scholarly journals A Bayesian framework for deriving sector-based methane emissions from top-down fluxes

2021 ◽  
Vol 2 (1) ◽  
Author(s):  
Daniel H. Cusworth ◽  
A. Anthony Bloom ◽  
Shuang Ma ◽  
Charles E. Miller ◽  
Kevin Bowman ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Transport Model ◽  
Estimation Method ◽  
Relative Weight ◽  
Optimal Estimation ◽  
Atmospheric Methane ◽  
Permian Basin ◽  
Top Down ◽  
Methane Fluxes ◽  
Reduce Emissions

AbstractAtmospheric methane observations are used to test methane emission inventories as the sum of emissions should correspond to observed methane concentrations. Typically, concentrations are inversely projected to a net flux through an atmospheric chemistry-transport model. Current methods to partition net fluxes to underlying sector-based emissions often scale fluxes based on the relative weight of sectors in a prior inventory. However, this approach imposes correlation between emission sectors which may not exist. Here we present a Bayesian optimal estimation method that projects inverse methane fluxes directly to emission sectors while accounting uncertainty structure and spatial resolution of prior fluxes and emissions. We apply this method to satellite-derived fluxes over the U.S. and at higher resolution over the Permian Basin to demonstrate that we can characterize a sector-based emission budget. This approach provides more robust comparisons between different top-down estimates, critical for assessing the efficacy of policies intended to reduce emissions.

scholarly journals Simultaneous atmospheric measurements using two Fourier transform infrared spectrometers at the Polar Environment Atmospheric Research Laboratory during spring 2006, and comparisons with the Atmospheric Chemistry Experiment-Fourier Transform Spectrometer

2008 ◽  
Vol 8 (2) ◽  
pp. 5305-5358 ◽  
Author(s):  
D. Fu ◽  
K. A. Walker ◽  
R. L. Mittermeier ◽  
K. Strong ◽  
K. Sung ◽  
...  
Keyword(s):  
Fourier Transform ◽  
Atmospheric Chemistry ◽  
Research Laboratory ◽  
Chemical Constituents ◽  
Estimation Method ◽  
Optimal Estimation ◽  
Atmospheric Measurements ◽  
Atmospheric Research ◽  
Polar Environment ◽  
Chemistry Experiment

Abstract. The 2006 Canadian Arctic ACE (Atmospheric Chemistry Experiment) Validation Campaign collected measurements at the Polar Environment Atmospheric Research Laboratory (PEARL, 80.05° N, 86.42° W, 610 m above sea level) at Eureka, Canada from 17 February to 31 March 2006. Two of the ten instruments involved in the campaign, both Fourier transform spectrometers (FTSs), were operated simultaneously, recording atmospheric solar absorption spectra. The first instrument was an ABB Bomem DA8 high-resolution infrared FTS. The second instrument was the Portable Atmospheric Research Interferometric Spectrometer for the Infrared (PARIS-IR), the ground-based version of the satellite-borne FTS on the ACE satellite (ACE-FTS). From the measurements collected by these two ground-based instruments, total column densities of seven stratospheric trace gases (O3, HNO3, NO2, HCl, HF, NO, and ClONO2 were retrieved using the optimal estimation method and these results were compared. Since the two instruments sampled the same portions of atmosphere by synchronizing observations during the campaign, the biases in retrieved columns from the two spectrometers represent the instrumental differences. These differences were consistent with those seen in previous FTS intercomparison studies. Partial column results from the ground-based spectrometers were also compared with partial columns derived from ACE-FTS version 2.2 (including updates for O3, HDO and N2O5 profiles and the differences found were consistent with the other validation comparison studies for the ACE-FTS version 2.2 data products. Column densities of O3, HCl, ClONO2, and HNO3 from the three FTSs were normalized with respect to HF and used to probe the time evolution of the chemical constituents in the atmosphere over Eureka during spring 2006.

scholarly journals Five years of CO, HCN, C<sub>2</sub>H<sub>6</sub>, C<sub>2</sub>H<sub>2</sub>, CH<sub>3</sub>OH, HCOOH and H<sub>2</sub>CO total columns measured in the Canadian high Arctic

