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Methane (CH4) is a strong greenhouse gas that has become the focus of climate mitigation policies in recent years. Ethane / methane ratios can be used to identify and partition the difference sources of methane, especially in areas with natural gas mixed with biogenic methane emissions, such as cities. We assessed the precision, accuracy and selectivity of three commercially available laser-based analyzers that have been marketed as measuring instantaneous dry mole fractions of methane and ethane in ambient air. The Aerodyne SuperDUAL instrument performed best of the three instruments but it requires expertise to operate and space for the large footprint. The Aeris Mira Ultra LDS analyzer also performed well for the price point and small footprint but required characterization of the water vapor dependence of reported concentrations and careful setup for use. The Picarro G2210-i precisely measured methane but it did not detect the 10 ppbv increases in ambient ethane detected by the other two instruments when sampling a plume of incompletely combusted natural gas. For long-term tower deployments or those with large mobile laboratories, the Aerodyne SuperDUAL provides the best precision for methane and ethane. For smaller mobile platforms, the Aeris MIRA is a more compact analyzer, and with careful use, can quantify thermogenic methane sources to sufficient precision for short term deployments in urban or oil and gas areas. We weighed the advantages of each instrument, including size, power requirement, ease of use on mobile platforms, and expertise needed to operate the instrument, and we recommend the Aerodyne SuperDUAL or the Aeris MIRA Ultra LDS depending on the situation.

Long-term atmospheric CO2 concentration records have suggested a reduction in the positive effect of warming on high-latitude carbon uptake since the 1990s. A variety of mechanisms have been proposed to explain the reduced net carbon sink of northern ecosystems with increased air temperature, including water stress on vegetation and increased respiration over recent decades. However, the lack of consistent long-term carbon flux and in situ soil moisture data has severely limited our ability to identify the mechanisms responsible for the recent reduced carbon sink strength. In this study, we used a record of nearly 100 site-years of eddy covariance data from 11 continuous permafrost tundra sites distributed across the circumpolar Arctic to test the temperature (expressed as growing degree days, GDD) responses of gross primary production (GPP), net ecosystem exchange (NEE), and ecosystem respiration (ER) at different periods of the summer (early, peak, and late summer) including dominant tundra vegetation classes (graminoids and mosses, and shrubs). We further tested GPP, NEE, and ER relationships with soil moisture and vapor pressure deficit to identify potential moisture limitations on plant productivity and net carbon exchange. Our results show a decrease in GPP with rising GDD during the peak summer (July) for both vegetation classes, and a significant relationship between the peak summer GPP and soil moisture after statistically controlling for GDD in a partial correlation analysis. These results suggest that tundra ecosystems might not benefit from increased temperature as much as suggested by several terrestrial biosphere models, if decreased soil moisture limits the peak summer plant productivity, reducing the ability of these ecosystems to sequester carbon during the summer.

Rapid Arctic environmental change affects the entire Earth system as thawing permafrost ecosystems release greenhouse gases to the atmosphere. Understanding how much permafrost carbon will be released, over what time frame, and what the relative emissions of carbon dioxide and methane will be is key for understanding the impact on global climate. In addition, the response of vegetation in a warming climate has the potential to offset at least some of the accelerating feedback to the climate from permafrost carbon. Temperature, organic carbon, and ground ice are key regulators for determining the impact of permafrost ecosystems on the global carbon cycle. Together, these encompass services of permafrost relevant to global society as well as to the people living in the region and help to determine the landscape-level response of this region to a changing climate.

Approximately half of the carbon dioxide (CO 2) released annually by the combustion of fossil fuels stays in the atmosphere (Friedlingstein et al., 2022; Keeling et al., 1976; Schimel et al., 2001). The remaining CO 2 is taken up by the terrestrial biosphere and ocean in roughly equal proportions (Keeling & Manning, 2014; Khatiwala et al., 2009; Sabine et al., 2004). The efficiency of the ocean and land sinks varies with both climate and atmospheric CO 2 , representing an important feedback in the climate system (e.g., Ballantyne et al., 2012

This article provides an overview of the NASA Atmospheric Tomography (ATom) mission and a summary of selected scientific findings to date. ATom was an airborne measurements and modeling campaign aimed at characterizing the composition and chemistry of the troposphere over the most remote regions of the Pacific, Southern, Atlantic, and Arctic Oceans, and examining the impact of anthropogenic and natural emissions on a global scale. These remote regions dominate global chemical reactivity and are exceptionally important for global air quality and climate. ATom data provide the in situ measurements needed to understand the range of chemical species and their reactions, and to test satellite remote sensing observations and global models over large regions of the remote atmosphere. Lack of data in these regions, particularly over the oceans, has limited our understanding of how atmospheric composition is changing in response to shifting anthropogenic emissions and physical climate change. ATom was designed as a global-scale tomographic sampling mission with extensive geographic and seasonal coverage, tropospheric vertical profiling, and detailed speciation of reactive compounds and pollution tracers. ATom flew the NASA DC-8 research aircraft over four seasons to collect a comprehensive suite of measurements of gases, aerosols, and radical species from the remote troposphere and lower stratosphere on four global circuits from 2016 to 2018. Flights maintained near-continuous vertical profiling of 0.15–13-km altitudes on long meridional transects of the Pacific and Atlantic Ocean basins. Analysis and modeling of ATom data have led to the significant early findings highlighted here.

