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Abstract. Carbonyl sulfide (COS) is the most abundant sulfur gas in the atmosphere with links to terrestrial and oceanic productivity. We measured COS in ice core air from an intermediate-depth ice core from the South Pole using both dry and wet extraction methods, recovering a 52 500-year record. We find evidence for COS production in the firn, altering the atmospheric signal preserved in the ice core. Mean sea salt aerosol concentrations from the same depth are a good proxy for the COS production, which disproportionately impacts the measurements from glacial period ice with high sea salt aerosol concentrations. The COS measurements are corrected using sea salt sodium (ssNa) as a proxy for the excess COS resulting from the production. The ssNa-corrected COS record displays substantially less COS in the glacial period atmosphere than the Holocene and a 2 to 4-fold COS rise during the deglaciation synchronous with the associated climate signal. The deglacial COS rise was primarily source driven. Oceanic emissions in the form of COS, carbon disulfide (CS2), and dimethylsulfide (DMS) are collectively the largest natural source of atmospheric COS. A large increase in ocean COS emissions during the deglaciation suggests enhancements in emissions of ocean sulfur gases via processes that involve ocean productivity, although we cannot quantify individual contributions from each gas. 

Abstract Where does the carbon released by burning fossil fuels go? Currently, ocean and land systems remove about half of the CO 2 emitted by human activities; the remainder stays in the atmosphere. These removal processes are sensitive to feedbacks in the energy, carbon, and water cycles that will change in the future. Observing how much carbon is taken up on land through photosynthesis is complicated because carbon is simultaneously respired by plants, animals, and microbes. Global observations from satellites and air samples suggest that natural ecosystems take up about as much CO 2 as they emit. To match the data, our land models generate imaginary Earths where carbon uptake and respiration are roughly balanced, but the absolute quantities of carbon being exchanged vary widely. Getting the magnitude of the flux is essential to make sure our models are capturing the right pattern for the right reasons. Combining two cutting-edge tools, carbonyl sulfide (OCS) and solar-induced fluorescence (SIF), will help develop an independent answer of how much carbon is being taken up by global ecosystems. Photosynthesis requires CO 2 , light, and water. OCS provides a spatially and temporally integrated picture of the “front door” of photosynthesis, proportional to CO 2 uptake and water loss through plant stomata. SIF provides a high-resolution snapshot of the “side door,” scaling with the light captured by leaves. These two independent pieces of information help us understand plant water and carbon exchange. A coordinated effort to generate SIF and OCS data through satellite, airborne, and ground observations will improve our process-based models to predict how these cycles will change in the future. 

Abstract. Land surface modellers need measurable proxies toconstrain the quantity of carbon dioxide (CO2) assimilated bycontinental plants through photosynthesis, known as gross primary production(GPP). Carbonyl sulfide (COS), which is taken up by leaves through theirstomates and then hydrolysed by photosynthetic enzymes, is a candidate GPPproxy. A former study with the ORCHIDEE land surface model used a fixedratio of COS uptake to CO2 uptake normalised to respective ambientconcentrations for each vegetation type (leaf relative uptake, LRU) tocompute vegetation COS fluxes from GPP. The LRU approach is known to havelimited accuracy since the LRU ratio changes with variables such asphotosynthetically active radiation (PAR): while CO2 uptake slows underlow light, COS uptake is not light limited. However, the LRU approach hasbeen popular for COS–GPP proxy studies because of its ease of applicationand apparent low contribution to uncertainty for regional-scaleapplications. In this study we refined the COS–GPP relationship andimplemented in ORCHIDEE a mechanistic model that describes COS uptake bycontinental vegetation. We compared the simulated COS fluxes againstmeasured hourly COS fluxes at two sites and studied the model behaviour andlinks 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). Basedon monthly mean fluxes simulated by the mechanistic approach in ORCHIDEE, wederived new LRU values for the different vegetation types, ranging between0.92 and 1.72, close to recently published averages for observed values of1.21 for C4 and 1.68 for C3 plants. We transported the COS using the monthlyvegetation COS fluxes derived from both the mechanistic and the LRUapproaches, and we evaluated the simulated COS concentrations at NOAA sites.Although the mechanistic approach was more appropriate when comparing tohigh-temporal-resolution COS flux measurements, both approaches gave similarresults when transporting with monthly COS fluxes and evaluating COSconcentrations at stations. In our study, uncertainties between these twoapproaches are of secondary importance compared to the uncertainties in theCOS global budget, which are currently a limiting factor to the potential ofCOS concentrations to constrain GPP simulated by land surface models on theglobal scale. 

