- NSF-PAR ID:
- 10311395
- Author(s) / Creator(s):
- ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; more »
- Date Published:
- Journal Name:
- Biogeosciences
- Volume:
- 18
- Issue:
- 24
- ISSN:
- 1726-4189
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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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.more » « less
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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.
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Abstract. Ground-level ozone (O3) is a major air pollutant that adversely affects human health and ecosystem productivity. Removal of troposphericO3 by plant stomatal uptake can in turn cause damage to plant tissues with ramifications for ecosystem and crop health. In manyatmospheric and land surface models, the functionality of stomata opening is represented by a bulk stomatal conductance, which is oftensemi-empirically parameterized and highly fitted to historical observations. A lack of mechanistic linkage to ecophysiological processes such asphotosynthesis may render models inadequate to represent plant-mediated responses of atmospheric chemistry to long-term changes in CO2,climate, and short-lived air pollutant concentrations. A new ecophysiology module was thus developed to mechanistically simulate land−atmosphereexchange of important gas species in GEOS-Chem, a chemical transport model widely used in atmospheric chemistry studies. The implementation not onlyallows for dry deposition to be coupled with plant ecophysiology but also enables plant and crop productivity and functions to respond dynamically toatmospheric chemical changes. We conduct simulations to evaluate the effects of the ecophysiology module on simulated dry deposition velocity andconcentration of surface O3 against an observation-derived dataset known as SynFlux. Our estimated stomatal conductance and dry depositionvelocity of O3 are close to SynFlux with root-mean-squared errors (RMSEs) below 0.3 cm s−1 across different plant functionaltypes (PFTs), despite an overall positive bias in surface O3 concentration (by up to 16 ppbv). Representing ecophysiology wasfound to reduce the simulated biases in deposition fluxes from the prior model but worsen the positive biases in simulated O3concentrations. The increase in positive concentration biases is mostly attributable to the ecophysiology-based stomatal conductance being generallysmaller (and closer to SynFlux values) than that estimated by the prior semi-empirical formulation, calling for further improvements in non-stomataldepositional and non-depositional processes relevant for O3 simulations. The estimated global O3 deposition flux is864 Tg O3 yr−1 with GEOS-Chem, and the new module decreases this estimate by 92 Tg O3 yr−1. Estimated global grossprimary production (GPP) without O3 damage is 119 Pg C yr−1. O3-induced reduction in GPP is 4.2 Pg C yr−1(3.5 %). An elevated CO2 scenario (580 ppm) yields higher global GPP (+16.8 %) and lower global O3depositional sink (−3.3 %). Global isoprene emission simulated with a photosynthesis-based scheme is 317.9 Tg C yr−1, which is31.2 Tg C yr−1 (−8.9 %) less than that calculated using the MEGAN(Model of Emissions of Gases and Aerosols from Nature) emission algorithm. This new model development dynamicallyrepresents the two-way interactions between vegetation and air pollutants and thus provides a unique capability in evaluating vegetation-mediatedprocesses and feedbacks that can shape atmospheric chemistry and air quality, as well as pollutant impacts on vegetation health, especially for anytimescales shorter than the multidecadal timescale.more » « less
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null (Ed.)The ocean is a reservoir for CFC-11, a major ozone-depleting chemical. Anthropogenic production of CFC-11 dramatically decreased in the 1990s under the Montreal Protocol, which stipulated a global phase out of production by 2010. However, studies raise questions about current overall emission levels and indicate unexpected increases of CFC-11 emissions of about 10 Gg ⋅ yr −1 after 2013 (based upon measured atmospheric concentrations and an assumed atmospheric lifetime). These findings heighten the need to understand processes that could affect the CFC-11 lifetime, including ocean fluxes. We evaluate how ocean uptake and release through 2300 affects CFC-11 lifetimes, emission estimates, and the long-term return of CFC-11 from the ocean reservoir. We show that ocean uptake yields a shorter total lifetime and larger inferred emission of atmospheric CFC-11 from 1930 to 2075 compared to estimates using only atmospheric processes. Ocean flux changes over time result in small but not completely negligible effects on the calculated unexpected emissions change (decreasing it by 0.4 ± 0.3 Gg ⋅ yr −1 ). Moreover, it is expected that the ocean will eventually become a source of CFC-11, increasing its total lifetime thereafter. Ocean outgassing should produce detectable increases in global atmospheric CFC-11 abundances by the mid-2100s, with emission of around 0.5 Gg ⋅ yr −1 ; this should not be confused with illicit production at that time. An illustrative model projection suggests that climate change is expected to make the ocean a weaker reservoir for CFC-11, advancing the detectable change in the global atmospheric mixing ratio by about 5 yr.more » « less
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null (Ed.)Robust estimates for the rates and trends in terrestrial gross primary production (GPP; plant CO 2 uptake) are needed. Carbonyl sulfide (COS) is the major long-lived sulfur-bearing gas in the atmosphere and a promising proxy for GPP. Large uncertainties in estimating the relative magnitude of the COS sources and sinks limit this approach. Sulfur isotope measurements ( 34 S/ 32 S; δ 34 S) have been suggested as a useful tool to constrain COS sources. Yet such measurements are currently scarce for the atmosphere and absent for the marine source and the plant sink, which are two main fluxes. Here we present sulfur isotopes measurements of marine and atmospheric COS, and of plant-uptake fractionation experiments. These measurements resulted in a complete data-based tropospheric COS isotopic mass balance, which allows improved partition of the sources. We found an isotopic (δ 34 S ± SE) value of 13.9 ± 0.1‰ for the troposphere, with an isotopic seasonal cycle driven by plant uptake. This seasonality agrees with a fractionation of −1.9 ± 0.3‰ which we measured in plant-chamber experiments. Air samples with strong anthropogenic influence indicated an anthropogenic COS isotopic value of 8 ± 1‰. Samples of seawater-equilibrated-air indicate that the marine COS source has an isotopic value of 14.7 ± 1‰. Using our data-based mass balance, we constrained the relative contribution of the two main tropospheric COS sources resulting in 40 ± 17% for the anthropogenic source and 60 ± 20% for the oceanic source. This constraint is important for a better understanding of the global COS budget and its improved use for GPP determination.more » « less