scholarly journals Inverse modelling of carbonyl sulfide: implementation, evaluation and implications for the global budget

2021 ◽  
Vol 21 (5) ◽  
pp. 3507-3529
Author(s):  
Jin Ma ◽  
Linda M. J. Kooijmans ◽  
Ara Cho ◽  
Stephen A. Montzka ◽  
Norbert Glatthor ◽  
...  
Keyword(s):  
Mole Fraction ◽  
Satellite Data ◽  
Dimethyl Sulfide ◽  
Transport Model ◽  
Carbonyl Sulfide ◽  
Stratospheric Aerosol ◽  
Inverse Modelling ◽  
Model Framework ◽  
Tropical Ocean ◽  
Biosphere Model

Abstract. Carbonyl sulfide (COS) has the potential to be used as a climate diagnostic due to its close coupling to the biospheric uptake of CO2 and its role in the formation of stratospheric aerosol. The current understanding of the COS budget, however, lacks COS sources, which have previously been allocated to the tropical ocean. This paper presents a first attempt at global inverse modelling of COS within the 4-dimensional variational data-assimilation system of the TM5 chemistry transport model (TM5-4DVAR) and a comparison of the results with various COS observations. We focus on the global COS budget, including COS production from its precursors carbon disulfide (CS2) and dimethyl sulfide (DMS). To this end, we implemented COS uptake by soil and vegetation from an updated biosphere model (Simple Biosphere Model – SiB4). In the calculation of these fluxes, a fixed atmospheric mole fraction of 500 pmol mol−1 was assumed. We also used new inventories for anthropogenic and biomass burning emissions. The model framework is capable of closing the COS budget by optimizing for missing emissions using NOAA observations in the period 2000–2012. The addition of 432 Gg a−1 (as S equivalents) of COS is required to obtain a good fit with NOAA observations. This missing source shows few year-to-year variations but considerable seasonal variations. We found that the missing sources are likely located in the tropical regions, and an overestimated biospheric sink in the tropics cannot be ruled out due to missing observations in the tropical continental boundary layer. Moreover, high latitudes in the Northern Hemisphere require extra COS uptake or reduced emissions. HIPPO (HIAPER Pole-to-Pole Observations) aircraft observations, NOAA airborne profiles from an ongoing monitoring programme and several satellite data sources are used to evaluate the optimized model results. This evaluation indicates that COS mole fractions in the free troposphere remain underestimated after optimization. Assimilation of HIPPO observations slightly improves this model bias, which implies that additional observations are urgently required to constrain sources and sinks of COS. We finally find that the biosphere flux dependency on the surface COS mole fraction (which was not accounted for in this study) may substantially lower the fluxes of the SiB4 biosphere model over strong-uptake regions. Using COS mole fractions from our inversion, the prior biosphere flux reduces from 1053 to 851 Gg a−1, which is closer to 738 Gg a−1 as was found by Berry et al. (2013). In planned further studies we will implement this biosphere dependency and additionally assimilate satellite data with the aim of better separating the role of the oceans and the biosphere in the global COS budget.

scholarly journals Inverse modelling of carbonyl sulfide: implementation, evaluation and implications for the global budget

2020 ◽  
Author(s):  
Jin Ma ◽  
Linda M. J. Kooijmans ◽  
Ara Cho ◽  
Stephen A. Montzka ◽  
Norbert Glatthor ◽  
...  
Keyword(s):  
Satellite Data ◽  
Dimethyl Sulfide ◽  
Transport Model ◽  
Carbonyl Sulfide ◽  
Monitoring Program ◽  
Stratospheric Aerosol ◽  
Inverse Modelling ◽  
Model Framework ◽  
Tropical Ocean ◽  
Biosphere Model

