scholarly journals Assessment of the theoretical limit in instrumental detectability of northern high-latitude methane sources using <i>δ</i><sup>13</sup>C<sub>CH4</sub> atmospheric signals

2019 ◽  
Vol 19 (19) ◽  
pp. 12141-12161 ◽  
Author(s):  
Thibaud Thonat ◽  
Marielle Saunois ◽  
Isabelle Pison ◽  
Antoine Berchet ◽  
Thomas Hocking ◽  
...  
Keyword(s):  
High Latitude ◽  
Oil And Gas ◽  
Transport Model ◽  
Isotopic Signatures ◽  
Sources And Sinks ◽  
Regional Sources ◽  
Northern High Latitude ◽  
Source Signal ◽  
Methane Source ◽  
Remote Sites

Abstract. Recent efforts have brought together bottom-up quantification approaches (inventories and process-based models) and top-down approaches using regional observations of methane atmospheric concentrations through inverse modelling to better estimate the northern high-latitude methane sources. Nevertheless, for both approaches, the relatively small number of available observations in northern high-latitude regions leaves gaps in our understanding of the drivers and distributions of the different types of regional methane sources. Observations of methane isotope ratios, performed with instruments that are becoming increasingly affordable and accurate, could bring new insights on the contributions of methane sources and sinks. Here, we present the source signal that could be observed from methane isotopic 13CH4 measurements if high-resolution observations were available and thus what requirements should be fulfilled in future instrument deployments in terms of accuracy in order to constrain different emission categories. This theoretical study uses the regional chemistry-transport model CHIMERE driven by different scenarios of isotopic signatures for each regional methane source mix. It is found that if the current network of methane monitoring sites were equipped with instruments measuring the isotopic signal continuously, only sites that are significantly influenced by emission sources could differentiate regional emissions with a reasonable level of confidence. For example, wetland emissions require daily accuracies lower than 0.2 ‰ for most of the sites. Detecting East Siberian Arctic Shelf (ESAS) emissions requires accuracies lower than 0.05 ‰ at coastal Russian sites (even lower for other sites). Freshwater emissions would be detectable with an uncertainty lower than 0.1 ‰ for most continental sites. Except Yakutsk, Siberian sites require stringent uncertainty (lower than 0.05 ‰) to detect anthropogenic emissions from oil and gas or coal production. Remote sites such as Zeppelin, Summit, or Alert require a daily uncertainty below 0.05 ‰ to detect any regional sources. These limits vary with the hypothesis on isotopic signatures assigned to the different sources.

scholarly journals Assessment of the theoretical limit in instrumental detectability of Arctic methane sources using <sup>13</sup>C atmospheric signal

2018 ◽  
Author(s):  
Thibaud Thonat ◽  
Marielle Saunois ◽  
Isabelle Pison ◽  
Antoine Berchet ◽  
Thomas Hocking ◽  
...  
Keyword(s):  
Transport Model ◽  
The Arctic ◽  
Atmospheric Methane ◽  
Chemistry Transport Model ◽  
Isotopic Signatures ◽  
Arctic Regions ◽  
Methane Budget ◽  
Source Signal ◽  
Methane Source ◽  
Global Emissions

Abstract. Despite their modest 4 % magnitude compared to global emissions, Arctic methane sources are key elements in closing the global atmospheric methane budget, due to high uncertainties in their quantification and to their strong climate sensitivity. Recent efforts brought together bottom-up quantification approaches (inventories, process-based models) and regional observations of methane concentrations through inverse modelling to better estimate the Arctic methane sources, but the relatively small number of available observations in Arctic regions leaves gaps in fully understanding the drivers and distributions of the different types of methane sources present in the Arctic. Observations of methane isotope ratios could bring new insights on methane processes with increasingly affordable and accurate instruments. Here, we present the source signal that could be observed from methane isotopic measurements if high-resolution observations were available, and thus what requirements should be fulfilled in future instrument deployments in terms of accuracy in order to constrain different emission categories. This theoretical study uses the regional chemistry-transport model CHIMERE driven by different scenarios of isotopic signatures for each regional methane source mix. It is found that if the current network of methane monitoring sites is equipped with instruments measuring the isotopic signal continuously, only sites that are significantly influenced by emission sources could differentiate regional emissions from the background with a reasonable level of confidence. Nevertheless, we show that the detection of individual Arctic sources requires daily accuracies of

scholarly journals Emission ratio and isotopic signatures of molecular hydrogen emissions from tropical biomass burning

2013 ◽  
Vol 13 (18) ◽  
pp. 9401-9413 ◽  
Author(s):  
F. A. Haumann ◽  
A. M. Batenburg ◽  
G. Pieterse ◽  
C. Gerbig ◽  
M. C. Krol ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Molecular Hydrogen ◽  
Tropical Rainforest ◽  
Transport Model ◽  
Air Masses ◽  
Isotopic Signatures ◽  
Emission Ratio ◽  
Mixing Ratios ◽  
Source Signal