2014 ◽  
Vol 7 (6) ◽  
pp. 1547-1570 ◽  
Author(s):  
C. Viatte ◽  
K. Strong ◽  
K. A. Walker ◽  
J. R. Drummond
Keyword(s):  
Time Series ◽  
Fourier Transform ◽  
Biomass Burning ◽  
Atmospheric Chemistry ◽  
A Priori ◽  
Estimation Method ◽  
Optimal Estimation ◽  
High Arctic ◽  
Retrieval Algorithm ◽  
Data Set

Abstract. We present a five-year time series of seven tropospheric species measured using a ground-based Fourier transform infrared (FTIR) spectrometer at the Polar Environment Atmospheric Research Laboratory (PEARL; Eureka, Nunavut, Canada; 80°05' N, 86°42' W) from 2007 to 2011. Total columns and temporal variabilities of carbon monoxide (CO), hydrogen cyanide (HCN) and ethane (C2H6) as well as the first derived total columns at Eureka of acetylene (C2H2), methanol (CH3OH), formic acid (HCOOH) and formaldehyde (H2CO) are investigated, providing a new data set in the sparsely sampled high latitudes. Total columns are obtained using the SFIT2 retrieval algorithm based on the optimal estimation method. The microwindows as well as the a priori profiles and variabilities are selected to optimize the information content of the retrievals, and error analyses are performed for all seven species. Our retrievals show good sensitivities in the troposphere. The seasonal amplitudes of the time series, ranging from 34 to 104%, are captured while using a single a priori profile for each species. The time series of the CO, C2H6 and C2H2 total columns at PEARL exhibit strong seasonal cycles with maxima in winter and minima in summer, in opposite phase to the HCN, CH3OH, HCOOH and H2CO time series. These cycles result from the relative contributions of the photochemistry, oxidation and transport as well as biogenic and biomass burning emissions. Comparisons of the FTIR partial columns with coincident satellite measurements by the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) show good agreement. The correlation coefficients and the slopes range from 0.56 to 0.97 and 0.50 to 3.35, respectively, for the seven target species. Our new data set is compared to previous measurements found in the literature to assess atmospheric budgets of these tropospheric species in the high Arctic. The CO and C2H6concentrations are consistent with negative trends observed over the Northern Hemisphere, attributed to fossil fuel emission decrease. The importance of poleward transport for the atmospheric budgets of HCN and C2H2 is highlighted. Columns and variabilities of CH3OH and HCOOH at PEARL are comparable to previous measurements performed at other remote sites. However, the small columns of H2CO in early May might reflect its large atmospheric variability and/or the effect of the updated spectroscopic parameters used in our retrievals. Overall, emissions from biomass burning contribute to the day-to-day variabilities of the seven tropospheric species observed at Eureka.

scholarly journals The added value of satellite observations of methane forunderstanding the contemporary methane budget

2021 ◽  
Vol 379 (2210) ◽  
pp. 20210106
Author(s):  
Paul I. Palmer ◽  
Liang Feng ◽  
Mark F. Lunt ◽  
Robert J. Parker ◽  
Hartmut Bösch ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Transport Model ◽  
A Priori ◽  
Added Value ◽  
Atmospheric Methane ◽  
Sources And Sinks ◽  
Methane Budget ◽  
Spatial Coverage ◽  
New Research ◽  
The Tropics

Surface observations have recorded large and incompletely understood changes to atmospheric methane (CH 4 ) this century. However, their ability to reveal the responsible surface sources and sinks is limited by their geographical distribution, which is biased towards the northern midlatitudes. Data from Earth-orbiting satellites designed specifically to measure atmospheric CH 4 have been available since 2009 with the launch of the Japanese Greenhouse gases Observing SATellite (GOSAT). We assess the added value of GOSAT to data collected by the US National Oceanic and Atmospheric Administration (NOAA), which have been the lynchpin for knowledge about atmospheric CH 4 since the 1980s. To achieve that we use the GEOS-Chem atmospheric chemistry transport model and an inverse method to infer a posteriori flux estimates from the NOAA and GOSAT data using common a priori emission inventories. We find the main benefit of GOSAT data is from its additional coverage over the tropics where we report large increases since the 2014/2016 El Niño, driven by biomass burning, biogenic emissions and energy production. We use data from the European TROPOspheric Monitoring Instrument to show how better spatial coverage and resolution measurements allow us to quantify previously unattainable diffuse sources of CH 4 , thereby opening up a new research frontier. This article is part of a discussion meeting issue ‘Rising methane: is warming feeding warming? (part 1)’.

