Marine carbonyl sulfide (OCS) and carbon disulfide (CS&amp;lt;sub&amp;gt;2&amp;lt;/sub&amp;gt;): a compilation of measurements in seawater and the marine boundary layer

Lennartz, Sinikka T.; Marandino, Christa; Hobe, Marc von; Andreae, Meinrat O.; Aranami, Kazushi; Atlas, Elliot L.; Berkelhammer, Max; Bingemer, Heinz; Booge, Dennis; Cutter, Gregory A.; Cortés, Pau; Kremser, Stefanie; Law, Cliff S.; Marriner, Andrew; Simó, Rafel; Quack, Birgit; Uher, G; Xie, Huixiang; Xu, Xiangde

doi:10.5194/essd-12-591-2020

Cited by 42 publications

(54 citation statements)

References 52 publications

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“…Rate r 3 represents an exponential decay of 1.2 d for DMS (r 3 = 9.6 × 10 −6 s −1 ). COS photolysis frequencies are calculated based on a troposphere ultraviolet and visible (TUV) radiation model (Madronich et al, 2003). Based on monthly climatologies of ozone profiles and temperatures, monthly averaged photolysis frequencies are calculated on a 1 km grid spanning 0-120 km and on 180 latitude bands.…”

Section: Tm5-4dvar Inverse Modelling Systemmentioning

confidence: 99%

Inverse modelling of carbonyl sulfide: implementation, evaluation and implications for the global budget

Kooijmans

Cho

et al. 2021

Atmos. Chem. Phys.

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Abstract. Carbonyl sulfide (COS) has the potential to be used as a climate diagnostic due to its close coupling to the biospheric uptake of CO2 and its role in the formation of stratospheric aerosol. The current understanding of the COS budget, however, lacks COS sources, which have previously been allocated to the tropical ocean. This paper presents a first attempt at global inverse modelling of COS within the 4-dimensional variational data-assimilation system of the TM5 chemistry transport model (TM5-4DVAR) and a comparison of the results with various COS observations. We focus on the global COS budget, including COS production from its precursors carbon disulfide (CS2) and dimethyl sulfide (DMS). To this end, we implemented COS uptake by soil and vegetation from an updated biosphere model (Simple Biosphere Model – SiB4). In the calculation of these fluxes, a fixed atmospheric mole fraction of 500 pmol mol−1 was assumed. We also used new inventories for anthropogenic and biomass burning emissions. The model framework is capable of closing the COS budget by optimizing for missing emissions using NOAA observations in the period 2000–2012. The addition of 432 Gg a−1 (as S equivalents) of COS is required to obtain a good fit with NOAA observations. This missing source shows few year-to-year variations but considerable seasonal variations. We found that the missing sources are likely located in the tropical regions, and an overestimated biospheric sink in the tropics cannot be ruled out due to missing observations in the tropical continental boundary layer. Moreover, high latitudes in the Northern Hemisphere require extra COS uptake or reduced emissions. HIPPO (HIAPER Pole-to-Pole Observations) aircraft observations, NOAA airborne profiles from an ongoing monitoring programme and several satellite data sources are used to evaluate the optimized model results. This evaluation indicates that COS mole fractions in the free troposphere remain underestimated after optimization. Assimilation of HIPPO observations slightly improves this model bias, which implies that additional observations are urgently required to constrain sources and sinks of COS. We finally find that the biosphere flux dependency on the surface COS mole fraction (which was not accounted for in this study) may substantially lower the fluxes of the SiB4 biosphere model over strong-uptake regions. Using COS mole fractions from our inversion, the prior biosphere flux reduces from 1053 to 851 Gg a−1, which is closer to 738 Gg a−1 as was found by Berry et al. (2013). In planned further studies we will implement this biosphere dependency and additionally assimilate satellite data with the aim of better separating the role of the oceans and the biosphere in the global COS budget.

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Section: Tm5-4dvar Inverse Modelling Systemmentioning

confidence: 99%

Inverse modelling of carbonyl sulfide: implementation, evaluation and implications for the global budget

Kooijmans

Cho

et al. 2021

Atmos. Chem. Phys.

