasonally recurring BB on trace gas concentration and air quality at the regional Global Atmosphere Watch (GAW) station Pha Din (PDI) in rural Northwestern Vietnam. PDI is located in a sparsely populated area on the top of a hill (1466 m a.s.l.) and is well suited to study the large-scale fires on the Indochinese Peninsula, whose pollution plumes are frequently transported towards the site [1]. We present continuous trace gas observations of CO<sub>2</sub>, CH<sub>4</sub>, CO, and O<sub>3</sub> conducted at PDI since 2014 and interpret the data with atmospheric transport simulations. Annually recurrent large scale BB leads to hourly time-scale peaks CO mixing ratios at PDI of 1000 to 1500 ppb around every April since the start of data collection in 2014. We complement this analysis with carbonaceous PM<sub>2.5 </sub>chemical composition analyzed during an intensive campaign in March-April 2015. This includes measurements of elemental and organic carbon (EC/OC) and more than 50 organic markers, such as sugars, PAHs, fatty acids and nitro-aromatics [2]. For the intensive campaign, we linked CO, CO<sub>2</sub>, CH<sub>4</sub> and O<sub>3</sub> mixing ratios to a statistical classification of BB events, which is based on OA composition. We found increased CO and O<sub>3</sub> levels during medium and high BB influence during the intensive campaign. A backward trajectory analysis confirmed different source regions for the identified periods based on the OA cluster. Typically, cleaner air masses arrived from northeast, i.e., mainland China and Yellow sea during the intensive campaign. The more polluted periods were characterized by trajectories from southwest, with more continental recirculation of the medium cluster, and more westerly advection for the high cluster. These findings highlight that BB activities in Northern Southeast Asia significantly enhances the regional OA loading, chemical PM<sub>2.5 </sub>composition and the trace gases in northwestern Vietnam. The presented analysis adds valuable data on air quality in a region of scarce data availability.</p><p> </p><p><strong>REFERENCES</strong></p><p>[1] Bukowiecki, N. et al. Effect of Large-scale Biomass Burning on Aerosol Optical Properties at the GAW Regional Station Pha Din, Vietnam. AAQR. 19, 1172–1187 (2019).</p><p>[2] Nguyen, D. L, et al. Carbonaceous aerosol composition in air masses influenced by large-scale biomass burning: a case-study in Northwestern Vietnam. ACPD., https://doi.org/10.5194/acp-2020-1027, in review, 2020.</p>

scholarly journals Seasonal characteristics of trace gas transport into the extratropical upper troposphere and lower stratosphere

2019 ◽  
Vol 19 (10) ◽  
pp. 7073-7103 ◽  
Author(s):  
Yoichi Inai ◽  
Ryo Fujita ◽  
Toshinobu Machida ◽  
Hidekazu Matsueda ◽  
Yousuke Sawa ◽  
...  
Keyword(s):  
Lower Stratosphere ◽  
Trace Gases ◽  
Source Region ◽  
Lower Troposphere ◽  
Trace Gas ◽  
Air Masses ◽  
Backward Trajectories ◽  
Upper Troposphere ◽  
Passive Behavior ◽  
Seasonal Characteristics

Abstract. To investigate the seasonal characteristics of trace gas distributions in the extratropical upper troposphere and lower stratosphere (ExUTLS) as well as stratosphere–troposphere exchange processes, origin fractions of air masses originating in the stratosphere, tropical troposphere, midlatitude lower troposphere (LT), and high-latitude LT in the ExUTLS are estimated using 10-year backward trajectories calculated with European Centre for Medium-Range Weather Forecasts (ECMWF) ERA-Interim data as the meteorological input. Time series of trace gases obtained from ground-based and airborne observations are incorporated into the trajectories, thus reconstructing spatiotemporal distributions of trace gases in the ExUTLS. The reconstructed tracer distributions are analyzed with the origin fractions and the stratospheric age of air (AoA) estimated using the backward trajectories. The reconstructed distributions of SF6 and CO2 in the ExUTLS are linearly correlated with those of AoA because of their chemically passive behavior and quasi-stable increasing trends in the troposphere. Distributions of CH4, N2O, and CO are controlled primarily by chemical decay along the transport path from the source region via the stratosphere and subsequent mixing of such stratospheric air masses with tropospheric air masses in the ExUTLS.

scholarly journals Upper tropospheric CH<sub>4</sub> and CO affected by the South Asian summer monsoon during OMO

2018 ◽  
Author(s):  
Laura Tomsche ◽  
Andrea Pozzer ◽  
Narendra Ojha ◽  
Uwe Parchatka ◽  
Jos Lelieveld ◽  
...  
Keyword(s):  
South Asian ◽  
Asian Summer Monsoon ◽  
Trace Gases ◽  
South Asian Summer Monsoon ◽  
The South ◽  
Transport Pathways ◽  
Air Masses ◽  
Upper Troposphere ◽  
Asian Summer