scholarly journals Nitrogen deposition in the UK at 1 km resolution from 1990 to 2017

2021 ◽  
Author(s):  
Samuel James Tomlinson ◽  
Edward John Carnell ◽  
Anthony J. Dore ◽  
Ulrike Dragosits
Keyword(s):  
Atmospheric Chemistry ◽  
Transport Model ◽  
N Deposition ◽  
Nitrogen Oxide Emissions ◽  
Chemistry Transport Model ◽  
Wet And Dry Deposition ◽  
Coarse Spatial Resolution ◽  
Reduce Emissions ◽  
The Uk

Abstract. An atmospheric chemistry transport model (FRAME) is used here to calculate the UK N deposition for the years 1990–2017. Reactive nitrogen (N) deposition is a threat that can lead to adverse effects on the environment and human health. In Europe, substantial reductions in N deposition from nitrogen oxide emissions have been achieved in recent decades, this paper quantifies reductions in UK N deposition following the N emissions peak in 1990. In the UK, estimates of N deposition are typically available at a coarse spatial resolution (typically 5 km × 5 km grid resolution) and it is often difficult to compare estimates between years due to methodological changes in emission estimates. Through efforts to reduce emissions of N from industry, traffic, and agriculture, this study predicts that UK N deposition has reduced from 465 kt N in 1990 to 278 kt N in 2017. However, as part of this overall reduction, there are non-uniform changes for wet and dry deposition of reduced N (NHx) and oxidised N (NOy). In 2017, it is estimated 59 % of all N deposition is in the form of reduced N, a change from 35 % in 1990. This dataset uses 28 years of emissions data from 1990 to 2017 to produce the first long-term dataset of 28 years of N deposition at 1 km × 1 km resolution in the UK.

scholarly journals Atmospheric methane isotopic record favors fossil sources flat in 1980s and 1990s with recent increase

2016 ◽  
Vol 113 (39) ◽  
pp. 10791-10796 ◽  
Author(s):  
Andrew L. Rice ◽  
Christopher L. Butenhoff ◽  
Doaa G. Teama ◽  
Florian H. Röger ◽  
M. Aslam K. Khalil ◽  
...  
Keyword(s):  
Fossil Fuel ◽  
Transport Model ◽  
Atmospheric Methane ◽  
Chemical Transport Model ◽  
Sensitivity Tests ◽  
Stable Isotopic ◽  
Methane Fluxes ◽  
Emissions Inventories ◽  
Year 2000 ◽  
Fossil Fuel Emissions

Observations of atmospheric methane (CH4) since the late 1970s and measurements of CH4 trapped in ice and snow reveal a meteoric rise in concentration during much of the twentieth century. Since 1750, levels of atmospheric CH4 have more than doubled to current globally averaged concentration near 1,800 ppb. During the late 1980s and 1990s, the CH4 growth rate slowed substantially and was near or at zero between 1999 and 2006. There is no scientific consensus on the drivers of this slowdown. Here, we report measurements of the stable isotopic composition of atmospheric CH4 (13C/12C and D/H) from a rare air archive dating from 1977 to 1998. Together with more modern records of isotopic atmospheric CH4, we performed a time-dependent retrieval of methane fluxes spanning 25 y (1984–2009) using a 3D chemical transport model. This inversion results in a 24 [18, 27] Tg y−1 CH4 increase in fugitive fossil fuel emissions since 1984 with most of this growth occurring after year 2000. This result is consistent with some bottom-up emissions inventories but not with recent estimates based on atmospheric ethane. In fact, when forced with decreasing emissions from fossil fuel sources our inversion estimates unreasonably high emissions in other sources. Further, the inversion estimates a decrease in biomass-burning emissions that could explain falling ethane abundance. A range of sensitivity tests suggests that these results are robust.

scholarly journals Biological regulation of atmospheric chemistry en route to planetary oxygenation

