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While wetlands are major sources of biogenic methane (CH4), our understanding of resident microbial metabolism is incomplete, which compromises the prediction of CH4 emissions under ongoing climate change. Here, we employed genome-resolved multi-omics to expand our understanding of methanogenesis in the thawing permafrost peatland of Stordalen Mire in Arctic Sweden. In quadrupling the genomic representation of the site’s methanogens and examining their encoded metabolism, we revealed that nearly 20% of the metagenome-assembled genomes (MAGs) encoded the potential for methylotrophic methanogenesis. Further, 27% of the transcriptionally active methanogens expressed methylotrophic genes; for Methanosarcinales and Methanobacteriales MAGs, these data indicated the use of methylated oxygen compounds (e.g., methanol), while for Methanomassiliicoccales, they primarily implicated methyl sulfides and methylamines. In addition to methanogenic methylotrophy, >1,700 bacterial MAGs across 19 phyla encoded anaerobic methylotrophic potential, with expression across 12 phyla. Metabolomic analyses revealed the presence of diverse methylated compounds in the Mire, including some known methylotrophic substrates. Active methylotrophy was observed across all stages of a permafrost thaw gradient in Stordalen, with the most frozen non-methanogenic palsa found to host bacterial methylotrophy and the partially thawed bog and fully thawed fen seen to house both methanogenic and bacterial methylotrophic activities. Methanogenesis across increasing permafrost thaw is thus revised from the sole dominance of hydrogenotrophic production and the appearance of acetoclastic at full thaw to consider the co-occurrence of methylotrophy throughout. Collectively, these findings indicate that methanogenic and bacterial methylotrophy may be an important and previously underappreciated component of carbon cycling and emissions in these rapidly changing wetland habitats.

Peatlands are climate critical carbon (C) reservoirs that could become a C source under continued warming. A strong relationship between plant tissue chemistry and the soil organic matter (SOM) that fuels C gas emissions is inferred, but rarely examined at the molecular level. Here we compared Fourier transform infrared (FT-IR) spectroscopy measurements of solid phase functionalities in plants and SOM to ultra-high-resolution mass spectrometric analyses of plant and SOM water extracts across a palsa-bog-fen thaw and moisture gradient in an Arctic peatland. From these analyses we calculated the C oxidation state (NOSC), a measure which can be used to assess organic matter quality. Palsa plant extracts had the highest NOSC, indicating high quality, whereas extracts of Sphagnum, which dominated the bog, had the lowest NOSC. The percentage of plant compounds that are less bioavailable and accumulate in the peat, increases from palsa (25%) to fen (41%) to bog (47%), reflecting the pattern of percent Sphagnum cover. The pattern of NOSC in the plant extracts was consistent with the high number of consumed compounds in the palsa and low number of consumed compounds in the bog. However, in the FT-IR analysis of the solid phase bog peat, carbohydrate content was high implying high quality SOM. We explain this discrepancy as the result of low solubilization of bog SOM facilitated by the low pH in the bog which makes the solid phase carbohydrates less available to microbial decomposition. Plant-associated condensed aromatics, tannins, and lignin-like compounds declined in the unsaturated palsa peat indicating decomposition, but lignin-like compounds accumulated in the bog and fen peat where decomposition was presumably inhibited by the anaerobic conditions. A molecular-level comparison of the aboveground C sources and peat SOM demonstrates that climate-associated vegetation shifts in peatlands are important controls on the mechanisms underlying changing C g

Permafrost thaw increases active layer thickness, changes landscape hydrology and influences vegetation species composition. These changes alter belowground microbial and geochemical processes, affecting production, consumption and net emission rates of climate forcing trace gases. Net carbon dioxide (CO2) and methane (CH4) fluxes determine the radiative forcing contribution from these climate-sensitive ecosystems. Permafrost peatlands may be a mosaic of dry frozen hummocks, semi-thawed or perched sphagnum dominated areas, wet permafrost-free sedge dominated sites and open water ponds. We revisited estimates of climate forcing made for 1970 and 2000 for Stordalen Mire in northern Sweden and found the trend of increasing forcing continued into 2014. The Mire continued to transition from dry permafrost to sedge and open water areas, increasing by 100% and 35%, respectively, over the 45-year period, causing the net radiative forcing of Stordalen Mire to shift from negative to positive. This trend is driven by transitioning vegetation community composition, improved estimates of annual CO2 and CH4 exchange and a 22% increase in the IPCC's 100-year global warming potential (GWP_100) value for CH4. These results indicate that discontinuous permafrost ecosystems, while still remaining a net overall sink of C, can become a positive feedback to climate change on decadal timescales. This article is part of a discussion meeting issue ‘Rising methane: is warming feeding warming? (part 2)’.