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“…480 ppt at land-based time series stations (Montzka et al, 2007) and ca. 550 ppt in the marine boundary layer (Lennartz et al, 2020b). The sources and sinks of atmospheric OCS are important in two contexts: first, OCS is transported to the stratosphere due to its long tropospheric lifetime of 1.5 to 3 years (Montzka et al, 2007), where it is a major precursor of sulphate aerosols (Brühl et al, 2012;Kremser et al, 2016;Turco et al, 1980).…”

Section: Introductionmentioning

confidence: 99%

Monthly resolved modelled oceanic emissions of carbonyl sulphide and carbon disulphide for the period 2000–2019

Lennartz

Gauss

Hobe³

et al. 2021

Earth Syst. Sci. Data

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Abstract. Carbonyl sulphide (OCS) is the most abundant, long-lived sulphur gas in the atmosphere and a major supplier of sulphur to the stratospheric sulphate aerosol layer. The short-lived gas carbon disulphide (CS2) is oxidized to OCS and constitutes a major indirect source to the atmospheric OCS budget. The atmospheric budget of OCS is not well constrained due to a large missing source needed to compensate for substantial evidence that was provided for significantly higher sinks. Oceanic emissions are associated with major uncertainties. Here we provide a first, monthly resolved ocean emission inventory of both gases for the period 2000–2019 (available at https://doi.org/10.5281/zenodo.4297010) (Lennartz et al., 2020a). Emissions are calculated with a numerical box model (2.8∘×2.8∘ resolution at the Equator, T42 grid) for the oceanic surface mixed layer, driven by ERA5 data from ECMWF and chromophoric dissolved organic matter (CDOM) from Aqua MODIS. We find that interannual variability in OCS emissions is smaller than seasonal variability and is mainly driven by variations in CDOM, which influences both photochemical and light-independent production. A comparison with a global database of more than 2500 measurements reveals overall good agreement. Emissions of CS2 constitute a larger sulphur source to the atmosphere than OCS and equally show interannual variability connected to variability in CDOM. The emission estimate of CS2 is associated with higher uncertainties as process understanding of the marine cycling of CS2 is incomplete. We encourage the use of the data provided here as input for atmospheric modelling studies to further assess the atmospheric OCS budget and the role of OCS in climate.

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“…The Ozone Monitoring Instrument (OMI) is a key instrument onboard NASA's Aura satellite. OMI is a nadir-viewing, wide-field-imaging spectrometer that measures backscattered radiances at a spectral resolution of 0.42-0.63 nm (Levelt et al, 2006). Its wide field-of-view of 114° with a swath width of 2600 km yields daily global coverage with a spatial resolution of 13 km×24 km (Liu et al, 2010).…”

Section: Ozone and Pollutants From Omi And Tropomimentioning

confidence: 99%

Atmospheric gas-phase composition over the Indian Ocean

Tegtmeier

Marandino

Jia

et al. 2020

Preprint

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Abstract. The Indian Ocean is coupled to atmospheric dynamics, transport and chemical composition via several unique mechanisms, such as the seasonally varying monsoon circulation. During the winter monsoon season, high pollution levels are regularly observed over the entire northern Indian Ocean, while during the summer monsoon, clean air dominates the atmospheric composition, leading to distinct chemical regimes. The changing atmospheric composition over the Indian Ocean can interact with oceanic biogeochemical cycles and impact marine ecosystems, resulting in potential climate feedbacks. Here, we review current progress in detecting and understanding atmospheric gas-phase composition over the Indian Ocean and its local and global impacts. The review takes into account results from recent Indian Ocean ship campaigns, satellite measurements, station data and information on continental and oceanic trace gas emissions. The distribution of all major pollutants and greenhouse gases shows pronounced differences between the landmass source regions and the Indian Ocean with strong gradients over the coastal areas. Surface pollution and ozone are highest during the winter monsoon over the Bay of Bengal and the Arabian Sea coastal waters due to air mass advection from the Indo-Gangetic Plain and continental outflow from Southeast Asia. We observe, however, that unusual types of wind patterns can lead to pronounced deviations of the typical trace gas distributions. For example, the ozone distribution maxima shift to different regions under different wind scenarios. The distribution of greenhouse gases over the Indian Ocean shows many similarities when compared to the pollution fields, but also some differences of the latitudinal and seasonal variations resulting from their long lifetimes and biogenic sources. Mixing ratios of greenhouse gases such as methane show positive trends over the Indian Ocean, but long-term changes of pollution and ozone, and in particular how they are driven by changing emissions and transport patterns, require further investigation in the future. Although we know that changing atmospheric composition and perturbations within the Indian Ocean affect each other, the impacts of atmospheric pollution on oceanic biogeochemistry and trace gas cycling is severely understudied. We highlight potential mechanisms, future research topics and observational requirements that need to be explored in order to fully understand interactions and feedbacks between the ocean and atmosphere in the Indian Ocean region.

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Marine carbonyl sulfide (OCS) and carbon disulfide (CS<sub>2</sub>): a compilation of measurements in seawater and the marine boundary layer

Cited by 42 publications

References 52 publications

Inverse modelling of carbonyl sulfide: implementation, evaluation and implications for the global budget

Inverse modelling of carbonyl sulfide: implementation, evaluation and implications for the global budget

Monthly resolved modelled oceanic emissions of carbonyl sulphide and carbon disulphide for the period 2000–2019

Atmospheric gas-phase composition over the Indian Ocean

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