Abstract. The GEOS-Chem simulation of atmospheric CH4 was evaluated against observations from the Thermal and Near Infrared Sensor for Carbon Observations Fourier Transform Spectrometer (TANSO-FTS) on the Greenhouse Gases Observing Satellite (GOSAT), the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS), and the Total Carbon Column Observing Network (TCCON). We focused on the model simulations at the 4∘×5∘ and 2∘×2.5∘ horizontal resolutions for the period of February–May 2010. Compared to the GOSAT, TCCON, and ACE-FTS data, we found that the 2∘×2.5∘ model produced a better simulation of CH4, with smaller biases and a higher correlation to the independent data. We found large resolution-dependent differences such as a latitude-dependent XCH4 bias, with higher column abundances of CH4 at high latitudes and lower abundances at low latitudes at the 4∘×5∘ resolution than at 2∘×2.5∘. We also found large differences in CH4 column abundances between the two resolutions over major source regions such as China. These differences resulted in up to 30 % differences in inferred regional CH4 emission estimates from the two model resolutions. We performed several experiments using 222Rn, 7Be, and CH4 to determine the origins of the resolution-dependent errors. The results suggested that the major source of the latitude-dependent errors is excessive mixing in the upper troposphere and lower stratosphere, including mixing at the edge of the polar vortex, which is pronounced at the 4∘×5∘ resolution. At the coarser resolution, there is weakened vertical transport in the troposphere at midlatitudes to high latitudes due to the loss of sub-grid tracer eddy mass flux in the storm track regions. The vertical air mass fluxes are calculated in the model from the degraded coarse-resolution wind fields and the model does not conserve the air mass flux between model resolutions; as a result, the low resolution does not fully capture the vertical transport. This produces significant localized discrepancies, such as much greater CH4 abundances in the lower troposphere over China at 4∘×5∘ than at 2∘×2.5∘. Although we found that the CH4 simulation is significantly better at 2∘×2.5∘ than at 4∘×5∘, biases may still be present at 2∘×2.5∘ resolution. Their importance, particularly in regards to inverse modeling of CH4 emissions, should be evaluated in future studies using online transport in the native general circulation model as a benchmark simulation.

Abstract. We examined biases in the global GEOS-Chem chemical transport model for the period of February–May 2010 using weak-constraint (WC) four-dimensional variational (4D-Var) data assimilation and dry-air mole fractions of CH4 (XCH4) from the Greenhouse gases Observing SATellite (GOSAT). The ability of the observations and the WC 4D-Var method to mitigate model errors in CH4 concentrations was first investigated in a set of observing system simulation experiments (OSSEs). We then assimilated the GOSAT XCH4 retrievals and found that they were capable of providing information on the vertical structure of model errors and of removing a significant portion of biases in the modeled CH4 state. In the WC 4D-Var assimilation, corrections were added to the modeled CH4 state at each model time step to account for model errors and improve the model fit to the assimilated observations. Compared to the conventional strong-constraint (SC) 4D-Var assimilation, the WC method was able to significantly improve the model fit to independent observations. Examination of the WC state corrections suggested that a significant source of model errors was associated with discrepancies in the model CH4 in the stratosphere. The WC state corrections also suggested that the model vertical transport in the troposphere at middle and high latitudes is too weak. The problem was traced back to biases in the uplift of CH4 over the source regions in eastern China and North America. In the tropics, the WC assimilation pointed to the possibility of biased CH4 outflow from the African continent to the Atlantic in the mid-troposphere. The WC assimilation in this region would greatly benefit from glint observations over the ocean to provide additional constraints on the vertical structure of the model errors in the tropics. We also compared the WC assimilation at 4∘ × 5∘ and 2∘ × 2.5∘ horizontal resolutions and found that the WC corrections to mitigate the model errors were significantly larger at 4∘ × 5∘ than at 2∘ × 2.5∘ resolution, indicating the presence of resolution-dependent model errors. Our results illustrate the potential utility of the WC 4D-Var approach for characterizing model errors. However, a major limitation of this approach is the need to better characterize the specified model error covariance in the assimilation scheme.

