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We present a comparison of atmospheric transport models that simulate carbonyl sulfide (COS). This is part II of the ongoing Atmospheric Transport Model Inter‐comparison Project (TransCom–COS). Differently from part I, we focus on seven model intercomparison by transporting two recent COS inversions of NOAA surface data within TM5‐4DVAR and LMDz models. The main goals of TransCom‐COS part II are (a) to compare the COS simulations using the two sets of optimized fluxes with simulations that use a control scenario (part I) and (b) to evaluate the simulated tropospheric COS abundance with aircraft‐based observations from various sources. The output of the seven transport models are grouped in terms of their vertical mixing strength: strong and weak mixing. The results indicate that all transport models capture the meridional distribution of COS at the surface well. Model simulations generally match the aircraft campaigns HIAPER Pole‐To‐Pole Observations (HIPPO) and Atmospheric Tomography Mission (ATom). Comparisons to HIPPO and ATom demonstrate a gap between observed and modeled COS over the Pacific Ocean at 0–40°N, indicating a potential missing source in the free troposphere. The effects of seasonal continental COS uptake by the biosphere, observed on HIPPO and ATom over oceans, is well reproduced by the simulations. We found that the strength of the vertical mixing within the column as represented in the various atmospheric transport models explains much of the model to model differences. We also found that weak‐mixing models transporting the optimized flux derived from the strong‐mixing TM5 model show a too strong seasonal cycle at high latitudes. Plain Language Summary: Carbonyl sulfide (COS) is a significant sulfur‐containing trace gas in the atmosphere, which makes it important for studying climate change. One of the reasons it is worth investigating is because plants take up COS in a similar way as CO2 during photosynthesis. However, the atmospheric sources and sinks of COS are not well understood. To address this knowledge gap, we evaluated the state‐of‐the‐art optimized surface COS fluxes from the inverse models TM5‐4DVAR and LMDz, and then seven atmospheric transport models were used to simulate COS mole fractions by transporting the optimized fluxes under the TransCom‐COS protocol. The results showed good agreement between the simulated COS and COS observations on independent platforms. The study also revealed that COS drawdown due to plant uptake can be observed over Pacific and Atlantic Oceans. However, discrepancies between the model simulations and observations were mainly found in free troposphere, emphasizing the need for further investigation into COS chemistry and model transport differences. These findings provide important reference for further investigation of COS global distribution and budget analysis. Key Points: Simulations in seven models propagating optimized carbonyl sulfide (COS) fluxes derived from two inversions agree with independent observationsSimulated and observed COS drawdowns are captured in boundary layer over the Pacific and Atlantic Oceans due to plant uptake over landsWeak vertical mixing models using fluxes optimized from the fast‐mixing TM5 model overestimate the COS seasonal amplitude at high latitudes [ABSTRACT FROM AUTHOR]

Gross primary production (GPP) by boreal forests is highly sensitive to environmental changes. However, GPP simulated by land surface models (LSMs) remains highly uncertain due to the lack of direct photosynthesis observations at large scales. Carbonyl sulfide (COS) has emerged as a promising proxy to improve the representation of GPP in LSMs. Because COS is absorbed by vegetation following the same diffusion pathway as CO2 during photosynthesis and not emitted back to the atmosphere, incorporating a mechanistic representation of vegetation COS uptake in LSMs allows using COS observations to refine GPP representation. Here, we perform ecosystem COS flux and GPP data assimilations to constrain the COS‐ and GPP‐related parameters in the ORCHIDEE LSM for boreal evergreen needleleaf forests (BorENF). Assimilating ecosystem COS fluxes at Hyytiälä forest increases the simulated net ecosystem COS uptake by 14%. This increase largely results from changes in the internal conductance to COS, highlighting the need to improve the representation of COS internal diffusion and consumption. Moreover, joint assimilation of ecosystem COS flux and GPP at Hyytiälä improves the simulated latent heat flux, contrary to the GPP‐only data assimilation, which fails to do so. Finally, we scaled