Abstract. In this study, we identify a biomass-burning signal in molecular hydrogen (H2) over the Amazonian tropical rainforest. To quantify this signal, we measure the mixing ratios of H2 and several other species as well as the H2 isotopic composition in air samples that were collected in the BARCA (Balanço Atmosférico Regional de Carbono na Amazônia) aircraft campaign during the dry season. We derive a relative H2 emission ratio with respect to carbon monoxide (CO) of 0.31 ± 0.04 ppb ppb−1 and an isotopic source signature of −280 ± 41‰ in the air masses influenced by tropical biomass burning. In order to retrieve a clear source signal that is not influenced by the soil uptake of H2, we exclude samples from the atmospheric boundary layer. This procedure is supported by data from a global chemistry transport model. The ΔH2 / ΔCO emission ratio is significantly lower than some earlier estimates for the tropical rainforest. In addition, our results confirm the lower values of the previously conflicting estimates of the H2 isotopic source signature from biomass burning. These values for the emission ratio and isotopic source signatures of H2 from tropical biomass burning can be used in future bottom-up and top-down approaches aiming to constrain the strength of the biomass-burning source for H2. Hitherto, these two quantities relied only on combustion experiments or on statistical relations, since no direct signal had been obtained from in-situ observations.

scholarly journals Variational inverse modelling within the Community Inversion Framework to assimilate δ<sup>13</sup>C(CH<sub>4</sub>) and CH<sub>4</sub>: a case study with model LMDz-SACS

2021 ◽  
Author(s):  
Joël Thanwerdas ◽  
Marielle Saunois ◽  
Antoine Berchet ◽  
Isabelle Pison ◽  
Bruce H. Vaughn ◽  
...  
Keyword(s):  
Inverse Modeling ◽  
Fossil Fuels ◽  
Transport Model ◽  
Initial Conditions ◽  
Top Down ◽  
Modeling Framework ◽  
Isotopic Signatures ◽  
Sources And Sinks ◽  
Mixing Ratios ◽  
Specific Source

Abstract. Atmospheric CH4 mixing ratios resumed their increase in 2007 after a plateau during the period 1999–2006, suggesting varying sources and sinks as main drivers. Estimating sources by exploiting observations within an inverse modeling framework (top-down approaches) is a powerful approach. It is nevertheless challenging to efficiently differentiate co-located emission categories and sinks by using CH4 observations alone. As a result, top-down approaches are limited when it comes to fully understanding CH4 burden changes and attribute these changes to specific source variations. CH4 source isotopic signatures differ between emission categories (biogenic, thermogenic and pyrogenic), and can therefore be used to address this limitation. Here, a new 3-D variational inverse modeling framework designed to assimilate δ13C(CH4) observations together with CH4 observations is presented. This system is capable of optimizing both emissions and associated source signatures of multiple emission categories. We present the technical implementation of joint CH4 and δ13C(CH4) constraints in a variational system, and analyze how sensitive the system is to the setup controlling the optimization using the 3-D Chemistry-Transport Model LMDz-SACS. We find that assimilating δ13C(CH4) observations and allowing the system to adjust source isotopic signatures provide relatively large differences in global flux estimates for wetlands (5 Tg yr−1), microbial (6 Tg yr−1), fossil fuels (8 Tg yr−1) and biofuels-biomass burning (4 Tg yr−1) categories compared to the results inferred without assimilating δ13C(CH4) observations. More importantly, when assimilating both CH4 and δ13C(CH4) observations, but assuming source signatures are perfectly known increase these differences between the system with CH4 and the enhanced one with δ13C(CH4) by a factor 3 or 4, strengthening the importance of having as accurate as possible signatures. Initial conditions, uncertainties on δ13C(CH4) observations or the number of optimized categories have a much smaller impact (less than 2 Tg yr−1).

scholarly journals Emission ratio and isotopic signatures of molecular hydrogen emissions from tropical biomass burning

2013 ◽  
Vol 13 (4) ◽  
pp. 11213-11245
Author(s):  
F. A. Haumann ◽  
A. M. Batenburg ◽  
G. Pieterse ◽  
C. Gerbig ◽  
M. C. Krol ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Molecular Hydrogen ◽  
Tropical Rainforest ◽  
Transport Model ◽  
Air Masses ◽  
Isotopic Signatures ◽  
Emission Ratio ◽  
Mixing Ratios ◽  
Source Signal