Abstract. The uptake of carbonyl sulfide (COS) by terrestrial plants is linked tophotosynthetic uptake of CO2 as these gases partly share the sameuptake pathway. Applying COS as a photosynthesis tracer in models requires anaccurate representation of biosphere COS fluxes, but these models have notbeen extensively evaluated against field observations of COS fluxes. In thispaper, the COS flux as simulated by the Simple Biosphere Model, version 4(SiB4), is updated with the latest mechanistic insights and evaluated with siteobservations from different biomes: one evergreen needleleaf forest, twodeciduous broadleaf forests, three grasslands, and two crop fields spread overEurope and North America. We improved SiB4 in several ways to improve itsrepresentation of COS. To account for the effect of atmospheric COS molefractions on COS biosphere uptake, we replaced the fixed atmospheric COS molefraction boundary condition originally used in SiB4 with spatially andtemporally varying COS mole fraction fields. Seasonal amplitudes of COS molefractions are ∼50–200 ppt at the investigated sites with aminimum mole fraction in the late growing season. Incorporating seasonalvariability into the model reduces COS uptake rates in the late growingseason, allowing better agreement with observations. We also replaced theempirical soil COS uptake model in SiB4 with a mechanistic model thatrepresents both uptake and production of COS in soils, which improves thematch with observations over agricultural fields and fertilized grasslandsoils. The improved version of SiB4 was capable of simulating the diurnal andseasonal variation in COS fluxes in the boreal, temperate, and Mediterraneanregion. Nonetheless, the daytime vegetation COS flux is underestimated onaverage by 8±27 %, albeit with large variability across sites. On aglobal scale, our model modifications decreased the modeled COS terrestrialbiosphere sink from 922 Gg S yr−1 in the original SiB4 to753 Gg S yr−1 in the updated version. The largest decrease influxes was driven by lower atmospheric COS mole fractions over regions withhigh productivity, which highlights the importance of accounting forvariations in atmospheric COS mole fractions. The change to a different soilmodel, on the other hand, had a relatively small effect on the globalbiosphere COS sink. The secondary role of the modeled soil component in theglobal COS budget supports the use of COS as a global photosynthesis tracer. Amore accurate representation of COS uptake in SiB4 should allow for improvedapplication of atmospheric COS as a tracer of local- to global-scaleterrestrial photosynthesis. 

Abstract Differentiating the contributions of photosynthesis and respiration to the global carbon cycle is critical for improving predictive climate models. Carbonic anhydrase (CA) activity in leaves is responsible for the largest biosphere-atmosphere trace gas fluxes of carbonyl sulfide (COS) and the oxygen-18 isotopologue of carbon dioxide (CO18O) that both reflect gross photosynthetic rates. However, CA activity also occurs in soils and will be a source of uncertainty in the use of COS and CO18O as carbon cycle tracers until process-based constraints are improved. In this study, we measured COS and CO18O exchange rates and estimated the corresponding CA activity in soils from a range of biomes and land use types. Soil CA activity was not uniform for COS and CO2, and patterns of divergence were related to microbial community composition and CA gene expression patterns. In some cases, the same microbial taxa and CA classes catalyzed both COS and CO2 reactions in soil, but in other cases the specificity towards the two substrates differed markedly. CA activity for COS was related to fungal taxa and β-D-CA expression, whereas CA activity for CO2 was related to algal and bacterial taxa and α-CA expression. This study integrates gas exchange measurements, enzyme activity models, and characterization of soil taxonomic and genetic diversity to build connections between CA activity and the soil microbiome. Importantly, our results identify kinetic parameters to represent soil CA activity during application of COS and CO18O as carbon cycle tracers. 

Abstract. For the past decade, observations of carbonyl sulfide (OCS or COS) have been investigated as a proxy for carbon uptake by plants. OCS is destroyed by enzymes that interact with CO₂ during photosynthesis, namely carbonic anhydrase (CA) and RuBisCO, where CA is the more important one. The majority of sources of OCS to the atmosphere are geographically separated from this large plant sink, whereas the sources and sinks of CO₂ are co-located in ecosystems. The drawdown of OCS can therefore be related to the uptake of CO₂ without the added complication of co-located emissions comparable in magnitude. Here we review the state of our understanding of the global OCS cycle and its applications to ecosystem carbon cycle science. OCS uptake is correlated well to plant carbon uptake, especially at the regional scale. OCS can be used in conjunction with other independent measures of ecosystem function, like solar-induced fluorescence and carbon and water isotope studies. More work needs to be done to generate global coverage for OCS observations and to link this powerful atmospheric tracer to systems where fundamental questions concerning the carbon and water cycle remain.