Abstract. Carbonyl sulfide (COS) has the potential to be used as a climate diagnostic due to its close coupling to the biospheric uptake of CO2 and its role in the formation of stratospheric aerosol. The current understanding of the COS budget, however, lacks COS sources, which have previously been allocated to the tropical ocean. This paper presents a first attempt of global inverse modelling of COS within the 4-Dimensional variational data-assimilation system of the TM5 chemistry transport model (TM5-4DVAR) and a comparison of the results with independent COS observations. We focus on the global COS budget, including COS production from its precursors carbon disulfide (CS2) and dimethyl sulfide (DMS). To this end, we implemented COS uptake by soil and vegetation from an updated biosphere model (SiB4), and new inventories for anthropogenic and biomass burning emissions. The model framework is capable of closing the COS budget by optimizing for missing emissions using NOAA observations in the period 2000–2012. The addition of 432 Gg S a−1 COS is required to obtain a good fit with NOAA observations. This missing source shows little year-to-year variations, but considerable seasonal variations. We found that the missing sources are likely located in the tropical regions, and an overestimated biospheric sink in the tropics cannot be ruled out. Moreover, high latitudes in the Northern Hemisphere require extra COS uptake or reduced emissions. HIPPO aircraft observations, NOAA airborne profiles from an ongoing monitoring program, and several satellite data sources are used to evaluate the optimized model results. This evaluation indicates that COS in the free troposphere remains underestimated after optimization. Assimilation of HIPPO observations slightly improves this model bias, which implies that additional observations are urgently required to constrain sources and sinks of COS. We finally find that the biosphere flux dependency on surface COS mixing ratio may substantially lower the fluxes of the SiB4 biosphere model over strong uptake regions. In planned further studies we will implement this biosphere dependency, and additionally assimilate satellite data with the aim to better separate the role of the oceans and the biosphere in the global COS budget.

scholarly journals Sensitivity of the recent methane budget to LMDz sub-grid scale physical parameterizations

2015 ◽  
Vol 15 (8) ◽  
pp. 11853-11888
Author(s):  
R. Locatelli ◽  
P. Bousquet ◽  
M. Saunois ◽  
F. Chevallier ◽  
C. Cressot
Keyword(s):  
Satellite Data ◽  
Transport Model ◽  
Deep Convection ◽  
Chemical Transport ◽  
Global Scale ◽  
Methane Emissions ◽  
Inverse Modelling ◽  
Chemical Transport Model ◽  
Methane Budget ◽  
Physical Parameterizations

Abstract. With the densification of surface observing networks and the development of remote sensing of greenhouse gases from space, estimations of methane (CH4) sources and sinks by inverse modelling face new challenges. Indeed, the chemical transport model used to link the flux space with the mixing ratio space must be able to represent these different types of constraints for providing consistent flux estimations. Here we quantify the impact of sub-grid scale physical parameterization errors on the global methane budget inferred by inverse modelling using the same inversion set-up but different physical parameterizations within one chemical-transport model. Two different schemes for vertical diffusion, two others for deep convection, and one additional for thermals in the planetary boundary layer are tested. Different atmospheric methane datasets are used as constraints (surface observations or satellite retrievals). At the global scale, methane emissions differ, on average, from 4.1 Tg CH4 per year due to the use of different sub-grid scale parameterizations. Inversions using satellite total-column retrieved by GOSAT satellite are less impacted, at the global scale, by errors in physical parameterizations. Focusing on large-scale atmospheric transport, we show that inversions using the deep convection scheme of Emanuel (1991) derive smaller interhemispheric gradient in methane emissions. At regional scale, the use of different sub-grid scale parameterizations induces uncertainties ranging from 1.2 (2.7%) to 9.4% (14.2%) of methane emissions in Africa and Eurasia Boreal respectively when using only surface measurements from the background (extended) surface network. When using only satellite data, we show that the small biases found in inversions using GOSAT-CH4 data and a coarser version of the transport model were actually masking a poor representation of the stratosphere–troposphere gradient in the model. Improving the stratosphere–troposphere gradient reveals a larger bias in GOSAT-CH4 satellite data, which largely amplifies inconsistencies between surface and satellite inversions. A simple bias correction is proposed. The results of this work provide the level of confidence one can have for recent methane inversions relatively to physical parameterizations included in chemical-transport models.