Author Posting. © American Geophysical Union, 2022. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Global Biogeochemical Cycles 36(1), (2022): e2021GB007113, https://doi.org/10.1029/2021GB007113., Stordalen Mire is a peatland in the discontinuous permafrost zone in arctic Sweden that exhibits a habitat gradient from permafrost palsa, to Sphagnum bog underlain by permafrost, to Eriophorum-dominated fully thawed fen. We used three independent approaches to evaluate the annual, multi-decadal, and millennial apparent carbon accumulation rates (aCAR) across this gradient: seven years of direct semi-continuous measurement of CO2 and CH4 exchange, and 21 core profiles for 210Pb and 14C peat dating. Year-round chamber measurements indicated net carbon balance of −13 ± 8, −49 ± 15, and −91 ± 43 g C m−2 y−1 for the years 2012–2018 in palsa, bog, and fen, respectively. Methane emission offset 2%, 7%, and 17% of the CO2 uptake rate across this gradient. Recent aCAR indicates higher C accumulation rates in surface peats in the palsa and bog compared to current CO2 fluxes, but these assessments are more similar in the fen. aCAR increased from low millennial-scale levels (17–29 g C m−2 y−1) to moderate aCAR of the past century (72–81 g C m−2 y−1) to higher recent aCAR of 90–147 g C m−2 y−1. Recent permafrost collapse, greater inundation and vegetation response has made the landscape a stronger CO2 sink, but this CO2 sink is increasingly offset by rising CH4 emissions, dominated by modern carbon as determined by 14C. The higher CH4 emissions result in higher net CO2-equivalent emissions, indicating that radiative forcing of this mire and similar permafrost ecosystems will exert a warming influence on future climate., We would like to acknowledge the following funding in support of this project: Swedish Research Council (Vetenskapsrådet, VR) grants (NT 2007-4547 and NT 2013-5562 to P. Crill), U.S. Department of Energy grants (DE-SC0004632 and DE-SC0010580 to V. Rich and S. Saleska), and U.S. National Science Foundation MacroSystems Biology grant (NSF EF #1241037, PI Varner). This work was supported by the U.S. Department of Energy, Office of Science, Office of Biological and Environmental Research under the Genomic Science program. We also acknowledge funding from the National Science Foundation for the EMERGE Biology Integration Institute, NSF Award #2022070., 2022-07-03

Northern post-glacial lakes are significant, increasing sources of atmospheric carbon through ebullition (bubbling) of microbially-produced methane (CH4) from sediments. Ebullitive CH4 flux correlates strongly with temperature, reflecting that solar radiation drives emissions. However, here we show that the slope of the temperature-CH4 flux relationship differs spatially across two post-glacial lakes in Sweden. We compared these CH4 emission patterns with sediment microbial (metagenomic and amplicon), isotopic, and geochemical data. The temperature-associated increase in CH4 emissions was greater in lake middles-where methanogens were more abundant-than edges, and sediment communities were distinct between edges and middles. Microbial abundances, including those of CH4-cycling microorganisms and syntrophs, were predictive of porewater CH4 concentrations. Results suggest that deeper lake regions, which currently emit less CH4 than shallower edges, could add substantially to CH4 emissions in a warmer Arctic and that CH4 emission predictions may be improved by accounting for spatial variations in sediment microbiota.

