scholarly journals Exploring the inorganic composition of the Asian Tropopause Aerosol Layer using medium-duration balloon flights

2021 ◽  
Author(s):  
Hazel Vernier ◽  
Neeraj Rastogi ◽  
Hongyu Liu ◽  
Amit Kumar Pandit ◽  
Kris Bedka ◽  
...  
Keyword(s):  
Particle Size ◽  
Large Scale ◽  
Transport Model ◽  
Large Fraction ◽  
Western China ◽  
Aerosol Layer ◽  
Fire Event ◽  
Air Mass ◽  
Air Masses ◽  
Model Simulations

Abstract. Satellite observations have revealed an enhanced aerosol layer near the tropopause over Asia during the summer monsoon, called the Asian Tropopause Aerosol Layer (ATAL). In this work, aerosol particles in the ATAL were collected with a balloon-borne impactor near the tropopause region over India, using extended duration balloon flights, in summer 2017 and winter 2018. Their chemical composition was further investigated by quantitative analysis using offline ion chromatography. Nitrate (NO3−) and nitrite (NO2−) were found to be the dominant ions in the collected aerosols with values ranging between 87–343 ng/m3 STP during the summer campaign. In contrast, sulfate (SO42−) levels were found above the detection limit (> 10 ng/m3 STP) only in winter. In addition, we determined the origin of the air masses sampled during the flights through analysis of back trajectories along with convective influence. The results obtained therein were put into a context of large-scale transport and aerosol distribution with GEOS-Chem chemical transport model simulations. The first flight of summer 2017 which sampled air mass within the Asian monsoon anticyclone (AMA), influenced by convection over Western China, was associated with particle size radius (0.05–2 μm). In contrast, the second flight sampled air mass at the edge of the AMA associated with larger particle size radius (> 2 μm) with higher nitrite concentration. The sampled air masses in winter 2018 were likely affected by smoke from the Pacific Northwest fire event in Canada, which occurred 7 months prior to our campaign, leading to concentration enhancements of SO42− and Ca2+. Overall, our results suggest that nitrogen-containing particles represent a large fraction of aerosols populating the ATAL, in agreement with the results from aircraft measurements during the StratoClim campaign. Furthermore, GEOS-Chem model simulations suggest that lightning NOx emissions had a significant impact on the production of nitrate aerosols sampled during the summer 2017.

Exploring the ionic composition of the Asian Tropopause Aerosol Layer using medium duration balloon flights

2021 ◽  
Author(s):  
Hazel Vernier ◽  
Neeraj Rastogi ◽  
Hongyu Liu ◽  
Duncan Fairlie ◽  
Amit Pandit ◽  
...  
Keyword(s):  
Particle Size ◽  
Large Scale ◽  
Transport Model ◽  
Large Fraction ◽  
Ionic Composition ◽  
Back Trajectory ◽  
Aerosol Layer ◽  
Air Mass ◽  
Air Masses ◽  
Model Simulations

<p>Satellite observations have revealed an enhanced aerosol layer near the tropopause over Asia during the summer monsoon, called the Asian Tropopause Aerosol Layer (ATAL). The chemical composition of the ATAL is investigated here using offline ionic analysis of aerosols collected with a balloon-borne impactor near the tropopause region over India onboard extended duration balloon flights in the summer of 2017 and winter 2018. We found NO<sub>3</sub><sup>- </sup>and NO<sub>2</sub><sup>-</sup> dominant among other ions with values ranging between 87-343 ng/m<sup>3</sup> during the summer campaign. In contrast, SO<sub>4</sub> levels were found above detection limit (>10 ng/m<sup>3</sup>) only in winter. In addition, we determined the origin of the air masses sampled during the flights through back trajectory analysis combined with convection. The results obtained therein were put into a context of large-scale transport and aerosol distribution with GEOS-Chem chemical transport model simulations. The first flight of summer 2017 sampled air mass within the Asian monsoon anticyclone (AMA), associated with smaller particle size found on stage 2 (particle size cut off > 0.15 microns) of the impactor, while the second flight sampled air mass at the edge of the AMA associated with larger particle size on stage 1 (particle size cut off between 2 and 0.5 microns). The sampled air masses in winter 2018 were affected by smoke from the Pacific Northwest fire event in Canada, which occurred 7 months prior to our campaign. Concentrations of SO<sub>4</sub><sup>2-</sup>, NH4<sup>+</sup>, and Ca<sup>2+</sup> were enhanced. Overall, our results suggest that nitrogen- containing particles represent a large fraction of aerosols populating the ATAL in agreement with aircraft measurements during the StratoClim campaign. Furthermore, GEOS-chem model simulations suggest that lightning NOx emissions had a minimal impact on the production of nitrate aerosols sampled during the two flights. </p>