scholarly journals Atmospheric methane source and sink sensitivity analysis using Gaussian process emulation

2020 ◽  
Author(s):  
Angharad C. Stell ◽  
Luke M. Western ◽  
Matthew Rigby
Keyword(s):  
Gaussian Process ◽  
Mole Fraction ◽  
Transport Model ◽  
Chemical Transport ◽  
Inverse Modelling ◽  
Atmospheric Methane ◽  
Chemical Transport Model ◽  
Gaussian Process Emulation ◽  
Source And Sink ◽  
Inputs And Outputs

Abstract. We present a method to efficiently approximate the response of atmospheric methane mole fraction and δ13C-CH4 to changes in uncertain emission and loss parameters in a three-dimensional global chemical transport model. Our approach, based on Gaussian process emulation, allows relationships between inputs and outputs in the model to be efficiently explored. The presented emulator successfully reproduces the chemical transport model output with a root-mean-square error of 1.2 ppb and 0.06 ‰ for hemispheric methane mole fraction and δ13C-CH4, respectively, for 28 uncertain model inputs. The method is shown to outperform multiple linear regression, because it captures non-linear relationships between inputs and outputs, as well as the interaction between model input parameters. The emulator was used to determine how sensitive methane mole fraction and δ13C-CH4 are to the major source and sink components of the atmospheric budget, given current estimates of their uncertainty. We find that our current knowledge of the methane budget, as inferred through hemispheric mole fraction observations, is limited primarily by uncertainty in the global mean hydroxyl radical concentration and emissions from fresh water. Our work quantitatively determines the added value of measurements of δ13C-CH4, which are sensitive to some uncertain parameters that mole fraction observations on their own are not. However, we demonstrate the critical importance of constraining isotopic initial conditions and isotopic source signatures, small uncertainties in which strongly influence long-term δ13C-CH4 trends, because of the long timescales over which transient perturbations propagate through the atmosphere. Our results also demonstrate that the magnitude and trend of methane mole fraction and δ13C-CH4 can be strongly influenced by the combined uncertainty of more minor components of the atmospheric budget, which are often fixed and assumed to be well-known in inverse modelling studies (e.g. emissions from termites, hydrates, and oceans). Overall, our work provides an overview of the sensitivity of atmospheric observations to budget uncertainties and outlines a method which could be employed to account for these uncertainties in future inverse modelling systems.

scholarly journals Evaluation of carbonyl sulfide biosphere exchange in the Simple Biosphere Model (SiB4)

2021 ◽  
Vol 18 (24) ◽  
pp. 6547-6565
Author(s):  
Linda M. J. Kooijmans ◽  
Ara Cho ◽  
Jin Ma ◽  
Aleya Kaushik ◽  
Katherine D. Haynes ◽  
...  
Keyword(s):  
Mole Fraction ◽  
Mechanistic Model ◽  
Carbonyl Sulfide ◽  
Growing Season ◽  
Global Scale ◽  
Terrestrial Plants ◽  
Large Variability ◽  
Accurate Representation ◽  
High Productivity ◽  
Biosphere Model