© The Author(s), 2020. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Wilson, S. T., Al-Haj, A. N., Bourbonnais, A., Frey, C., Fulweiler, R. W., Kessler, J. D., Marchant, H. K., Milucka, J., Ray, N. E., Suntharalingam, P., Thornton, B. F., Upstill-Goddard, R. C., Weber, T. S., Arevalo-Martinez, D. L., Bange, H. W., Benway, H. M., Bianchi, D., Borges, A., V., Chang, B. X., Crill, P. M., del Valle, D. A., Farias, L., Joye, S. B., Kock, A., Labidi, J., Manning, C. C., Pohlman, J. W., Rehder, G., Sparrow, K. J., Tortell, P. D., Treude, T., Valentine, D. L., Ward, B. B., Yang, S., & Yurganov, L. N. Ideas and perspectives: a strategic assessment of methane and nitrous oxide measurements in the marine environment. Biogeosciences, 17(22), (2020): 5809-5828, https://doi.org/10.5194/bg-17-5809-2020., In the current era of rapid climate change, accurate characterization of climate-relevant gas dynamics – namely production, consumption, and net emissions – is required for all biomes, especially those ecosystems most susceptible to the impact of change. Marine environments include regions that act as net sources or sinks for numerous climate-active trace gases including methane (CH4) and nitrous oxide (N2O). The temporal and spatial distributions of CH4 and N2O are controlled by the interaction of complex biogeochemical and physical processes. To evaluate and quantify how these mechanisms affect marine CH4 and N2O cycling requires a combination of traditional scientific disciplines including oceanography, microbiology, and numerical modeling. Fundamental to these efforts is ensuring that the datasets produced by independent scientists are comparable and interoperable. Equally critical is transparent communication within the research community about the technical improvements required to increase our collective understanding of marine CH4 and N2O. A workshop sponsored by Ocean Carbon and Biogeochemistry (OCB) was organized to enhance dialogue and collaborations pertaining to marine CH4 and N2O. Here, we summarize the outcomes from the workshop to describe the challenges and opportunities for near-future CH4 and N2O research in the marine environment., This article was an outcome of a workshop organized by the Ocean Carbon and Biogeochemistry (OCB) project office, which is supported by the US National Science Foundation (grant no. 1558412) and the National Aeronautics and Space Administration (grant no. NNX17AB17G). The workshop received additional funding from the Scientific Committee on Ocean Research (SCOR) which receives funding from the US National Science Foundation (grant no. 1840868) and contributions by additional national SCOR committees. The Chilean COPAS N2O time-series measurements were supported by Agencia Nacional de Investigación y Desarrollo (grant no. 1200861).

Mechanisms controlling CO2 and CH4 production in wetlands are central to understanding carbon cycling and greenhouse gas exchange. However, the volatility of these respiration products complicates quantifying their rates of production in the field. Attempts to circumvent the challenges through closed system incubations, from which gases cannot escape, have been used to investigate bulk in situ geochemistry. Efforts towards mapping mechanistic linkages between geochemistry and microbiology have raised concern regarding sampling and incubation-induced perturbations. Microorganisms are impacted by oxygen exposure, increased temperatures and accumulation of metabolic products during handling, storage, and incubation. We probed the extent of these perturbations, and their influence on incubation results, using high-resolution geochemical and microbial gene-based community profiling of anaerobically incubated material from three wetland habitats across a permafrost peatland. We compared the original field samples to the material anaerobically incubated over 50 days. Bulk geochemistry and phylum-level microbiota in incubations largely reflected field observations, but divergence between field and incubations occurred in both geochemistry and lineage-level microbial composition when examined at closer resolution. Despite the changes in representative lineages over time, inferred metabolic function with regards to carbon cycling largely reproduced field results suggesting functional consistency. Habitat differences among the source materials remained the largest driver of variation in geochemical and microbial differences among the samples in both incubations and field results. While incubations may have limited usefulness for identifying specific mechanisms, they remain a viable tool for probing bulk-scale questions related to anaerobic C cycling, including CO2 and CH4 dynamics

Abstract. Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. Atmospheric emissions and concentrations of CH4 continue to increase, making CH4 the second most important human-influenced greenhouse gas in terms of climate forcing, after carbon dioxide (CO2). The relative importance of CH4 compared to CO2 depends on its shorter atmospheric lifetime, stronger warming potential, and variations in atmospheric growth rate over the past decade, the causes of which are still debated. Two major challenges in reducing uncertainties in the atmospheric growth rate arise from the variety of geographically overlapping CH4 sources and from the destruction of CH4 by short-lived hydroxyl radicals (OH). To address these challenges, we have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate new research aimed at improving and regularly updating the global methane budget. Following Saunois et al. (2016), we present here the second version of the living review paper dedicated to the decadal methane budget, integrating results of top-down studies (atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up estimates (including process-based models for estimating land surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations). For the 2008–2017 decade, global methane emissions are estimated by atmospheric inversions (a top-down approach) to be 576 Tg CH4 yr−1 (range 550–594, corresponding to the minimum and maximum estimates of the model ensemble). Of this total, 359 Tg CH4 yr−1 or ∼ 60 % is attributed to anthropogenic sources, that is emissions caused by direct human activity (i.e. anthropogenic emissions; range 336–376 Tg CH4 yr−1 or 50 %–65 %). The mean annual total emission for the new decade (2008–2017) is 29 Tg CH4 yr−1 large

Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. Atmospheric emissions and concentrations of CH4 continue to increase, making CH4 the second most important human-influenced greenhouse gas in terms of climate forcing, after carbon dioxide (CO2). The relative importance of CH4 compared to CO2 depends on its shorter atmospheric lifetime, stronger warming potential, and variations in atmospheric growth rate over the past decade, the causes of which are still debated. Two major challenges in reducing uncertainties in the atmospheric growth rate arise from the variety of geographically overlapping CH4 sources and from the destruction of CH4 by short-lived hydroxyl radicals (OH). To address these challenges, we have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate new research aimed at improving and regularly updating the global methane budget. Following Saunois et al. (2016), we present here the second version of the living review paper dedicated to the decadal methane budget, integrating results of top-down studies (atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up estimates (including process-based models for estimating land surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations). For the 2008-2017 decade, global methane emissions are estimated by atmospheric inversions (a top-down approach) to be 576 Tg CH4 yr(-1) (range 550-594, corresponding to the minimum and maximum estimates of the model ensemble). Of this total, 359 Tg CH4 yr(-1) or similar to 60 % is attributed to anthropogenic sources, that is emissions caused by direct human activity (i.e. anthropogenic emissions; range 336-376 Tg CH4 yr(-1) or 50 %-65 %). The mean annual total emission for the new decade (2008-2017) is 29 Tg CH4 yr(-1) larger, Funding Agencies|FAO

Lake emissions of the climate forcing trace gas methane (CH4) are spatiotemporally variable, but biases in flux measurements arising from undersampling are poorly quantified. We use a multiyear data set (2009-2017) of ice-free CH(4)emissions from three subarctic lakes obtained with bubble traps (n = 14,677), floating chambers (n = 1,306), and surface concentrations plus a gas transfer model (n = 535) to quantify these biases and evaluate corrections. Sampling primarily in warmer summer months, as is common, overestimates the ice-free season flux by a factor 1.4-1.8. Temperature proxies based on Arrhenius functions that closely fit measured fluxes (R-2 >= 0.93) enable gap filling the colder months of the ice-free season and reduce sampling bias. Ebullition (activation energy 1.36 eV) expressed greater temperature sensitivity than diffusion (1.00 eV). Resolving seasonal and interannual variability in fluxes with proxies requires similar to 135 sampling days for ebullition, and 22 and 14 days for diffusion via models and chambers, respectively.

The release of long-stored carbon from thawed permafrost could fuel increased methanogenesis in northern lakes, but it remains unclear whether old carbon substrates released from permafrost are metabolized as rapidly by methanogenic microbial communities as recently produced organic carbon. Here, we apply methane (CH4) clumped isotope (Delta(18)) and C-14 measurements to test whether rates of methanogenesis are related to carbon substrate age. Results from culture experiments indicate that Delta(18) values are negatively correlated with CH4 production rate. Measurements of ebullition samples from thermokarst lakes in Alaska and glacial lakes in Sweden indicate strong negative correlations between CH4 Delta(18) and the fraction modern carbon. These correlations imply that CH4 derived from older carbon substrates is produced relatively slowly. Relative rates of methanogenesis, as inferred from Delta(18) values, are not positively correlated with CH4 flux estimates, highlighting the likely importance of environmental variables other than CH4 production rates in controlling ebullition fluxes. Plain Language Summary There is concern that carbon from thawed permafrost will be emitted to the atmosphere as methane (CH4). It is currently uncertain whether old organic carbon from thawed permafrost can be converted to CH4 as rapidly as organic carbon recently fixed by primary producers. We address this question by combining radiocarbon and clumped isotope measurements of CH4 from lakes in permafrost landscapes. Radiocarbon (C-14) measurements indicate the age of CH4 carbon sources. We present data from culture experiments that support the hypothesis that clumped isotope values are dependent on microbial CH4 production rate. In lake bubble samples, we observe a strong correlation between these two measurements, which implies that CH4 formed from older carbon is produced relatively slowly. We also find that higher rates of CH4 production, as inferred from clumped isotopes, are n