Abstract. The GEOS-Chem simulation of atmospheric CH4 was evaluated against observations from the Thermal And Near infrared Sensor for carbon Observations Fourier Transform Spectrometer (TANSO-FTS) on the Greenhouse gases Observing SATellite (GOSAT), the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS), and the Total Carbon Column Observing Network (TCCON). We focused on the model simulations at the 4° × 5° and 2° × 2.5° horizontal resolutions for the period of February–May 2010. Compared to the GOSAT, TCCON, and ACE-FTS data, we found that the 2° × 2.5° model produced a better simulation of CH4, with smaller biases and a higher correlation to the independent data. We found large resolution-dependent differences such as a latitude-dependent XCH4 bias, with higher columns abundances of CH4 at high latitudes and lower abundances at low latitudes at the 4° × 5° resolution than at 2° × 2.5°. We also found large differences in CH4 column abundances between the two resolutions over major source regions such as China. These differences resulted in up to 30 % differences in inferred regional CH4 emission estimates from the two model resolutions. We performed several experiments using 222Rn, 7Be and CH4 to determine the origins of the resolution-dependent errors. The results suggested that the major source of the latitude-dependent errors is excessive mixing in the upper troposphere and lower stratosphere, including mixing at the edge of the polar vortex, that is pronounced at the 4° × 5° resolution. At the coarser resolution, there is weakened vertical transport in the troposphere at mid- to high latitudes due to the loss of sub-grid tracer eddy mass flux in the storm track regions. We also identified reduced vertical transport at the coarser resolution. The vertical air mass fluxes are calculated in the model from the degraded coarse-resolution wind fields and the model does not conserve the air mass flux between model resolutions; as a result, the low resolution does not fully capture the vertical transport. This produces significant localized discrepancies, such as much greater CH4 abundances in the lower troposphere over China at 4° × 5° than at 2° × 2.5°. Although we found that the CH4 simulation is significantly better at 2° × 2.5° than at 4° × 5°, biases may still be present at 2° × 2.5° resolution. Their importance, particularly, in regards to inverse modeling of CH4 emissions, should be evaluated in future studies using on-line transport in the native general circulation model as a benchmark simulation.

<p><strong>Abstract.</strong> We examined biases in the global GEOS-Chem chemical transport model for the period of February–May 2010 using weak constraint (WC) four-dimensional variational (4D-Var) data assimilation and dry-air mole fractions of CH<sub>4</sub> (XCH<sub>4</sub>) from the Greenhouse gases Observing SATellite (GOSAT). The ability of the observations and the WC 4D-Var method to mitigate model errors in CH<sub>4</sub> concentrations was first investigated in a set of observing system simulation experiments (OSSEs). We then assimilated the GOSAT XCH<sub>4</sub> retrievals and found that they were capable of differentiating the vertical distribution of model errors and of removing a significant portion of biases in the modelled CH<sub>4</sub> state. In the WC 4D-Var assimilation, corrections were added to the modeled CH<sub>4</sub> state at each model time step to account for model errors and improve the model fit to the assimilated observations. Compared to the conventional strong constraint (SC) 4D-Var assimilation, the WC method was able to significantly improve the model fit to independent observations. Examination of the WC state corrections suggested that a significant source of the model errors was associated with discrepancies in the model CH<sub>4</sub> in the stratosphere. The WC state corrections also suggested that the model vertical transport in the troposphere at mid- and high-latitudes is too weak. The problem was traced back to biases in the uplift of CH<sub>4</sub> over the source regions in eastern China and North America. In the tropics, the WC assimilation pointed to the possibility of biased CH<sub>4</sub> outflow from the African continent to the Atlantic in the mid-troposphere. The WC assimilation in this region would greatly benefit from glint observations over the ocean to provide additional constraints on the vertical structure of the model errors in the tropics. We also compared the WC assimilation at the 4° × 5° and 2° × 2.5° horizontal resolutions and found that the WC corrections to mitigate the model errors were significantly larger at 4° × 5° than at 2° × 2.5° resolution, indicating the presence of resolution-dependent model errors. Our results illustrate the potential utility of the WC 4D-Var approach for characterizing model errors. However, a major limitation of this approach is the need to better characterize the specified model error covariance in the assimilation scheme.</p>

We describe the use of ground-based Fourier transform (FTIR) solar absorption spectroscopy to measure vertical columns of tropospheric and stratospheric trace gases. We focus on measurements made at the University of Toronto Atmospheric Observatory and the Polar Environment Atmospheric Research Laboratory in the high Arctic, and introduce the new Canadian FTIR Observing Network.