2017 ◽  
Vol 114 (13) ◽  
pp. E2571-E2579 ◽  
Author(s):  
Gareth Izon ◽  
Aubrey L. Zerkle ◽  
Kenneth H. Williford ◽  
James Farquhar ◽  
Simon W. Poulton ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Atmospheric Chemistry ◽  
Atmospheric Oxygen ◽  
Earth System ◽  
Atmospheric Methane ◽  
Biological Regulation ◽  
Biological Source ◽  
The Earth ◽  
Methane Fluxes ◽  
Haze Formation

Emerging evidence suggests that atmospheric oxygen may have varied before rising irreversibly ∼2.4 billion years ago, during the Great Oxidation Event (GOE). Significantly, however, pre-GOE atmospheric aberrations toward more reducing conditions—featuring a methane-derived organic-haze—have recently been suggested, yet their occurrence, causes, and significance remain underexplored. To examine the role of haze formation in Earth’s history, we targeted an episode of inferred haze development. Our redox-controlled (Fe-speciation) carbon- and sulfur-isotope record reveals sustained systematic stratigraphic covariance, precluding nonatmospheric explanations. Photochemical models corroborate this inference, showing Δ36S/Δ33S ratios are sensitive to the presence of haze. Exploiting existing age constraints, we estimate that organic haze developed rapidly, stabilizing within ∼0.3 ± 0.1 million years (Myr), and persisted for upward of ∼1.4 ± 0.4 Myr. Given these temporal constraints, and the elevated atmospheric CO2 concentrations in the Archean, the sustained methane fluxes necessary for haze formation can only be reconciled with a biological source. Correlative δ13COrg and total organic carbon measurements support the interpretation that atmospheric haze was a transient response of the biosphere to increased nutrient availability, with methane fluxes controlled by the relative availability of organic carbon and sulfate. Elevated atmospheric methane concentrations during haze episodes would have expedited planetary hydrogen loss, with a single episode of haze development providing up to 2.6–18 × 1018 moles of O2 equivalents to the Earth system. Our findings suggest the Neoarchean likely represented a unique state of the Earth system where haze development played a pivotal role in planetary oxidation, hastening the contingent biological innovations that followed.

scholarly journals Five years of CO, HCN, C<sub>2</sub>H<sub>6</sub>, C<sub>2</sub>H<sub>2</sub>, CH<sub>3</sub>OH, HCOOH, and H<sub>2</sub>CO total columns measured in the Canadian High Arctic

2013 ◽  
Vol 6 (6) ◽  
pp. 11345-11403
Author(s):  
C. Viatte ◽  
K. Strong ◽  
K. A. Walker ◽  
J. R. Drummond
Keyword(s):  
Fourier Transform ◽  
Biomass Burning ◽  
Atmospheric Chemistry ◽  
A Priori ◽  
Estimation Method ◽  
Correlation Coefficients ◽  
Optimal Estimation ◽  
High Arctic ◽  
Retrieval Algorithm ◽  
Atmospheric Variability

Abstract. We present a five-year timeseries of seven tropospheric species measured using a ground-based Fourier Transform InfraRed (FTIR) spectrometer at the Polar Environment Atmospheric Research Laboratory (PEARL, Eureka, Nunavut, Canada, 80°05' N, 86°42' W) from 2007 to 2011. Total columns and temporal variabilities of carbon monoxide (CO), hydrogen cyanide (HCN), and ethane (C2H6), as well as the first derived total columns at Eureka of acetylene (C2H2), methanol (CH3OH), formic acid (HCOOH), and formaldehyde (H2CO) are investigated, providing a new dataset in the sparsely sampled high latitudes. Total columns are obtained using the SFIT2 retrieval algorithm based on the Optimal Estimation Method. The microwindows, as well as the a priori profiles and variabilities are selected to optimize the information content of the retrievals, and error analyses are performed for all seven species. Our retrievals show good sensitivities in the troposphere. The seasonal amplitudes of the timeseries, ranging from 34 to 104%, are captured while using a single a priori profile for each species. The timeseries of the CO, C2H6 and C2H2 total columns at PEARL exhibit strong seasonal cycles with maxima in winter and minima in summer, in opposite phase to the HCN, CH3OH, HCOOH and H2CO timeseries. These cycles result from the relative contributions of the photochemistry, oxidation, and transport, as well as biogenic and biomass burning emissions. Comparisons of the FTIR partial columns with coincident satellite measurements by the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) show good agreement. The correlation coefficients and the slopes range from 0.56 to 0.97, and 0.50 to 3.35, respectively, for the seven target species. Our new dataset is compared with previous measurements found in the literature to assess atmospheric budgets of these tropospheric species in the high Arctic. The CO and C2H6 concentrations are consistent with negative trends observed over the Northern Hemisphere, attributed to fossil fuel emission decrease. The importance of poleward transport on the atmospheric budgets of HCN and C2H2 is highlighted. Columns and variabilities of CH3OH, and HCOOH at PEARL are comparable to previous measurements performed at other remote sites. However, the small columns of H2CO in early May might reflect its large atmospheric variability, and/or the effect of the updated spectroscopic parameters used in our retrievals. Overall, emissions from biomass burning contribute to the day-to-day variabilities of the seven tropospheric species observed at Eureka.