Abstract. The Asian monsoon anticyclone (AMA) is a yearly recurring phenomenon in the northern hemispheric upper troposphere and lower stratosphere. It is connected to the South Asian summer monsoon, and the circulation extends approximately across 20°–120° E and 15°–40° N longitude-latitude. It has a clearly observable signature due to vertical transport of polluted air masses from the surface to the upper troposphere by the monsoon convection. However, the transport pathways and the fate of pollutants in the upper troposphere are not yet fully understood. As pollution emissions in South Asia are increasing, changes in the chemical composition of the AMA can be expected. We performed in situ measurements of carbon monoxide (CO) and methane (CH4) in the region of monsoon outflow and in background air in the upper troposphere (Mediterranean, Arabian Peninsula, Arabian Sea) by optical absorption spectroscopy on board the German High Altitude and Long range (HALO) research aircraft during the OMO (Oxidation Mechanism Observations) mission in summer 2015. We identified the transport pathways and the origin of the trace gases with back trajectories, calculated with the Lagrangian particle dispersion model FLEXPART, and we compared the in situ data with simulations of the atmospheric chemistry general circulation model EMAC. CH4 and CO mixing ratios were found to be enhanced within the AMA, on average by 72.1 ppb and 20.1 ppb, respectively, originating in the South Asian region (Indio-Gangetic Plain, North East India, Bangladesh and Bay of Bengal). It appears that CH4 is an ideal monsoon tracer in the upper troposphere due to its extended lifetime and the strong South Asian emissions. Furthermore, we used the measurements and model results to study the dynamics of the AMA, with an emphasis on the southern and western areas within the upper troposphere. For example, we distinguished four AMA modes based on different meteorological conditions. During one occasion we observed that under the influence of dwindling flow the transport barrier between the anticyclone and its surroundings weakened, expelling air masses from the AMA. The trace gases exhibited a distinct fingerprint of the AMA, and we also found that CH4 accumulated over the course of the OMO campaign.

scholarly journals Characterization of non-methane hydrocarbons in Asian summer monsoon outflow observed by the CARIBIC aircraft

2011 ◽  
Vol 11 (2) ◽  
pp. 503-518 ◽  
Author(s):  
A. K. Baker ◽  
T. J. Schuck ◽  
F. Slemr ◽  
P. van Velthoven ◽  
A. Zahn ◽  
...  
Keyword(s):  
Carbon Monoxide ◽  
Summer Monsoon ◽  
Fossil Fuels ◽  
Asian Summer Monsoon ◽  
Trace Gases ◽  
Northern Region ◽  
Monsoon Circulation ◽  
Upper Troposphere ◽  
Mixing Ratios ◽  
Asian Summer

Abstract. Between April and December 2008 the CARIBIC commercial aircraft conducted monthly measurement flights between Frankfurt, Germany and Chennai, India. These flights covered the period of the Asian summer monsoon (June–September), during which enhancements in a number of atmospheric species were observed in the upper troposphere over southwestern Asia. In addition to in situ measurements of trace gases and aerosols, whole air samples were collected during the flights, and these were subsequently analyzed for a suite of trace gases that included a number of C2–C8 non-methane hydrocarbons. Non-methane hydrocarbons are relatively short-lived compounds and the large enhancements in their mixing ratios in the upper troposphere over southwestern Asia during the monsoon, sometimes more than double their spring and fall means, provides qualitative evidence for the influence of convectively uplifted boundary layer air. The particularly large enhancements of the combustion tracers benzene and ethyne, along with the similarity of their ratios with carbon monoxide and emission ratios from the burning of household biofuels, indicate a strong influence of biofuel burning to NMHC emissions in this region. Conversely, the ratios of ethane and propane to carbon monoxide, along with the ratio between i-butane and n-butane, indicate a significant source of these compounds from the use of fossil fuels, and comparison to previous campaigns suggests that this source could be increasing. Photochemical aging patterns of NMHCs showed that the CARIBIC samples were collected in two distinctly different regions of the monsoon circulation: a southern region where air masses had been recently influenced by low level contact and a northern region, where air parcels had spent substantial time in transit in the upper troposphere before being probed. Estimates of age using ratios of individual NMHCs have ranges of 3–6 days in the south and 9–12 days in the north.

scholarly journals Level 2 processing for the imaging Fourier transform spectrometer GLORIA: derivation and validation of temperature and trace gas volume mixing ratios from calibrated dynamics mode spectra

