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International audience; The ability of current global models to simulate the transport of CO 2 by mid-latitude, synopticscale weather systems (i.e., CO 2 weather) is important for inverse estimates of regional and global carbon budgets but remains unclear without comparisons to targeted measurements. Here, we evaluate ten models that participated in the Orbiting Carbon Observatory-2 model intercomparison project (OCO-2 MIP version 9) with intensive aircraft measurements collected from the Atmospheric Carbon Transport (ACT)-America mission. We quantify model-data differences in the spatial variability of CO 2 mole fractions, mean winds, and boundary layer depths in 27 mid-latitude cyclones spanning four seasons over the central and eastern United States. We find that the OCO-2 MIP models are able to simulate observed CO 2 frontal differences with varying degrees of success in summer and spring, and most underestimate frontal differences in winter and autumn. The models may underestimate the observed boundary layer-to-free troposphere CO 2 differences in spring and autumn due to model errors in boundary layer height. Attribution of the causes of model biases in other seasons remains elusive. Transport errors, prior fluxes, and/or inversion algorithms appear to be the primary cause of these biases since model performance is not highly sensitive to the CO 2 data used in the inversion. The metrics presented here provide new benchmarks regarding the ability of atmospheric inversion systems to reproduce the CO 2 structure of mid-latitude weather systems. Controlled experiments are needed to link these metrics more directly to the accuracy of regional or global flux estimates. Plain Language Summary Global flux estimate systems use CO 2 observations, atmospheric transport models, CO 2 flux models (emissions and absorption), and mathematical optimization methods to estimate biosphere-atmosphere CO 2 exchange. Accurate representation of atmospheric transport is important for a reliable optimization of fluxes in these systems. We use intensive aircraft measurements of wind speed, boundary layer height, and horizontal and vertical differences of CO 2 concentrations within 27 mid-latitude cyclones collected by the Atmospheric Carbon Transport (ACT)-America mission to evaluate the performance of ten global flux estimate systems from the Orbiting Carbon Observatory-2 model intercomparison project (OCO-2 MIP). We find the models can simulate observed horizontal CO 2 differences between the warm and cold parts of cyclones with different degrees of success in summer and spring, but often underestimate the observed cross-frontal and vertical differences in CO 2 in winter and autumn. The models may underestimate the CO 2 differences between the boundary layer and the free troposphere due to model errors in boundary layer height and surface fluxes. These weather-oriented CO 2 metrics provide benchmarks for testing simulations of the CO 2 structure within cyclones. Future efforts are needed to link these metrics more directly to the accuracy of CO 2 flux estimates. ZHANG ET AL.

Carbonyl sulfide (COS) is an atmospheric trace gas of interest for C cycle research because COS uptake by continental vegetation is strongly related to terrestrial gross primary productivity (GPP), the largest and most uncertain flux in atmospheric CO2 budgets. However, to use atmospheric COS as an additional tracer of GPP, an accurate quantification of COS exchange by soils is also needed. At present, the atmospheric COS budget is unbalanced globally, with total COS flux estimates from oxic and anoxic soils that vary between −409 and −89 GgS yr−1. This uncertainty hampers the use of atmospheric COS concentrations to constrain GPP estimates through atmospheric transport inversions. In this study we implemented a mechanistic soil COS model in the ORCHIDEE (Organising Carbon and Hydrology In Dynamic Ecosystems) land surface model to simulate COS fluxes in oxic and anoxic soils. Evaluation of the model against flux measurements at seven sites yields a mean root mean square deviation of 1.6 pmol m−2 s−1, instead of 2 pmol m−2 s−1 when using a previous empirical approach that links soil COS uptake to soil heterotrophic respiration. However, soil COS model evaluation is still limited by the scarcity of observation sites and long-term measurement periods, with all sites located in a latitudinal band between 39 and 62∘ N and no observations during wintertime in this study. The new model predicts that, globally and over the 2009–2016 period, oxic soils act as a net uptake of −126 GgS yr−1 and anoxic soils are a source of +96 GgS yr−1, leading to a global net soil sink of only −30 GgS yr−1, i.e. much smaller than previous estimates. The small magnitude of the soil fluxes suggests that the error in the COS budget is dominated by the much larger fluxes from plants, oceans, and industrial activities. The predicted spatial distribution of soil COS fluxes, with large emissions from oxic (up to 68.2 pmol COS m−2 s−1) and anoxic (up to 36.8 pmol COS m−2 s−1) soils in the tropics, especially in India and in the Sahel region, marginally improves the latitudinal gradient of atmospheric COS concentrations, after transport by the LMDZ (Laboratoire de Météorologie Dynamique) atmospheric transport model. The impact of different soil COS flux representations on the latitudinal gradient of the atmospheric COS concentrations is strongest in the Northern Hemisphere. We also implemented spatiotemporal variations in near-ground atmospheric COS concentrations in the modelling of biospheric COS fluxes, which helped reduce the imbalance of the atmospheric COS budget by lowering soil COS uptake by 10 % and plant COS uptake by 8 % globally (with a revised mean vegetation budget of −576 GgS yr−1 over 2009–2016). Sensitivity analyses highlighted the different parameters to which each soil COS flux model is the most responsive, selected in a parameter optimization framework. Having both vegetation and soil COS fluxes modelled within ORCHIDEE opens the way for using observed ecosystem COS fluxes and larger-scale atmospheric COS mixing ratios to improve the simulated GPP, through data assimilation techniques.

