Sources and sinks of carbonyl sulfide inferred from tower and mobile atmospheric observations in the Netherlands

Carbonyl sulfide (COS) is a promising tracer for the estimation of terrestrial ecosystem gross primary production (GPP). However, understanding its non-GPP-related sources and sinks, e.g., anthropogenic sources and soil sources and sinks, is also critical to the success of the approach. Here we infer the regional sources and sinks of COS using continuous in situ mole fraction profile measurements of COS along the 60m tall Lutjewad tower (1ma.s.l.; 53 degrees 24' N, 6 degrees 21' E) in the Netherlands. To identify potential sources that caused the observed enhancements of COS mole fractions at Lutjewad, both discrete flask samples and in situ measurements in the province of Groningen were made from a mobile van using a quantum cascade laser spectrometer (QCLS). We also simulated the COS mole fractions at Lutjewad using the Stochastic Time-Inverted Lagrangian Transport (STILT) model combined with emission inventories and plant uptake fluxes. We determined the nighttime COS fluxes to be -3.0 +/- 2.6 pmolm(-2) s(-1) using the radon-tracer correlation approach and Lutjewad observations. Furthermore, we identified and quantified several COS sources, including biodigesters, sugar production facilities and silicon carbide production facilities in the province of Groningen. Moreover, the simulation results show that the observed COS enhancements can be partially explained by known industrial sources of COS and CS2, in particular from the Ruhr Valley (51.5 degrees N, 7.2 degrees E) and Antwerp (51.2 degrees N, 4.4 degrees E) areas. The contribution of likely missing anthropogenic sources of COS and CS2 in the inventory may be significant. The impact of the identified sources in the province of Groningen is estimated to be negligible in terms of the observed COS enhancements. However, in specific conditions, these sources may influence the measurements in Lutjewad. These results are valuable for improving our understanding of the sources and sinks of COS, contributing to the use of COS as a tracer for GPP.Peer reviewe