Abstract. In this study, we identify a biomass-burning signal in molecular hydrogen (H2) over the Amazonian tropical rainforest. To quantify this signal, we measure the mixing ratios of H2 and several other species as well as the H2 isotopic composition in air samples that were collected in the BARCA (Balanço Atmosférico Regional de Carbono na Amazônia) aircraft campaign during the dry season. We derive a relative H2 emission ratio with respect to carbon monoxide (CO) of 0.31 ± 0.04 ppb/ppb and an isotopic source signature of −280 &amp;pm; 41‰ in the air masses influenced by tropical biomass burning. In order to retrieve a clear source signal that is not influenced by the soil uptake of H2, we exclude samples from the atmospheric boundary layer. This procedure is supported by data from a global chemistry transport model. The ΔH2/ΔCO emission ratio is significantly lower than some earlier estimates for the tropical rainforest. In addition, our results confirm the lower values of the previously conflicting estimates of the H2 isotopic source signature from biomass burning. These values for the emission ratio and isotopic source signatures of H2 from tropical biomass burning can be used in future bottom-up and top-down approaches aiming to constrain the strength of the biomass-burning source for H2. Hitherto, these two quantities relied only on combustion experiments or on statistical relations, since no direct signal had been obtained from in-situ observations.

scholarly journals Source attributions of pollution to the Western Arctic during the NASA ARCTAS field campaign

2013 ◽  
Vol 13 (9) ◽  
pp. 4707-4721 ◽  
Author(s):  
H. Bian ◽  
P. R. Colarco ◽  
M. Chin ◽  
G. Chen ◽  
J. M. Rodriguez ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Field Experiments ◽  
Transport Model ◽  
Background Level ◽  
Anthropogenic Emissions ◽  
Airborne Measurements ◽  
Ch4 Production ◽  
Regional Sources ◽  
Western Arctic ◽  
Co Concentrations

Abstract. We use the NASA GEOS-5 transport model with tagged tracers to investigate the contributions of different regional sources of CO and black carbon (BC) to their concentrations in the Western Arctic (i.e., 50–90° N and 190–320° E) in spring and summer 2008. The model is evaluated by comparing the results with airborne measurements of CO and BC from the NASA Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) field campaigns to demonstrate the strengths and limitations of our simulations. We also examine the reliability of tagged CO tracers in characterizing air mass origins using the measured fossil fuel tracer of dichloromethane and the biomass burning tracer of acetonitrile. Our tagged CO simulations suggest that most of the enhanced CO concentrations (above background level from CH4 production) observed during April originate from Asian anthropogenic emissions. Boreal biomass burning emissions and Asian anthropogenic emissions are of similar importance in July domain wise, although the biomass burning CO fraction is much larger in the area of the ARCTAS field experiments. The fraction of CO from Asian anthropogenic emissions is larger in spring than in summer. European sources make up no more than 10% of CO levels in the campaign domain during either period. Comparisons of CO concentrations along the flight tracks with regional averages from GEOS-5 show that the along-track measurements are representative of the concentrations within the large domain of the Western Arctic in April but not in July.

Climatic thresholds shape northern high-latitude fire regimes and imply vulnerability to future climate change

Ecography ◽  
2016 ◽  
Vol 40 (5) ◽  
pp. 606-617 ◽  
Author(s):  
Adam M. Young ◽  
Philip E. Higuera ◽  
Paul A. Duffy ◽  
Feng Sheng Hu
Keyword(s):  
Climate Change ◽  
High Latitude ◽  
Fire Regimes ◽  
Future Climate ◽  
Future Climate Change ◽  
Northern High Latitude

scholarly journals Average versus high surface ozone levels over the continental U.S.A.: Model bias, background influences, and interannual variability

2018 ◽  
Author(s):  
Jean J. Guo ◽  
Arlene M. Fiore ◽  
Lee T. Murray ◽  
Daniel A. Jaffe ◽  
Jordan L. Schnell ◽  
...  
Keyword(s):  
Interannual Variability ◽  
Transport Model ◽  
Surface Ozone ◽  
High Surface ◽  
Anthropogenic Sources ◽  
Pollution Transport ◽  
Natural Sources ◽  
Model Biases ◽  
Regional Sources ◽  
Surface O3