scholarly journals Analysis of a rapid increase of stratospheric ozone during late austral summer 2008 over Kerguelen (49.4° S, 70.3° E)

2011 ◽  
Vol 11 (1) ◽  
pp. 363-373 ◽  
Author(s):  
H. Bencherif ◽  
L. El Amraoui ◽  
G. Kirgis ◽  
J. Leclair De Bellevue ◽  
A. Hauchecorne ◽  
...  
Keyword(s):  
Potential Vorticity ◽  
Large Scale ◽  
Lower Stratosphere ◽  
Transport Model ◽  
Stratospheric Ozone ◽  
Three Dimensional ◽  
Austral Summer ◽  
Air Masses ◽  
Global Mapping ◽  
The Tropics

Abstract. This paper reports on an increase of ozone event observed over Kerguelen (49.4° S, 70.3° E) in relationship with large-scale isentropic transport. This is evidenced by ground-based observations (co-localised radiosonde and SAOZ experiments) together with satellite global observations (Aura/MLS) assimilated into MOCAGE, a Méteo-France model. The study is based on the analyses of the first ozonesonde experiment never recorded at the Kerguelen site within the framework of a French campaign called ROCK that took place from April to August 2008. Comparisons and interpretations of the observed event are supported by co-localised SAOZ observations, by global mapping of tracers (O3, N2O and columns of O3) from Aura/MLS and Aura/OMI experiments, and by model simulations of Ertel Potential Vorticity initialised by the ECMWF (European Centre for Medium-Range Weather Forecasts) data reanalyses. Satellite and ground-based observational data revealed a consistent increase of ozone in the local stratosphere by mid-April 2008. Additionally, Ozone (O3) and nitrous oxide (N2O) profiles obtained during January–May 2008 using the Microwave Limb Sounder (MLS) aboard the Aura satellite are assimilated into MOCAGE (MOdèle de Chimie Atmosphérique à Grande Echelle), a global three-dimensional chemistry transport model of Météo-France. The assimilated total O3 values are consistent with SAOZ ground observations (within ±5%), and isentropic distributions of O3 match well with maps of advected potential vorticity (APV) derived from the MIMOSA model, a high-resolution advection transport model, and from the ECMWF reanalysis. The event studied seems to be related to the isentropic transport of air masses that took place simultaneously in the lower- and middle-stratosphere, respectively from the polar region and from the tropics to the mid-latitudes. In fact, the ozone increase observed by mid April 2008 resulted simultaneously: (1) from an equator-ward departure of polar air masses characterised with a high-ozone layer in the lower stratosphere (near the 475 K isentropic level), and (2) from a reverse isentropic transport from the tropics to mid- and high-latitudes in the upper stratosphere (nearby the 700 K level). The increase of ozone observed over Kerguelen from the 16-April ozonesonde profile is thus attributed to a concomitant isentropic transport of ozone in two stratospheric layers: the tropical air moving southward and reaching over Kerguelen in the upper stratosphere, and the polar air passing over the same area but in the lower stratosphere.

