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An estimated 1700 Pg of carbon is frozen in the Arctic permafrost and the fate of this carbon is unclear because of the complex interaction of biophysical, ecological and biogeochemical processes that govern the Arctic carbon budget. Two key processes determining the region’s long-term carbon budget are: (a) carbon uptake through increased plant growth, and (b) carbon release through increased heterotrophic respiration (HR) due to warmer soils. Previous predictions for how these two opposing carbon fluxes may change in the future have varied greatly, indicating that improved understanding of these processes and their feedbacks is critical for advancing our predictive ability for the fate of Arctic peatlands. In this study, we implement and analyze a vertically-resolved model of peatland soil carbon into a cohort-based terrestrial biosphere model to improve our understanding of how on-going changes in climate are altering the Arctic carbon budget. A key feature of the formulation is that accumulation of peat within the soil column modifies its texture, hydraulic conductivity, and thermal conductivity, which, in turn influences resulting rates of HR within the soil column. Analysis of the model at three eddy covariance tower sites in the Alaskan tundra shows that the vertically-resolved soil column formulation accurately captures the zero-curtain phenomenon, in which the temperature of soil layers remain at or near 0 °C during fall freezeback due to the release of latent heat, is critical to capturing observed patterns of wintertime respiration. We find that significant declines in net ecosystem productivity (NEP) occur starting in 2013 and that these declines are driven by increased HR arising from increased precipitation and warming. Sensitivity analyses indicate that the cumulative NEP over the decade responds strongly to the estimated soil carbon stock and more weakly to vegetation abundance at the beginning of the simulation.

 

Mercury is toxic to wildlife and humans, and forests are thought to be a globally important sink for gaseous elemental mercury (GEM) deposition from the atmosphere. Yet there are currently no annual GEM deposition measurements over rural forests. Here we present measurements of ecosystem–atmosphere GEM exchange using tower-based micrometeorological methods in a midlatitude hardwood forest. We measured an annual GEM deposition of 25.1 µg ⋅ m −2 (95% CI: 23.2 to 26.7 1 µg ⋅ m −2 ), which is five times larger than wet deposition of mercury from the atmosphere. Our observed annual GEM deposition accounts for 76% of total atmospheric mercury deposition and also is three times greater than litterfall mercury deposition, which has previously been used as a proxy measure for GEM deposition in forests. Plant GEM uptake is the dominant driver for ecosystem GEM deposition based on seasonal and diel dynamics that show the forest GEM sink to be largest during active vegetation growing periods and middays, analogous to photosynthetic carbon dioxide assimilation. Soils and litter on the forest floor are additional GEM sinks throughout the year. Our study suggests that mercury loading to this forest was underestimated by a factor of about two and that global forests may constitute a much larger global GEM sink than currently proposed. The larger than anticipated forest GEM sink may explain the high mercury loads observed in soils across rural forests, which impair water quality and aquatic biota via watershed Hg export. 

Abstract. The continued warming of the Arctic could release vast stores of carbon into the atmosphere from high-latitude ecosystems, especially from thawingpermafrost. Increasing uptake of carbon dioxide (CO2) by vegetation during longer growing seasons may partially offset such release of carbon. However, evidence of significant net annual release of carbon from site-level observations and model simulations across tundra ecosystems has been inconclusive. To address this knowledge gap, we combined top-down observations of atmospheric CO2 concentration enhancements from aircraft and a tall tower, which integrate ecosystem exchange over large regions, with bottom-up observed CO2 fluxes from tundraenvironments and found that the Alaska North Slope is not a consistent net source nor net sink of CO2 to the atmosphere (ranging from −6 to+6 Tg C yr−1 for 2012–2017). Our analysis suggests that significant biogenic CO2 fluxes from unfrozen terrestrial soils, and likely inland waters, during the early cold season (September–December) are major factors in determining the net annual carbon balance of the North Slope, implying strong sensitivity to the rapidly warming freeze-up period. At the regional level, we find no evidence of the previously reported large late-cold-season (January–April) CO2 emissions to the atmosphere during the study period. Despite the importance of the cold-season CO2 emissions to the annual total, the interannual variability in the net CO2 flux is driven by the variability in growing season fluxes. During the growing season, the regional net CO2 flux is also highly sensitive to the distribution of tundra vegetation types throughout the North Slope. This study shows that quantification and characterization of year-round CO2 fluxes from the heterogeneous terrestrial and aquatic ecosystems in the Arctic using both site-level and atmospheric observations are important to accurately project the Earth system response to future warming. 

The Southern Ocean plays an important role in determining atmospheric carbon dioxide (CO 2 ), yet estimates of air-sea CO 2 flux for the region diverge widely. In this study, we constrained Southern Ocean air-sea CO 2 exchange by relating fluxes to horizontal and vertical CO 2 gradients in atmospheric transport models and applying atmospheric observations of these gradients to estimate fluxes. Aircraft-based measurements of the vertical atmospheric CO 2 gradient provide robust flux constraints. We found an annual mean flux of –0.53 ± 0.23 petagrams of carbon per year (net uptake) south of 45°S during the period 2009–2018. This is consistent with the mean of atmospheric inversion estimates and surface-ocean partial pressure of CO 2 ( P co 2 )–based products, but our data indicate stronger annual mean uptake than suggested by recent interpretations of profiling float observations. 

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. 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.

 

Acetone is one of the most abundant oxygenated volatile organic compounds (VOCs) in the atmosphere. The oceans impose a strong control on atmospheric acetone, yet the oceanic fluxes of acetone remain poorly constrained. In this work, the global budget of acetone is evaluated using two global models: CAM‐chem and GEOS‐Chem. CAM‐chem uses an online air‐sea exchange framework to calculate the bidirectional oceanic acetone fluxes, which is coupled to a data‐oriented machine‐learning approach. The machine‐learning algorithm is trained using a global suite of seawater acetone measurements. GEOS‐Chem uses a fixed surface seawater concentration of acetone to calculate the oceanic fluxes. Both model simulations are compared to airborne observations from a recent global‐scale, multiseasonal campaign, the NASA Atmospheric Tomography Mission (ATom). We find that both CAM‐chem and GEOS‐Chem capture the measured acetone vertical distributions in the remote atmosphere reasonably well. The combined observational and modeling analysis suggests that (i) the ocean strongly regulates the atmospheric budget of acetone. The tropical and subtropical oceans are mostly a net source of acetone, while the high‐latitude oceans are a net sink. (ii) CMIP6 anthropogenic emission inventory may underestimate acetone and/or its precursors in the Northern Hemisphere. (iii) The MEGAN biogenic emissions model may overestimate acetone and/or its precursors, and/or the biogenic oxidation mechanisms may overestimate the acetone yields. (iv) The models consistently overestimate acetone in the upper troposphere‐lower stratosphere over the Southern Ocean in austral winter. (v) Acetone contributes up to 30–40% of hydroxyl radical production in the tropical upper troposphere/lower stratosphere.