Land surface modellers need measurable proxies to constrain the quantity of carbon dioxide (CO2) assimilated by continental plants through photosynthesis, known as gross primary production (GPP). Carbonyl sulfide (COS), which is taken up by leaves through their stomates and then hydrolysed by photosynthetic enzymes, is a candidate GPP proxy. A former study with the ORCHIDEE land surface model used a fixed ratio of COS uptake to CO2 uptake normalised to respective ambient concentrations for each vegetation type (leaf relative uptake, LRU) to compute vegetation COS fluxes from GPP. The LRU approach is known to have limited accuracy since the LRU ratio changes with variables such as photosynthetically active radiation (PAR): while CO2 uptake slows under low light, COS uptake is not light limited. However, the LRU approach has been popular for COS–GPP proxy studies because of its ease of application and apparent low contribution to uncertainty for regional-scale applications. In this study we refined the COS–GPP relationship and implemented in ORCHIDEE a mechanistic model that describes COS uptake by continental vegetation. We compared the simulated COS fluxes against measured hourly COS fluxes at two sites and studied the model behaviour and links with environmental drivers. We performed simulations at a global scale, and we estimated the global COS uptake by vegetation to be −756 Gg S yr−1, in the middle range of former studies (−490 to −1335 Gg S yr−1). Based on monthly mean fluxes simulated by the mechanistic approach in ORCHIDEE, we derived new LRU values for the different vegetation types, ranging between 0.92 and 1.72, close to recently published averages for observed values of 1.21 for C4 and 1.68 for C3 plants. We transported the COS using the monthly vegetation COS fluxes derived from both the mechanistic and the LRU approaches, and we evaluated the simulated COS concentrations at NOAA sites. Although the mechanistic approach was more appropriate when comparing to high-temporal-resolution COS flux measurements, both approaches gave similar results when transporting with monthly COS fluxes and evaluating COS concentrations at stations. In our study, uncertainties between these two approaches are of secondary importance compared to the uncertainties in the COS global budget, which are currently a limiting factor to the potential of COS concentrations to constrain GPP simulated by land surface models on the global scale.

The quality of the representation of greenhouse gas (GHG) transport in atmospheric general circulation models (GCMs) drives the potential of inverse systems to retrieve GHG surface fluxes to a large extent. In this work, the transport of CO2 is evaluated in the latest version of the Laboratoire de Météorologie Dynamique (LMDz) GCM, developed for the Climate Model Intercomparison Project 6 (CMIP6) relative to the LMDz version developed for CMIP5. Several key changes have been implemented between the two versions, which include a more elaborate radiative scheme, new subgrid-scale parameterizations of convective and boundary layer processes and a refined vertical resolution. We performed a set of simulations of LMDz with different physical parameterizations, two different horizontal resolutions and different land surface schemes, in order to test the impact of those different configurations on the overall transport simulation. By modulating the intensity of vertical mixing, the physical parameterizations control the interhemispheric gradient and the amplitude of the seasonal cycle in the Northern Hemisphere, as emphasized by the comparison with observations at surface sites. However, the effect of the new parameterizations depends on the region considered, with a strong impact over South America (Brazil, Amazonian forest) but a smaller impact over Europe, East Asia and North America. A finer horizontal resolution reduces the representation errors at observation sites near emission hotspots or along the coastlines. In comparison, the sensitivities to the land surface model and to the increased vertical resolution are marginal.