Abstract

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 budgets 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 −104 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 land surface model to simulate COS fluxes in oxic and anoxic soils. Evaluation of the model against flux measurements at 7 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. 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 in the tropics 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, marginally improves the latitudinal gradient of atmospheric COS concentrations, after transport by the LMDZ 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 spatio-temporal variations of near-ground atmospheric COS concentrations in the modelling of biospheric COS fluxes, which helped reduce the imbalance of the atmospheric COS budget by lowering COS uptake by soils and vegetation globally (−10 % for soil, and −8 % for vegetation with a revised mean estimate of −576 GgS y−r1 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.

Highlights

  • Carbonyl sulfide (COS) has been proposed as a tracer for constraining the simulated Gross Primary Productivity (GPP) in Land Surface Models (LSMs) (Launois et al, 2015; Remaud et al, 2021; Campbell et al, 2008)

  • The empirical model mainly differs from the mechanistic model with a stronger seasonal amplitude of soil carbonyl sulfide (COS) fluxes (34% higher), except at the sites where a net COS production is found with the mechanistic model in summer (ES-LMA and IT-CRO)

  • The strong COS uptake in summer from the empirical model can be explained by the proportionality of soil COS uptake to simulated soil respiration, which increases with the high temperatures in summer

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Summary

Introduction

Carbonyl sulfide (COS) has been proposed as a tracer for constraining the simulated Gross Primary Productivity (GPP) in Land Surface Models (LSMs) (Launois et al, 2015; Remaud et al, 2021; Campbell et al, 2008). To infer GPP at the regional scale using COS observations, modelers can use measurements of ecosystem COS fluxes directly, or measurements of atmospheric COS concentrations combined with an atmospheric transport inversion model, provided all COS flux components are taken into account In both cases, net soil COS flux estimates are needed, as well as a functional relationship between GPP and COS uptake by foliage. With high temperature or radiation, soils were found to emit COS through thermal or photo degradation processes (Kitz et al, 2017, 2020; Whelan and Rhew, 2015; Whelan et al, 2016, 2018) Such COS emissions can be large in some conditions, they are usually neglected in current figures of the atmospheric COS budget. Ogée et al (2016) developed a mechanistic model including both COS uptake

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