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 Strong variability of the Asian Tropopause Aerosol Layer (ATAL) in August 2016 at the Himalayan foothills

2020 ◽  
Author(s):  
Sreeharsha Hanumanthu ◽  
Bärbel Vogel ◽  
Rolf Müller ◽  
Simone Brunamonti ◽  
Suvarna Fadnavis ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Large Scale ◽  
Asian Summer Monsoon ◽  
Aerosol Layer ◽  
South Asian Summer Monsoon ◽  
Air Masses ◽  
Source Regions ◽  
Himalayan Foothills ◽  
Asian Summer ◽  
Aerosol Backscatter

Abstract. The South Asian summer monsoon is associated with a large-scale anticyclonic circulation in the Upper Troposphere and Lower Stratosphere (UTLS), which confines the air mass inside. During boreal summer, the confinement of this air mass leads to an accumulation of aerosol between about 13 km and 18 km (360 K and 440 K potential temperature), this accumulation of aerosol constitutes the Asian Tropopause Aerosol Layer (ATAL). We present balloon-borne aerosol backscatter measurements of the ATAL performed by the Compact Optical Backscatter Aerosol Detector (COBALD) instrument in Nainital in Northern India in August 2016, and compare these with COBALD measurements in the post-monsoon time in November 2016. The measurements demonstrate a strong variability of the ATAL's altitude, vertical extent, aerosol backscatter intensity and cirrus cloud occurrence frequency. Such a variability cannot be deduced from climatological means of the ATAL as they are derived from satellite measurements. To explain this observed variability we performed a Lagrangian back-trajectory analysis using the Chemical Lagrangian Model of the Stratosphere (CLaMS). We identify the transport pathways of air parcels contributing to the ATAL over Nainital in August 2016, as well as the source regions of the air masses contributing to the composition of the ATAL. Our analysis reveals a variety of factors contributing to the observed day-to-day variability of the ATAL: continental convection, tropical cyclones (maritime convection), dynamics of the anticyclone and stratospheric intrusions. Thus, the ATAL is a mixture of air masses coming from different atmospheric height layers. In addition, contributions from the model boundary layer originate in different geographic source regions. The location of strongest updraft along the backward trajectories reveal a cluster of strong upward transport at the southern edge of the Himalayan foothills. From the top of the convective outflow level (about 13 km; 360 K) the air parcels ascend slowly to ATAL altitudes within a large-scale upward spiral driven by the diabatic heating in the anticyclonic flow of the South Asian summer monsoon at UTLS altitudes. Cases with a strong ATAL typically show boundary layer contributions from the Tibetan Plateau, the foothills of the Himalayas and other continental regions below the Asian monsoon. Weaker ATAL cases show higher contributions from the maritime boundary layer, often related to tropical cyclones, indicating a mixing of unpolluted and polluted air masses. Because of the strong growth of Asian economies, increasing anthropogenic emissions in the future are expected to enhance the thickness and intensity of the ATAL, thereby also enhancing the global stratospheric aerosol loading, which likely impacts surface climate.

scholarly journals Using ship-borne observations of methane isotopic ratio in the Arctic Ocean to understand methane sources in the Arctic

2019 ◽  
Author(s):  
Antoine Berchet ◽  
Isabelle Pison ◽  
Patrick M. Crill ◽  
Brett Thornton ◽  
Philippe Bousquet ◽  
...  
Keyword(s):  
Arctic Ocean ◽  
Large Scale ◽  
Transport Model ◽  
Isotopic Ratio ◽  
The Arctic ◽  
Isotopic Ratios ◽  
Air Masses ◽  
Remote Areas ◽  
The Arctic Ocean

Abstract. Due to the large variety and heterogeneity of sources in remote areas hard to document, the Arctic regional methane budget remain very uncertain. In situ campaigns provide valuable data sets to reduce these uncertainties. Here we analyse data from the SWERUS-C3 campaign, on-board the icebreaker Oden, that took place during summer 2014 in the Arctic Ocean along the Northern Siberian and Alaskan shores. Total concentrations of methane, as well as isotopic ratios were measured continuously during this campaign for 35 days in July and August 2014. Using a chemistry-transport model, we link observed concentrations and isotopic ratios to regional emissions and hemispheric transport structures. A simple inversion system helped constraining source signatures from wetlands in Siberia and Alaska and oceanic sources, as well as the isotopic composition of lower stratosphere air masses. The variation in the signature of low stratosphere air masses, due to strongly fractionating chemical reactions in the stratosphere, was suggested to explain a large share of the observed variability in isotopic ratios. These points at required efforts to better simulate large scale transport and chemistry patterns to use isotopic data in remote areas. It is found that constant and homogeneous source signatures for each type of emission in the region (mostly wetlands and oil and gas industry) is not compatible with the strong synoptic isotopic signal observed in the Arctic. A regional gradient in source signatures is highlighted between Siberian and Alaskan wetlands, the later ones having a lighter signatures than the first ones. Arctic continental shelf sources are suggested to be a mixture of methane from a dominant thermogenic origin and a secondary biogenic one, consistent with previous in-situ isotopic analysis of seepage along the Siberian shores.