Abstract. The uptake of carbonyl sulfide (COS) by terrestrial plants is linked to photosynthetic uptake of CO2 as these gases partly share the same uptake pathway. Applying COS as a photosynthesis tracer in models requires an accurate representation of biosphere COS fluxes, but these models have not been extensively evaluated against field observations of COS fluxes. In this paper, the COS flux as simulated by the Simple Biosphere Model, version 4 (SiB4), is updated with the latest mechanistic insights and evaluated with site observations from different biomes: one evergreen needleleaf forest, two deciduous broadleaf forests, three grasslands, and two crop fields spread over Europe and North America. We improved SiB4 in several ways to improve its representation of COS. To account for the effect of atmospheric COS mole fractions on COS biosphere uptake, we replaced the fixed atmospheric COS mole fraction boundary condition originally used in SiB4 with spatially and temporally varying COS mole fraction fields. Seasonal amplitudes of COS mole fractions are ∼50–200 ppt at the investigated sites with a minimum mole fraction in the late growing season. Incorporating seasonal variability into the model reduces COS uptake rates in the late growing season, allowing better agreement with observations. We also replaced the empirical soil COS uptake model in SiB4 with a mechanistic model that represents both uptake and production of COS in soils, which improves the match with observations over agricultural fields and fertilized grassland soils. The improved version of SiB4 was capable of simulating the diurnal and seasonal variation in COS fluxes in the boreal, temperate, and Mediterranean region. Nonetheless, the daytime vegetation COS flux is underestimated on average by 8±27 %, albeit with large variability across sites. On a global scale, our model modifications decreased the modeled COS terrestrial biosphere sink from 922 Gg S yr−1 in the original SiB4 to 753 Gg S yr−1 in the updated version. The largest decrease in fluxes was driven by lower atmospheric COS mole fractions over regions with high productivity, which highlights the importance of accounting for variations in atmospheric COS mole fractions. The change to a different soil model, on the other hand, had a relatively small effect on the global biosphere COS sink. The secondary role of the modeled soil component in the global COS budget supports the use of COS as a global photosynthesis tracer. A more accurate representation of COS uptake in SiB4 should allow for improved application of atmospheric COS as a tracer of local- to global-scale terrestrial photosynthesis.

scholarly journals Towards understanding the variability in biospheric CO<sub>2</sub> fluxes: using FTIR spectrometry and a chemical transport model to investigate the sources and sinks of carbonyl sulfide and its link to CO<sub>2</sub>

2016 ◽  
Vol 16 (4) ◽  
pp. 2123-2138 ◽  
Author(s):  
Yuting Wang ◽  
Nicholas M. Deutscher ◽  
Mathias Palm ◽  
Thorsten Warneke ◽  
Justus Notholt ◽  
...  
Keyword(s):  
Northern Hemisphere ◽  
Transport Model ◽  
Carbonyl Sulfide ◽  
Co2 Concentration ◽  
Chemical Transport ◽  
Chemical Transport Model ◽  
Solar Absorption ◽  
Ftir Spectrometry ◽  
Carbon Dioxide Co2 ◽  
Biosphere Model

Abstract. Understanding carbon dioxide (CO2) biospheric processes is of great importance because the terrestrial exchange drives the seasonal and interannual variability of CO2 in the atmosphere. Atmospheric inversions based on CO2 concentration measurements alone can only determine net biosphere fluxes, but not differentiate between photosynthesis (uptake) and respiration (production). Carbonyl sulfide (OCS) could provide an important additional constraint: it is also taken up by plants during photosynthesis but not emitted during respiration, and therefore is a potential means to differentiate between these processes. Solar absorption Fourier Transform InfraRed (FTIR) spectrometry allows for the retrievals of the atmospheric concentrations of both CO2 and OCS from measured solar absorption spectra. Here, we investigate co-located and quasi-simultaneous FTIR measurements of OCS and CO2 performed at five selected sites located in the Northern Hemisphere. These measurements are compared to simulations of OCS and CO2 using a chemical transport model (GEOS-Chem). The coupled biospheric fluxes of OCS and CO2 from the simple biosphere model (SiB) are used in the study. The CO2 simulation with SiB fluxes agrees with the measurements well, while the OCS simulation reproduced a weaker drawdown than FTIR measurements at selected sites, and a smaller latitudinal gradient in the Northern Hemisphere during growing season when comparing with HIPPO (HIAPER Pole-to-Pole Observations) data spanning both hemispheres. An offset in the timing of the seasonal cycle minimum between SiB simulation and measurements is also seen. Using OCS as a photosynthesis proxy can help to understand how the biospheric processes are reproduced in models and to further understand the carbon cycle in the real world.