this assimilation framework up to the boreal region and find that the joint assimilation of COS at Hyytiälä and GPP fluxes at 10 BorENF sites increases the modeled vegetation COS uptake up to 18%, but not GPP. Therefore, this study encourages the use of COS flux observations to inform GPP and latent heat flux representations in LSMs. Plain Language Summary: Carbon uptake by boreal forests is highly sensitive to environmental changes. There is large uncertainty about how much carbon dioxide (CO2) boreal forests absorb through photosynthesis, as represented by land surface models. Carbonyl sulfide (COS), a trace gas that tracks photosynthesis, can help improve the representation of simulated plant CO2 uptake because COS and CO2 share a common pathway during leaf uptake. Using a mechanistic model of biospheric COS processes implemented in the ORCHIDEE land surface model, we assimilated ecosystem COS flux and plant CO2 uptake measured at Hyytiälä boreal forest. We find that this joint assimilation improves the simulated plant CO2 uptake, as well as transpiration because of the strong link between COS, CO2 and H2O fluxes through stomatal diffusion. Scaling up this assimilation framework to evergreen needleleaf boreal forests, we find that assimilating ecosystem COS flux and plant CO2 uptake data increases the vegetation COS uptake for this biome, but not plant CO2 uptake. Our results imply that COS has the potential to constrain both plant carbon uptake and transpiration in land surface models, which should be further investigated, especially during drought events. Key Points: Jointly assimilating ecosystem carbonyl sulfide (COS) flux and gross primary production data improves both simulated plant carbon uptake and transpirationAssimilating ecosystem COS flux does not increase gross primary production (GPP) over boreal evergreen needleleaf forests, in contrast with previous inversion studiesCOS flux observations help to identify misrepresentation of the sensitivity of GPP to droughts in models [ABSTRACT FROM AUTHOR]

We present a comparison of atmospheric transport model (ATM) simulations for carbonyl sulfide (COS), within the framework of the atmospheric tracer transport model intercomparison project "TransCom‐COS." Seven ATMs participated in the experiment and provided simulations of COS mixing ratios over the years 2010–2018, using state‐of‐the‐art surface fluxes for various components of the COS budget: biospheric sink, oceanic source, sources from fire and industry. The main goal of TransCom‐COS is to investigate the impact of the transport uncertainty and emission distribution in simulating the spatio‐temporal variability of tropospheric COS mixing ratios. A control case with seasonal surface fluxes of COS was constructed. The results indicate that the COS mixing ratios are underestimated by at least 50 parts per trillion (ppt) in the tropics, pointing to a missing tropical source. In summer, the mixing ratios are overestimated by at least 50 ppt above 40°N, pointing to a likely missing sink in the high northern latitudes. Regarding the latitudinal profile, the model spread is greater than 60 ppt above 40°N in boreal summer. Regarding the seasonal amplitude, the model spread reaches 50 ppt at 6 out of 15 sites, compared to an observed seasonal amplitude of 100 ppt. All models simulated a too late minimum by at least 2–3 months at two high northern‐latitude sites, likely owing to errors in the seasonal cycle in the ocean emissions. This study highlighted the shortcomings in the COS global budget that need to be resolved before using COS as a photosynthesis tracer. Plain Language Summary: In this study, we evaluate the state‐of‐the‐art fluxes for various components of the carbonyl sulfide (COS) budget: biospheric sink, oceanic source, sources from fire and industry. A control case with seasonal surface fluxes of COS was constructed. Seven atmospheric transport models provided simulations of COS mixing ratios. Then, the simulated mixing ratios were evaluated against atmospheric measurements at several surface sites. Results show that all models fail to capture the observed latitudinal distribution and that the model spread is small compared to the model‐observation mismatch. In summer, the overestimated mixing ratios above 40°N point to a likely missing sink in the high northern latitudes. The underestimated mixing ratios in the tropics point to a missing tropical source. This study highlighted the shortcomings in the COS global budget that need to be resolved before using COS as a photosynthesis tracer. Key Points: The model‐observation mismatch suggests there is a missing source in the tropics and a missing sink in the high northern latitude in summerAt northern latitude sites, the model spread in seasonal amplitude reaches 50 ppt compared to a mean seasonal amplitude of about 100 pptThe diurnal rectifier effect is small, decreasing the seasonal amplitude by up to 20% at continental sites [ABSTRACT FROM AUTHOR]