scholarly journals Leveraging the signature of heterotrophic respiration on atmospheric CO<sub>2</sub> for model benchmarking

2020 ◽  
Vol 17 (5) ◽  
pp. 1293-1308 ◽  
Author(s):  
Samantha J. Basile ◽  
Xin Lin ◽  
William R. Wieder ◽  
Melannie D. Hartman ◽  
Gretchen Keppel-Aleks
Keyword(s):  
Large Scale ◽  
Transport Model ◽  
Heterotrophic Respiration ◽  
Atmospheric Co2 ◽  
Scale Model ◽  
Future Research ◽  
Tracer Transport ◽  
Test Bed ◽  
Model Simulations ◽  
Soil Heterotrophic Respiration

Abstract. Spatial and temporal variations in atmospheric carbon dioxide (CO2) reflect large-scale net carbon exchange between the atmosphere and terrestrial ecosystems. Soil heterotrophic respiration (HR) is one of the component fluxes that drive this net exchange, but, given observational limitations, it is difficult to quantify this flux or to evaluate global-scale model simulations thereof. Here, we show that atmospheric CO2 can provide a useful constraint on large-scale patterns of soil heterotrophic respiration. We analyze three soil model configurations (CASA-CNP, MIMICS, and CORPSE) that simulate HR fluxes within a biogeochemical test bed that provides each model with identical net primary productivity (NPP) and climate forcings. We subsequently quantify the effects of variation in simulated terrestrial carbon fluxes (NPP and HR from the three soil test-bed models) on atmospheric CO2 distributions using a three-dimensional atmospheric tracer transport model. Our results show that atmospheric CO2 observations can be used to identify deficiencies in model simulations of the seasonal cycle and interannual variability in HR relative to NPP. In particular, the two models that explicitly simulated microbial processes (MIMICS and CORPSE) were more variable than observations at interannual timescales and showed a stronger-than-observed temperature sensitivity. Our results prompt future research directions to use atmospheric CO2, in combination with additional constraints on terrestrial productivity or soil carbon stocks, for evaluating HR fluxes.

scholarly journals Transport pathways of CO in the African upper troposphere during the monsoon season: a study based upon the assimilation of spaceborne observations

2008 ◽  
Vol 8 (12) ◽  
pp. 3231-3246 ◽  
Author(s):  
B. Barret ◽  
P. Ricaud ◽  
C. Mari ◽  
J.-L. Attié ◽  
N. Bousserez ◽  
...  
Keyword(s):  
Southeast Asia ◽  
Southern Africa ◽  
Large Scale ◽  
Transport Model ◽  
Hadley Cell ◽  
High Time Resolution ◽  
Transport Pathways ◽  
Air Masses ◽  
Upper Troposphere ◽  
African Monsoon

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.

scholarly journals Relationships between submicrometer particulate air pollution and air mass history in Beijing, China, 2004–2006

2008 ◽  
Vol 8 (20) ◽  
pp. 6155-6168 ◽  
Author(s):  
B. Wehner ◽  
W. Birmili ◽  
F. Ditas ◽  
Z. Wu ◽  
M. Hu ◽  
...  
Keyword(s):  
Air Pollution ◽  
Large Scale ◽  
Northwest China ◽  
Back Trajectory ◽  
Anthropogenic Aerosol ◽  
Air Mass ◽  
Air Masses ◽  
Rapid Economic Growth ◽  
Trajectory Classification ◽  
History Of