2015 ◽  
Vol 8 (6) ◽  
pp. 2473-2489 ◽  
Author(s):  
J. Ungermann ◽  
J. Blank ◽  
M. Dick ◽  
A. Ebersoldt ◽  
F. Friedl-Vallon ◽  
...  
Keyword(s):  
Fourier Transform ◽  
Horizontal Resolution ◽  
Trace Gas ◽  
Radiative Transfer Model ◽  
Transfer Model ◽  
Ionization Mass ◽  
Fourier Transform Spectrometer ◽  
Upper Troposphere ◽  
Mixing Ratios

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.

scholarly journals Mercury distribution in the upper troposphere and lower most stratosphere according to measurements by the IAGOS-CARIBIC observatory, 2014–2016

2018 ◽  
Author(s):  
Franz Slemr ◽  
Andreas Weigelt ◽  
Ralf Ebinghaus ◽  
Johannes Bieser ◽  
Carl A. M. Brenninkmeijer ◽  
...  
Keyword(s):  
Large Scale ◽  
Total Mercury ◽  
Trace Gases ◽  
Boreal Winter ◽  
Signal Integration ◽  
Upper Troposphere ◽  
Cloud Scavenging ◽  
Passenger Aircraft ◽  
North And South America ◽  
North And South

Abstract. Mercury was measured onboard the IAGOS-CARIBIC passenger aircraft since May 2005 until February 2016 during nearly monthly sequences of mostly four intercontinental flights from Germany to destinations in North and South America, Africa, and South and East Asia. Most of these mercury data were obtained using an internal default signal integration procedure of the Tekran instrument but since April 2014 more precise and accurate data were obtained using post-flight manual integration of the instrument raw signal. In this paper we use the latter data. Elevated upper tropospheric total mercury (TM) concentrations due to large scale biomass burning were observed in the upper troposphere (UT) at the equator and southern latitudes during the flights to Latin America and South Africa in boreal autumn (SON) and boreal winter (DJF). TM concentrations in the lowermost stratosphere (LMS) decrease with altitude above the thermal tropopause but the gradient is less steep than reported before. Seasonal variation of the vertical TM distribution in the UT and LMS is similar to that of other trace gases with surface sources and stratospheric sinks. Using speciation experiments, we show that nearly identical TM and gaseous elementary mercury (GEM) concentrations exist at and below the tropopause. Above the thermal tropopause GEM concentrations are almost always smaller than those of TM and the TM – GEM (i.e. Hg2+) difference increases up to ~ 40 % of TM at ~ 2 km and more above the thermal tropopause. Correlations with N2O as a reference tracer suggest stratospheric lifetimes of 72 ± 37 and 74 ± 27 yr for TM and GEM, respectively, comparable to the stratospheric lifetime of COS. This coincidence, combined with pieces of evidence from us and other researchers, corroborates the hypothesis that Hg2+ formed by oxidation in the stratosphere attaches to sulfate particles formed mainly by oxidation of COS and is removed with them from the stratosphere by air mass exchange, gravitational sedimentation, and cloud scavenging processes.

scholarly journals Multilevel Cloud Structures over Svalbard

2017 ◽  
Vol 145 (4) ◽  
pp. 1149-1159 ◽  
Author(s):  
Andreas Dörnbrack ◽  
Sonja Gisinger ◽  
Michael C. Pitts ◽  
Lamont R. Poole ◽  
Marion Maturilli
Keyword(s):  
Large Scale ◽  
Wave Structure ◽  
Horizontal Resolution ◽  
Temperature Fields ◽  
The Arctic ◽  
Mountain Waves ◽  
Air Masses ◽  
Flow Features ◽  
Stratospheric Clouds ◽  
Lidar Observations

Abstract The presented picture of the month is a superposition of spaceborne lidar observations and high-resolution temperature fields of the ECMWF Integrated Forecast System (IFS). It displays complex tropospheric and stratospheric clouds in the Arctic winter of 2015/16. Near the end of December 2015, the unusual northeastward propagation of warm and humid subtropical air masses as far north as 80°N lifted the tropopause by more than 3 km in 24 h and cooled the stratosphere on a large scale. A widespread formation of thick cirrus clouds near the tropopause and of synoptic-scale polar stratospheric clouds (PSCs) occurred as the temperature dropped below the thresholds for the existence of cloud particles. Additionally, mountain waves were excited by the strong flow at the western edge of the ridge across Svalbard, leading to the formation of mesoscale ice PSCs. The most recent IFS cycle using a horizontal resolution of 8 km globally reproduces the large-scale and mesoscale flow features and leads to a remarkable agreement with the wave structure revealed by the spaceborne observations.