scholarly journals Atmospheric-methane source and sink sensitivity analysis using Gaussian process emulation

2021 ◽  
Vol 21 (3) ◽  
pp. 1717-1736
Author(s):  
Angharad C. Stell ◽  
Luke M. Western ◽  
Tomás Sherwen ◽  
Matthew Rigby
Keyword(s):  
Gaussian Process ◽  
Mole Fraction ◽  
Transport Model ◽  
Chemical Transport ◽  
Inverse Modelling ◽  
Atmospheric Methane ◽  
Chemical Transport Model ◽  
Gaussian Process Emulation ◽  
Source And Sink ◽  
Inputs And Outputs

Abstract. We present a method to efficiently approximate the response of atmospheric-methane mole fraction and δ13C–CH4 to changes in uncertain emission and loss parameters in a three-dimensional global chemical transport model. Our approach, based on Gaussian process emulation, allows relationships between inputs and outputs in the model to be efficiently explored. The presented emulator successfully reproduces the chemical transport model output with a root-mean-square error of 1.0 ppb and 0.05 ‰ for hemispheric-methane mole fraction and δ13C–CH4, respectively, for 28 uncertain model inputs. The method is shown to outperform multiple linear regression because it captures non-linear relationships between inputs and outputs as well as the interaction between model input parameters. The emulator was used to determine how sensitive methane mole fraction and δ13C–CH4 are to the major source and sink components of the atmospheric budget given current estimates of their uncertainty. We find that our current knowledge of the methane budget, as inferred through hemispheric mole fraction observations, is limited primarily by uncertainty in the global mean hydroxyl radical concentration and freshwater emissions. Our work quantitatively determines the added value of measurements of δ13C–CH4, which are sensitive to some uncertain parameters to which mole fraction observations on their own are not. However, we demonstrate the critical importance of constraining isotopic initial conditions and isotopic source signatures, small uncertainties in which strongly influence long-term δ13C–CH4 trends because of the long timescales over which transient perturbations propagate through the atmosphere. Our results also demonstrate that the magnitude and trend of methane mole fraction and δ13C–CH4 can be strongly influenced by the combined uncertainty in more minor components of the atmospheric budget, which are often fixed and assumed to be well-known in inverse-modelling studies (e.g. emissions from termites, hydrates, and oceans). Overall, our work provides an overview of the sensitivity of atmospheric observations to budget uncertainties and outlines a method which could be employed to account for these uncertainties in future inverse-modelling systems.

Inverse modelling of Carbonyl Sulfide (COS): towards nonlinear model and satellite data assimilation

2021 ◽  
Author(s):  
Jin Ma ◽  
Linda M.J Kooijmans ◽  
Ara Cho ◽  
Stephen A. Montzka ◽  
Norbert Glatthor ◽  
...  
Keyword(s):  
Data Assimilation ◽  
Satellite Data ◽  
Transport Model ◽  
Gross Primary Production ◽  
Current Model ◽  
Carbonyl Sulfide ◽  
Linear Inversion ◽  
Sources And Sinks ◽  
First Order ◽  
The Tropics