Abstract. The Chinese capital Beijing is one of the global megacities where the effects of rapid economic growth have led to complex air pollution problems that are not well understood. In this study, ambient particle number size distributions in Beijing between 2004 and 2006 are analysed as a function of regional meteorological transport. An essential result is that the particle size distribution in Beijing depends to large extent on the history of the synoptic scale air masses. A first approach based on manual back trajectory classification yielded differences in particulate matter mass concentration by a factor of two between four different air mass categories, including three main wind directions plus the case of stagnant air masses. A back trajectory cluster analysis refined these results, yielding a total of six trajectory clusters. Besides the large scale wind direction, the transportation speed of an air mass was found to play an essential role on the PM concentrations in Beijing. Slow-moving air masses were shown to be associated with an effective accumulation of surface-based anthropogenic emissions due to both, an increased residence time over densely populated land, and their higher degree of vertical stability. For the six back trajectory clusters, differences in PM1 mass concentrations by a factor of 3.5, in the mean air mass speed by a factor of 6, and in atmospheric visibility by a factor of 4 were found. The main conclusion is that the air quality in Beijing is not only degraded by anthropogenic aerosol sources from within the megacity, but also by sources across the entire Northwest China plain depending on the meteorological situation.

scholarly journals Transport pathways of CO in the African upper troposphere during the monsoon season: a study based upon the assimilation of spaceborne observations

2008 ◽  
Vol 8 (1) ◽  
pp. 2863-2902 ◽  
Author(s):  
B. Barret ◽  
P. Ricaud ◽  
C. Mari ◽  
J.-L. Attié ◽  
N. Bousserez ◽  
...  
Keyword(s):  
Southeast Asia ◽  
Southern Africa ◽  
Large Scale ◽  
Transport Model ◽  
Hadley Cell ◽  
High Time Resolution ◽  
Transport Pathways ◽  
Air Masses ◽  
Upper Troposphere ◽  
African Monsoon

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.

scholarly journals Using ship-borne observations of methane isotopic ratio in the Arctic Ocean to understand methane sources in the Arctic

2020 ◽  
Vol 20 (6) ◽  
pp. 3987-3998 ◽  
Author(s):  
Antoine Berchet ◽  
Isabelle Pison ◽  
Patrick M. Crill ◽  
Brett Thornton ◽  
Philippe Bousquet ◽  
...  
Keyword(s):  
Arctic Ocean ◽  
Large Scale ◽  
Oil And Gas ◽  
Lower Stratosphere ◽  
Transport Model ◽  
Isotopic Ratio ◽  
Oil And Gas Industry ◽  
The Arctic ◽  
Isotopic Ratios ◽  
Air Masses

Abstract. Characterizing methane sources in the Arctic remains challenging due to the remoteness, heterogeneity and variety of such emissions. In situ campaigns provide valuable datasets to reduce these uncertainties. Here we analyse data from the summer 2014 SWERUS-C3 campaign in the eastern Arctic Ocean, off the shore of Siberia and Alaska. Total concentrations of methane, as well as relative concentrations of 12CH4 and 13CH4, were measured continuously during this campaign for 35 d in July and August. Using a chemistry-transport model, we link observed concentrations and isotopic ratios to regional emissions and hemispheric transport structures. A simple inversion system helped constrain source signatures from wetlands in Siberia and Alaska, and oceanic sources, as well as the isotopic composition of lower-stratosphere air masses. The variation in the signature of lower-stratosphere air masses, due to strongly fractionating chemical reactions in the stratosphere, was suggested to explain a large share of the observed variability in isotopic ratios. These results point towards necessary efforts to better simulate large-scale transport and chemistry patterns to make relevant use of isotopic data in remote areas. It is also found that constant and homogeneous source signatures for each type of emission in a given region (mostly wetlands and oil and gas industry in our case at high latitudes) are not compatible with the strong synoptic isotopic signal observed in the Arctic. A regional gradient in source signatures is highlighted between Siberian and Alaskan wetlands, the latter having lighter signatures (more depleted in 13C). Finally, our results suggest that marine emissions of methane from Arctic continental-shelf sources are dominated by thermogenic-origin methane, with a secondary biogenic source as well.

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