scholarly journals Evolution of the Distribution of Upper-Tropospheric Humidity over the Indian Ocean: Connection with Large-Scale Advection and Local Cloudiness

2017 ◽  
Vol 56 (7) ◽  
pp. 2035-2052 ◽  
Author(s):  
Thomas Garot ◽  
Hélène Brogniez ◽  
Renaud Fallourd ◽  
Nicolas Viltard
Keyword(s):  
Indian Ocean ◽  
Large Scale ◽  
Transport Model ◽  
Intraseasonal Variability ◽  
Back Trajectory ◽  
Time Step ◽  
Air Masses ◽  
Upper Troposphere ◽  
Upper Tropospheric Humidity ◽  
The Indian Ocean

AbstractThe spatial and temporal distribution of upper-tropospheric humidity (UTH) observed by the Sounder for Atmospheric Profiling of Humidity in the Intertropics by Radiometry (SAPHIR)/Megha-Tropiques radiometer is analyzed over two subregions of the Indian Ocean during October–December over 2011–14. The properties of the distribution of UTH were studied with regard to the phase of the Madden–Julian oscillation (active or suppressed) and large-scale advection versus local production of moisture. To address these topics, first, a Lagrangian back-trajectory transport model was used to assess the role of the large-scale transport of air masses in the intraseasonal variability of UTH. Second, the temporal evolution of the distribution of UTH is analyzed using the computation of the higher moments of its probability distribution function (PDF) defined for each time step over the domain. The results highlight significant differences in the PDF of UTH depending on the phase of the MJO. The modeled trajectories ending in the considered domain originate from an area that strongly varies depending on the phases of the MJO: during the active phases, the air masses are spatially constrained within the tropical Indian Ocean domain, whereas a distinct upper-tropospheric (200–150 hPa) westerly flow guides the intraseasonal variability of UTH during the suppressed phases. Statistical relationships between the cloud fractions and the UTH PDF moments of are found to be very similar regardless of the convective activity. However, the occurrence of thin cirrus clouds is associated with a drying of the upper troposphere (enhanced during suppressed phases), whereas the occurrence of thick cirrus anvil clouds appears to be significantly related to a moistening of the upper troposphere.

scholarly journals Trapping, chemistry and export of trace gases in the South Asian summer monsoon observed during CARIBIC flights in 2008

2015 ◽  
Vol 15 (5) ◽  
pp. 6967-7018 ◽  
Author(s):  
A. Rauthe-Schöch ◽  
A. K. Baker ◽  
T. J. Schuck ◽  
C. A. M. Brenninkmeijer ◽  
A. Zahn ◽  
...  
Keyword(s):  
South Asian ◽  
Summer Monsoon ◽  
Asian Summer Monsoon ◽  
Trace Gases ◽  
Particle Dispersion ◽  
Atmospheric Pollutants ◽  
South Asian Summer Monsoon ◽  
The South ◽  
Air Masses ◽  
Asian Summer

Abstract. The CARIBIC (Civil Aircraft for the Regular Investigation of the Atmosphere Based on an Instrument Container) passenger aircraft observatory performed in situ measurements at 10–12 km altitude in the South Asian summer monsoon anticyclone between June and September 2008. These measurements enable us to investigate this atmospheric region, which so far has mostly been observed from satellites, using the broad suite of trace gases and aerosols measured by CARIBIC. Elevated levels of a range of atmospheric pollutants were recorded e.g. carbon monoxide, total reactive nitrogen oxides, aerosol particles and several volatile organic compounds. The measurements provide detailed information about the chemical composition of air in different parts of the monsoon anticyclone, particularly of ozone precursors. While covering a range of 3500 km inside the monsoon anticyclone, CARIBIC observations show remarkable consistency, i.e. with regular latitudinal patterns of trace gases during the entire monsoon period. Trajectory calculations indicate that these air masses originated mainly from South Asia and Mainland Southeast Asia. Using the CARIBIC trace gas and aerosol measurements in combination with the Lagrangian particle dispersion model FLEXPART we investigated the characteristics of monsoon outflow and the chemical evolution of air masses during transport. Estimated photochemical ages of the air were found to agree well with transport times from a source region east of 95° E. The photochemical ages of the air in the southern part of the monsoon anticyclone were consistently younger (less than 7 days) and the air masses mostly in an ozone forming chemical regime. In its northern part the air masses were older (up to 13 days) and had unclear ozone formation or destruction potential. Based on analysis of forward trajectories several receptor regions were identified. In addition to predominantly westward transport, we found evidence for efficient transport (within 10 days) to the Pacific and North America, particularly during June and September, and also of cross-tropopause exchange, which was strongest during June and July. Westward transport to Africa and further to the Mediterranean was the main pathway during July.

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