&lt;p&gt;Atmospheric Carbonyl Sulfide (COS) is a useful tracer for assessing gross primary production (GPP). COS is also an important contributor to stratospheric sulfate aerosols (SSA) which cool the climate. However, the global budget of COS remains unresolved due to insufficient observations. We implemented a linear inversion framework within the TM5-4DVAR global chemistry transport model constrained by NOAA surface network to investigate the sources and sinks of COS (Ma et al., 2020). To close the gap between sources and sinks, we focused on inversions that optimize what is thought to be a &amp;#8220;missing&amp;#8221; source amounting to 432 GgS a&lt;sup&gt;-1&lt;/sup&gt;. We found that a tropical missing source was likely, which could either be an indication of an underestimated ocean source, or overestimated biosphere uptake. Additionally, we found the biosphere uptake to be underestimated at higher latitudes of the Northern Hemisphere. Inversions were validated with HIPPO aircraft data, NOAA airborne profiles and satellite data (MIPAS, TES and ACE-FTS), indicating an underestimation of COS in troposphere. We further implemented a first-order dependency of COS biosphere flux on COS mole fractions in the atmosphere boundary layer, which renders the inversions nonlinear. As expected based on the known drawdown of COS by biosphere uptake, it is found that the dependence of the biosphere flux on COS mole fractions reduced the budget gap by 137 GgS a&lt;sup&gt;-1&lt;/sup&gt;. We further optimized COS fluxes separately over ocean and land, accounting for the first-order dependency of biosphere uptake on COS mole fractions. These results suggest that the missing COS sources may originate from the ocean (207 GgS a&lt;sup&gt;-1&lt;/sup&gt;), despite recent work in which the ocean is explicitly studied suggesting otherwise.&amp;#160; Understanding this apparent discrepancy will be an important topic to elucidate. In the future, we plan to take the advantage of available satellite data products to better constrain the COS flux budget in the tropics. COS products from the MIPAS and TES satellites are good candidates for data assimilation in the current model.&lt;/p&gt;

scholarly journals Evaluation of carbonyl sulfide biosphere exchange in the Simple Biosphere Model (SiB4)

2021 ◽  
Author(s):  
Linda M. J. Kooijmans ◽  
Ara Cho ◽  
Jin Ma ◽  
Aleya Kaushik ◽  
Katherine D. Haynes ◽  
...  
Keyword(s):  
Mole Fraction ◽  
Mechanistic Model ◽  
Carbonyl Sulfide ◽  
Global Scale ◽  
Terrestrial Plants ◽  
Large Variability ◽  
High Productivity ◽  
Crop Fields ◽  
Soil Component ◽  
Biosphere Model

Abstract. The uptake of carbonyl sulfide (COS) by terrestrial plants is linked to photosynthetic uptake of CO2 by a shared diffusion pathway. Applying COS as a photosynthesis tracer in models requires an accurate representation of biosphere COS fluxes, but these models have not been extensively evaluated against field observations of COS fluxes. In this paper, the COS flux as simulated by the Simple Biosphere Model, version 4 (SiB4) is updated with the latest mechanistic insights and evaluated with site observations from different biomes: one evergreen needleleaf forest, two deciduous broadleaf forests, three grasslands, and two crop fields spread over Europe and North America. To account for the effect of atmospheric COS mole fractions on COS biosphere uptake, we replaced the fixed COS mole fraction originally used in SiB4 with spatially and temporally varying COS mole fraction fields. The lower COS mole fractions in the late growing season reduces COS uptake rates in agreement with observations. We also replaced the empirical soil COS uptake model in SiB4 with a mechanistic model that represents both uptake and production of COS in soils, which improves the match with observations over agricultural fields and fertilized grassland soils. SiB4 was capable of simulating the diurnal and seasonal variation of COS fluxes in the boreal, temperate and Mediterranean region. The daytime vegetation COS flux is on average 8 ± 27 % underestimated, albeit with large variability across sites. On a global scale, our model modifications caused a drop in the COS biosphere sink from 922 Gg S yr−1 in the original SiB4 model to 753 Gg S yr−1 in the updated version. The largest drop in fluxes was driven by lower atmospheric COS mole fractions over regions with high productivity, which highlights the importance of accounting for variations in atmospheric COS mole fractions. The change to a different soil model, on the other hand, had a relatively small effect on the global biosphere COS sink. The small role of the modeled soil component in the COS budget supports the use of COS as a global photosynthesis tracer.

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