Modern microbial and ecosystem sciences require diverse interdisciplinary teams that are often challenged in “speaking” to one another due to different languages and data product types. Here we introduce the IsoGenie Database (IsoGenieDB; https://isogenie-db.asc.ohio-state.edu/), a de novo developed data management and exploration platform, as a solution to this challenge of accurately representing and integrating heterogenous environmental and microbial data across ecosystem scales. The IsoGenieDB is a public and private data infrastructure designed to store and query data generated by the IsoGenie Project, a ~10 year DOE-funded project focused on discovering ecosystem climate feedbacks in a thawing permafrost landscape. The IsoGenieDB provides (i) a platform for IsoGenie Project members to explore the project’s interdisciplinary datasets across scales through the inherent relationships among data entities, (ii) a framework to consolidate and harmonize the datasets needed by the team’s modelers, and (iii) a public venue that leverages the same spatially explicit, disciplinarily integrated data structure to share published datasets. The IsoGenieDB is also being expanded to cover the NASA-funded Archaea to Atmosphere (A2A) project, which scales the findings of IsoGenie to a broader suite of Arctic peatlands, via the umbrella A2A Database (A2A-DB). The IsoGenieDB’s expandability and flexible architecture allow it to serve as an example ecosystems database., IsoGenie Project Team, A2A Project Team

In the current era of rapid climate change, accurate characterization of climate-relevant gas dynamics-namely production, consumption, and net emissions-is required for all biomes, especially those ecosystems most susceptible to the impact of change. Marine environments include regions that act as net sources or sinks for numerous climateactive trace gases including methane (CH4) and nitrous oxide (N2O). The temporal and spatial distributions of CH4 and N2O are controlled by the interaction of complex biogeochemical and physical processes. To evaluate and quantify how these mechanisms affect marine CH4 and N2O cycling requires a combination of traditional scientific disciplines including oceanography, microbiology, and numerical modeling. Fundamental to these efforts is ensuring that the datasets produced by independent scientists are comparable and interoperable. Equally critical is transparent communication within the research community about the technical improvements required to increase our collective understanding of marine CH4 and N2O. A workshop sponsored by Ocean Carbon and Biogeochemistry (OCB) was organized to enhance dialogue and collaborations pertaining to marine CH4 and N2O. Here, we summarize the outcomes from the workshop to describe the challenges and opportunities for near-future CH4 and N2O research in the marine environment.

Northern lakes are important sources of the climate forcing trace gases methane (CH4) and carbon dioxide (CO2). A substantial portion of lakes' annual emissions can take place immediately after ice melt in spring. The drivers of these fluxes are neither well constrained nor fully understood. We present a detailed carbon gas budget for three subarctic lakes, using 6 years of eddy covariance and 9 years of manual flux measurements. We combine measurements of temperature, dissolved oxygen, and CH4 stable isotopologues to quantify functional relationships between carbon gas production and conversion, energy inputs, and the redox regime. Spring emissions were regulated by the availability of oxygen in winter, rather than temperature as during ice‐free conditions. Under‐ice storage increased predictably with ice‐cover duration, and CH4 accumulation rates (25 ± 2 mg CH4‐C·m−2·day−1) exceeded summer emissions (19 ± 1 mg CH4‐C·m−2·day−1). The seasonally ice‐covered lakes emitted 26–59% of the annual CH4 flux and 15–30% of the annual CO2 flux at ice‐off. Reduced spring emissions were associated with winter snowmelt events, which can transport water downstream and oxygenate the water column. Stable isotopes indicate that 64–96% of accumulated CH4 escaped oxidation, implying that a considerable portion of the dissolved gases produced over winter may evade to the atmosphere.

Arctic regions are experiencing rapid warming, leading to permafrost thaw and formation of numerous water bodies. Although small ponds in particular are considered hot spots for methane (CH4) release, long-term studies of CH4 efflux from these surfaces are rare. We have collected an extensive data set of CH4 ebullition (bubbling) measurements from eight small thaw ponds (<0.001 km(2)) with different physical and hydrological characteristics over four summer seasons, the longest set of observations from thaw ponds to date. The measured fluxes were highly variable with an average of 20.0 mg CH4 . m(-2) . day(-1) (median: 4.1 mg CH4 . m(-2) . day(-1), n = 2,063) which is higher than that of most nearby lakes. The ponds were categorized into four types based on clear and significant differences in bubble flux. We found that the amount of CH4 released as bubbles from ponds was very weakly correlated with environmental variables, like air temperature and atmospheric pressure, and was potentially more related to differences in physical characteristics of the ponds. Using our measured average daily bubble flux plus the available literature, we estimate circumpolar thaw ponds <0.001 km(2) in size to emit between 0.2 and 1.0 Tg of CH4 through ebullition. Our findings exemplify the importance of high-frequency measurements over long study periods in order to adequately capture the variability of these water bodies. Through the expansion of current spatial and temporal monitoring efforts, we can increase our ability to estimate CH4 emissions from permafrost pond ecosystems now and in the future.