scholarly journals Inter-model comparison of global hydroxyl radical (OH) distributions and their impact on atmospheric methane over the 2000–2016 period

2019 ◽  
Vol 19 (21) ◽  
pp. 13701-13723 ◽  
Author(s):  
Yuanhong Zhao ◽  
Marielle Saunois ◽  
Philippe Bousquet ◽  
Xin Lin ◽  
Antoine Berchet ◽  
...  
Keyword(s):  
Hydroxyl Radical ◽  
Atmospheric Chemistry ◽  
Model Comparison ◽  
Emission Scenario ◽  
Transport Model ◽  
Historical Period ◽  
Mixing Ratio ◽  
Atmospheric Methane ◽  
Vertical Distributions ◽  
The Impact

Abstract. The modeling study presented here aims to estimate how uncertainties in global hydroxyl radical (OH) distributions, variability, and trends may contribute to resolving discrepancies between simulated and observed methane (CH4) changes since 2000. A multi-model ensemble of 14 OH fields was analyzed and aggregated into 64 scenarios to force the offline atmospheric chemistry transport model LMDz (Laboratoire de Meteorologie Dynamique) with a standard CH4 emission scenario over the period 2000–2016. The multi-model simulated global volume-weighted tropospheric mean OH concentration ([OH]) averaged over 2000–2010 ranges between 8.7×105 and 12.8×105 molec cm−3. The inter-model differences in tropospheric OH burden and vertical distributions are mainly determined by the differences in the nitrogen oxide (NO) distributions, while the spatial discrepancies between OH fields are mostly due to differences in natural emissions and volatile organic compound (VOC) chemistry. From 2000 to 2010, most simulated OH fields show an increase of 0.1–0.3×105 molec cm−3 in the tropospheric mean [OH], with year-to-year variations much smaller than during the historical period 1960–2000. Once ingested into the LMDz model, these OH changes translated into a 5 to 15 ppbv reduction in the CH4 mixing ratio in 2010, which represents 7 %–20 % of the model-simulated CH4 increase due to surface emissions. Between 2010 and 2016, the ensemble of simulations showed that OH changes could lead to a CH4 mixing ratio uncertainty of >±30 ppbv. Over the full 2000–2016 time period, using a common state-of-the-art but nonoptimized emission scenario, the impact of [OH] changes tested here can explain up to 54 % of the gap between model simulations and observations. This result emphasizes the importance of better representing OH abundance and variations in CH4 forward simulations and emission optimizations performed by atmospheric inversions.

scholarly journals Impact of atomic chlorine on the modelling of total methane and its <sup>13</sup>C : <sup>12</sup>C isotopic ratio at global scale

2019 ◽  
Author(s):  
Joël Thanwerdas ◽  
Marielle Saunois ◽  
Antoine Berchet ◽  
Isabelle Pison ◽  
Didier Hauglustaine ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Transport Model ◽  
Isotopic Ratio ◽  
Circulation Model ◽  
Global Scale ◽  
Major Influence ◽  
Atmospheric Methane ◽  
Global Circulation Model ◽  
Substantial Impact ◽  
The Impact