Abstract. U.S. background ozone (O3) includes O3 produced from anthropogenic O3 precursors emitted outside of the U.S.A., from global methane, and from any natural sources. Using a suite of sensitivity simulations in the GEOS-Chem global chemistry-transport model, we estimate the influence from individual background versus U.S. anthropogenic sources on total surface O3 over ten continental U.S. regions from 2004–2012. Evaluation with observations reveals model biases of +0–19 ppb in seasonal mean maximum daily 8-hour average (MDA8) O3, highest in summer over the eastern U.S.A. Simulated high-O3 events cluster too late in the season. We link these model biases to regional O3 production (e.g., U.S. anthropogenic, biogenic volatile organic compounds (BVOC), and soil NOx, emissions), or coincident missing sinks. On the ten highest observed O3 days during summer (O3_top10obs_JJA), U.S. anthropogenic emissions enhance O3 by 5–11 ppb and by less than 2 ppb in the eastern versus western U.S.A. The O3 enhancement from BVOC emissions during summer is 1–7 ppb higher on O3_top10obs_JJA days than on average days, while intercontinental pollution is up to 2 ppb higher on average vs. on O3_top10obs_JJA days. In the model, regional sources of O3 precursor emissions drive interannual variability in the highest observed O3 levels. During the summers of 2004–2012, monthly regional mean U.S. background O3 MDA8 levels vary by 10–20 ppb. Simulated summertime total surface O3 levels on O3_top10obs_JJA days decline by 3 ppb (averaged over all regions) from 2004–2006 to 2010–2012 in both the observations and the model, reflecting rising U.S. background (+2 ppb) and declining U.S. anthropogenic O3 emissions (−6 ppb). The model attributes interannual variability in U.S. background O3 on O3_top10obs days to natural sources, not international pollution transport. We find that a three-year averaging period is not long enough to eliminate interannual variability in background O3.

scholarly journals A three-dimensional model study of long-term mid-high latitude lower stratosphere ozone changes

2003 ◽  
Vol 3 (1) ◽  
pp. 1081-1107 ◽  
Author(s):  
M. P. Chipperfield
Keyword(s):  
High Latitude ◽  
Lower Stratosphere ◽  
Transport Model ◽  
Three Dimensional ◽  
Horizontal Resolution ◽  
Chemical Transport Model ◽  
Three Dimensional Model ◽  
Detailed Chemistry ◽  
Basic Model ◽  
Column Ozone

Abstract. We have used a 3D off-line chemical transport model (CTM) to study the causes of the observed changes in ozone in the mid-high latitude lower stratosphere from 1979–1998. The model was forced by European Centre for Medium Range Weather Forecasts (ECMWF) analyses and contains a detailed chemistry scheme. A series of model runs were performed at a horizontal resolution of 7.5°×7.5° and covered the domain from about 12 km to 30 km. The basic model performs well in reproducing the decadal evolution of the springtime depletion in the northern hemisphere (NH) and southern hemisphere (SH) high latitudes in the 1980s and early 1990s. After about 1994 the modelled interannual variability does not match the observations as well, which is probably due in part to changes in the operational ECMWF analyses – which places limits on using this dataset to diagnose dynamical trends. For mid-latitudes (35°–60°) the basic model reproduces the observed column ozone decreases from 1980 until the early 1990s. Model experiments show that the halogen trends appear to dominate this modelled decrease and of this around 30–50% is due to high-latitude processing on polar stratospheric clouds (PSCs). Dynamically induced ozone variations in the model correlate with observations over the timescale of a few years. Large discrepancies between the modelled and observed variations in the mid 1980s and mid 1990s can be largely resolved by assuming that the 11-year solar cycle (not explicitly included in the 3D model) causes a 2% (min-max) change in mid-latitude column ozone.

scholarly journals δ 13 C methane source signatures from tropical wetland and rice field emissions

2021 ◽  
Vol 380 (2215) ◽  
Author(s):  
James L. France ◽  
Rebecca E. Fisher ◽  
David Lowry ◽  
Grant Allen ◽  
Marcos F. Andrade ◽  
...  
Keyword(s):  
Rice Field ◽  
Ambient Air ◽  
Atmospheric Methane ◽  
Isotopic Signatures ◽  
Methane Budget ◽  
Significant Seasonal Variation ◽  
Methane Source ◽  
Wetland Extent ◽  
Term Monitoring

The atmospheric methane (CH 4 ) burden is rising sharply, but the causes are still not well understood. One factor of uncertainty is the importance of tropical CH 4 emissions into the global mix. Isotopic signatures of major sources remain poorly constrained, despite their usefulness in constraining the global methane budget. Here, a collection of new δ 13 C CH 4 signatures is presented for a range of tropical wetlands and rice fields determined from air samples collected during campaigns from 2016 to 2020. Long-term monitoring of δ 13 C CH 4 in ambient air has been conducted at the Chacaltaya observatory, Bolivia and Southern Botswana. Both long-term records are dominated by biogenic CH 4 sources, with isotopic signatures expected from wetland sources. From the longer-term Bolivian record, a seasonal isotopic shift is observed corresponding to wetland extent suggesting that there is input of relatively isotopically light CH 4 to the atmosphere during periods of reduced wetland extent. This new data expands the geographical extent and range of measurements of tropical wetland and rice δ 13 C CH 4 sources and hints at significant seasonal variation in tropical wetland δ 13 C CH 4 signatures which may be important to capture in future global and regional models. This article is part of a discussion meeting issue ‘Rising methane: is warming feeding warming? (part 2)’.

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