Projected 21st century changes in high-latitude climate are expected to have significant impacts on permafrost thaw, which could cause substantial increases in emissions to the atmosphere of carbon dioxide (CO2) and methane (CH4, which has a global warming potential 28 times larger than CO2 over a 100-year horizon). However, predicted CH4 emission rates are very uncertain due to difficulties in modeling complex interactions among hydrological, thermal, biogeochemical, and plant processes. Methanogenic production pathways (i.e., acetoclastic [AM] and hydrogenotrophic [HM]) and the magnitude of CH4 emissions may both change as permafrost thaws, but a mechanistic analysis of controls on such shifts in CH4 dynamics is lacking. In this study, we reproduced observed shifts in CH4 emissions and production pathways with a comprehensive biogeochemical model (ecosys) at the Stordalen Mire in subarctic Sweden. Our results demonstrate that soil temperature changes differently affect AM and HM substrate availability, which regulates magnitudes of AM, HM, and thereby net CH4 emissions. We predict very large landscape-scale, vertical, and temporal variations in the modeled HM fraction, highlighting that measurement strategies for metrics that compare CH4 production pathways could benefit from model informed scale of temporal and spatial variance. Finally, our findings suggest that the warming and wetting trends projected in northern peatlands could enhance peatland AM fraction and CH4 emissions even without further permafrost degradation.

Recent efforts have brought together bottom-up quantification approaches (inventories and process-based models) and top-down approaches using regional observations of methane atmospheric concentrations through inverse modelling to better estimate the northern high-latitude methane sources. Nevertheless, for both approaches, the relatively small number of available observations in northern high-latitude regions leaves gaps in our understanding of the drivers and distributions of the different types of regional methane sources. Observations of methane isotope ratios, performed with instruments that are becoming increasingly affordable and accurate, could bring new insights on the contributions of methane sources and sinks. Here, we present the source signal that could be observed from methane isotopic (CH4)-C-13 measurements if high-resolution observations were available and thus what requirements should be fulfilled in future instrument deployments in terms of accuracy in order to constrain different emission categories. This theoretical study uses the regional chemistry-transport model CHIMERE driven by different scenarios of isotopic signatures for each regional methane source mix. It is found that if the current network of methane monitoring sites were equipped with instruments measuring the isotopic signal continuously, only sites that are significantly influenced by emission sources could differentiate regional emissions with a reasonable level of confidence. For example, wetland emissions require daily accuracies lower than 0.2 parts per thousand for most of the sites. Detecting East Siberian Arctic Shelf (ESAS) emissions requires accuracies lower than 0.05 parts per thousand at coastal Russian sites (even lower for other sites). Freshwater emissions would be detectable with an uncertainty lower than 0.1 parts per thousand for most continental sites. Except Yakutsk, Siberian sites require stringent uncertainty (lower than 0.05 parts per thousand) to detect anth

Warming Arctic temperatures have led to permafrost thaw that threatens to release previously sequestered mercury (Hg) back into the environment. Mobilisation of Hg in permafrost waters is of concern, as Hg methylation produced under water-saturated conditions results in the neurotoxin, methyl Hg (MeHg). Thawing permafrost may enhance Hg export, but the magnitude and mechanisms of this mobilisation within Arctic ecosystems remain poorly understood. Such uncertainty limits prognostic modelling of Hg mobilisation and impedes a comprehensive assessment of its threat to Arctic ecosystems and peoples. Here, we address this knowledge gap through an assessment of Hg dynamics across a well-studied permafrost thaw sequence at the peak of the growing season in biologically active peat overlying permafrost, quantifying total gaseous mercury (TGM) fluxes, total mercury (Hg-Tot) in the active layer peat, porewater MeHg concentrations, and identifying microbes with the potential to methylate Hg. During the initial thaw, TGM is liberated, likely by photoreduction from permafrost where it was previously stored for decades to centuries. As thawing proceeds, TGM is largely driven by hydrologic changes as evidenced by Hg accumulation in water-logged, organic-rich peat sediments in fen sites. MeHg in porewaters increase across the thaw gradient, a pattern coincident with increases in the relative abundance of microbes possibly containing genes allowing for methylation of ionic Hg. Findings suggest that under changing climate, frozen, well-drained habitats will thaw and collapse into saturated landscapes, increasing the production of MeHg and providing a significant source of the toxic, bioaccumulative contaminant.