Abstract. Methane (CH4) is the second strongest anthropogenic greenhouse gas after carbon dioxide (CO2) and is responsible for about 20 % of the warming induced by long-lived greenhouse gases since pre-industrial times. Oxidation by the hydroxyl radical (OH) is the dominant atmospheric sink for methane, contributing to approximately 90 % of the total methane loss. Chemical losses by reaction with atomic oxygen (O1D) and chlorine radicals (Cl) in the stratosphere are other sinks, contributing about 3 % to the total methane destruction. Moreover, the reaction with Cl is very fractionating, thus it has a much larger impact on δ13C-CH4 than the reaction with OH. In this paper, we assess the impact of atomic Cl on atmospheric methane mixing ratios, methane atmospheric loss and atmospheric δ13C-CH4. The offline version of the Global Circulation Model (GCM) LMDz, coupled to a chemistry module including the major methane chemical reactions, is run to simulate CH4 concentrations and δ13C-CH4 at the global scale. Atmospheric methane sink by Cl atoms in the stratosphere is found to be 7.32 ± 0.16 Tg/yr. Methane observations from vertical profiles obtained using AirCore samplers above 11 different locations across the globe and balloon measurements of δ13C-CH4 and methane are used to assess the impact of the Cl sink in the chemistry transport model. Above 10 km, the presence of Cl in the model is found to have only a small impact on the vertical profile of total methane but a major influence on δ13C-CH4 values, significantly improving the agreement between simulations and available observations. Stratospheric Cl is also found to have a substantial impact on surface δ13C-CH4 values, leading to a difference of +0.27 ‰ (less negative values) after a 19-year run. As a result, this study suggests that the Cl sink needs to be properly taken into account (magnitude and trends) in order to better understand trends in the atmospheric δ13C-CH4 signal when using atmospheric chemistry transport models for forward or inverse calculations.

scholarly journals Inter-model comparison of global hydroxyl radical (OH) distributions and their impact on atmospheric methane over the 2000–2016 period

2019 ◽  
Author(s):  
Yuanhong Zhao ◽  
Marielle Saunois ◽  
Philippe Bousquet ◽  
Xin Lin ◽  
Michaela I. Hegglin ◽  
...  
Keyword(s):  
Hydroxyl Radical ◽  
Atmospheric Chemistry ◽  
Model Comparison ◽  
Emission Scenario ◽  
Transport Model ◽  
Historical Period ◽  
Mixing Ratio ◽  
Atmospheric Methane ◽  
Vertical Distributions ◽  
The Impact

Abstract. The modeling study presented here aims to estimate how uncertainties in global hydroxyl radical (OH) distributions, variability, and trends may contribute to resolve discrepancies between simulated and observed methane (CH4) changes since 2000. A multi-model ensemble of 14 OH fields were analysed and were aggregated into 64 scenarios to force the offline atmospheric chemistry transport model LMDz with a standard CH4 emission scenario over the period 2000–2016. The multi-model simulated global volume-weighted tropospheric mean OH concentration ([OH]) averaged over 2000–2010 ranges between 8.7 × 105 and 12.8 × 105 molec cm−3. The inter-model differences in tropospheric OH burden and vertical distributions are mainly determined by the differences in the nitrogen oxide (NO) distributions, while the spatial discrepancies between OH fields are mostly due to differences in natural emissions and VOC chemistry. From 2000 to 2010, most simulated OH fields show an increase of 0.1–0.3 × 105 molec cm−3 in the tropospheric mean [OH], with year-to-year variations much smaller than during the historical period 1960–2000. Once ingested into the LMDz model, these OH changes translated into a 5 to 15 ppbv reduction in CH4 mixing ratio in 2010, which represent 7 %–20 % of the model simulated CH4 increase due to surface emissions. Between 2010 and 2016, the ensemble of simulations showed that OH changes could lead to a CH4 mixing ratio uncertainty of > ±30 ppbv. Over the full 2000–2016 time period, using a common state-of-the-art but non-optimized emission scenario, the impact of [OH] changes tested here can explain up to 54 % of the gap between model simulations and observations. This result emphasizes the importance of better representing OH abundance and variations in CH4 forward simulations and emission optimizations performed by atmospheric inversions.

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