The ability of global transport models to go up in resolution becomes discriminating for greenhouse gas atmospheric inversions. This paper describes the porting on Graphics Processing Units of the global transport model currently used in the European operational Copernicus Atmosphere Monitoring Service (CAMS) for CO2 and N2O inversions. It represents an important milestone to achieve sub‐degree resolution. The code includes not only the direct model but also its tangent‐linear and its adjoint versions which are needed in variational inversions. Tests were carried out for CO2 at a resolution of 2.50° in longitude, 1.27° in latitude and 79 layers in the vertical, corresponding to 1,626,768 3D cells, 4.5 times more than the current standard resolution of the model used in the CAMS reanalyzes. A month's worth of computation of the tangent‐linear and of the adjoint versions now takes 2.5 min, including 50 s for reading meteorological data. Plain Language Summary: Atmospheric transport models are intensively used to infer global greenhouse gas emissions and removals, from atmospheric measurements: a single global analysis involves repeated and long transport simulations. This intensive use has limited the spatial resolution of such analyses despite an increasing need for national greenhouse gas budgets, despite an increasing number of corresponding space‐based observations at kilometer resolution, and despite an increasing number of high‐quality surface measurements made in sites marked by strong local influences. For the global transport model currently used in the European operational atmosphere monitoring service, our objective within the next 5 years is to make it reach a resolution of about 50 km over the whole globe. This paper describes an important milestone in this direction with the porting of this transport model on hardware components initially developed for video display but now used for high performance computing. Tests were carried out at a resolution of 2.50° in longitude, 1.27° in latitude and 79 layers in the vertical, corresponding to 4.5 times more 3D cells than the current standard resolution of the model. The direct model itself now takes less time than reading the input meteorological data. Key Points: The workload in a Eulerian transport model on a longitude‐latitude grid can be embarrassingly parallel enough to run efficiently on a Graphics Processing UnitThe transport model of the Laboratoire de Météorologie Dynamique was run in a new grid of 1,626,768 3D cellsThe calculation time in the direct version of the model is now less than the time to read the input meteorological data [ABSTRACT FROM AUTHOR]

The ability of current global models to simulate the transport of CO2 by mid‐latitude, synoptic‐scale weather systems (i.e., CO2 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 CO2 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 CO2 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 CO2 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 CO2 data used in the inversion. The metrics presented here provide new benchmarks regarding the ability of atmospheric inversion systems to reproduce the CO2 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 CO2 observations, atmospheric transport models, CO2 flux models (emissions and absorption), and mathematical optimization methods to estimate biosphere‐atmosphere CO2 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 CO2 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 CO2 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 CO2 in winter and autumn. The models may underestimate the CO2 differences between the boundary layer and the free troposphere due to model errors in boundary layer height and surface fluxes. These weather‐oriented CO2 metrics provide benchmarks for testing simulations of the CO2 structure within cyclones. Future efforts are needed to link these metrics more directly to the accuracy of CO2 flux estimates. Key Points: Global inversion systems are able to simulate observed CO2 frontal differences but with varying degrees of successMost global inversion systems underestimate dormant‐season frontal and vertical CO2 differencesInversion systems appear to explain more of the model‐data differences in CO2 weather metrics than CO2 data sources [ABSTRACT FROM AUTHOR]