Past efforts to synthesize and quantify the magnitude and change in carbon dioxide (CO2) fluxes in terrestrial ecosystems across the rapidly warming Arctic–boreal zone (ABZ) have provided valuable information but were limited in their geographical and temporal coverage. Furthermore, these efforts have been based on data aggregated over varying time periods, often with only minimal site ancillary data, thus limiting their potential to be used in large-scale carbon budget assessments. To bridge these gaps, we developed a standardized monthly database of Arctic–boreal CO2 fluxes (ABCflux) that aggregates in situ measurements of terrestrial net ecosystem CO2 exchange and its derived partitioned component fluxes: gross primary productivity and ecosystem respiration. The data span from 1989 to 2020 with over 70 supporting variables that describe key site conditions (e.g., vegetation and disturbance type), micrometeorological and environmental measurements (e.g., air and soil temperatures), and flux measurement techniques. Here, we describe these variables, the spatial and temporal distribution of observations, the main strengths and limitations of the database, and the potential research opportunities it enables. In total, ABCflux includes 244 sites and 6309 monthly observations; 136 sites and 2217 monthly observations represent tundra, and 108 sites and 4092 observations represent the boreal biome. The database includes fluxes estimated with chamber (19 % of the monthly observations), snow diffusion (3 %) and eddy covariance (78 %) techniques. The largest number of observations were collected during the climatological summer (June–August; 32 %), and fewer observations were available for autumn (September–October; 25 %), winter (December–February; 18 %), and spring (March–May; 25 %). ABCflux can be used in a wide array of empirical, remote sensing and modeling studies to improve understanding of the regional and temporal variability in CO2 fluxes and to better estimate the terrestrial ABZ CO2 budget. ABCflux is openly and freely available online (Virkkala et al., 2021b, https://doi.org/10.3334/ORNLDAAC/1934).

The NASA Atmospheric Tomography (ATom) mission built a photochemical climatology of air parcels based on in situ measurements with the NASA DC-8 aircraft along objectively planned profiling transects through the middle of the Pacific and Atlantic oceans. In this paper we present and analyze a data set of 10 s (2 km) merged and gap-filled observations of the key reactive species driving the chemical budgets of O3 and CH4 (O3, CH4, CO, H2O, HCHO, H2O2, CH3OOH, C2H6, higher alkanes, alkenes, aromatics, NOx, HNO3, HNO4, peroxyacetyl nitrate, and other organic nitrates), consisting of 146 494 distinct air parcels from ATom deployments 1 through 4. Six models calculated the O3 and CH4 photochemical tendencies from this modeling data stream for ATom 1. We find that 80 %–90 % of the total reactivity lies in the top 50 % of the parcels and 25 %–35 % in the top 10 %, supporting previous model-only studies that tropospheric chemistry is driven by a fraction of all the air. Surprisingly, the probability densities of species and reactivities averaged on a model scale (100 km) differ only slightly from the 2 km ATom 10 s data, indicating that much of the heterogeneity in tropospheric chemistry can be captured with current global chemistry models. Comparing the ATom reactivities over the tropical oceans with climatological statistics from six global chemistry models, we find generally good agreement with the reactivity rates for O3 and CH4. Models distinctly underestimate O3 production below 2 km relative to the mid-troposphere, and this can be traced to lower NOx levels than observed. Attaching photochemical reactivities to measurements of chemical species allows for a richer, yet more constrained-to-what-matters, set of metrics for model evaluation. This paper presents a corrected version of the paper published under the same authors and title (sans “corrected”) as https://doi.org/10.5194/acp-21-13729-2021.

Arctic-boreal landscapes are experiencing profound warming, along with changes in ecosystem moisture status and disturbance from fire. This region is of global importance in terms of carbon feedbacks to climate, yet the sign (sink or source) and magnitude of the Arctic-boreal carbon budget within recent years remains highly uncertain. Here, we provide new estimates of recent (2003–2015) vegetation gross primary productivity (GPP), ecosystem respiration (Reco), net ecosystem CO2 exchange (NEE; Reco − GPP), and terrestrial methane (CH4) emissions for the Arctic-boreal zone using a satellite data-driven process-model for northern ecosystems (TCFM-Arctic), calibrated and evaluated using measurements from >60 tower eddy covariance (EC) sites. We used TCFM-Arctic to obtain daily 1-km2 flux estimates and annual carbon budgets for the pan-Arctic-boreal region. Across the domain, the model indicated an overall average NEE sink of −850 Tg CO2-C year−1. Eurasian boreal zones, especially those in Siberia, contributed to a majority of the net sink. In contrast, the tundra biome was relatively carbon neutral (ranging from small sink to source). Regional CH4 emissions from tundra and boreal wetlands (not accounting for aquatic CH4) were estimated at 35 Tg CH4-C year−1. Accounting for additional emissions from open water aquatic bodies and from fire, using available estimates from the literature, reduced the total regional NEE sink by 21% and shifted many far northern tundra landscapes, and some boreal forests, to a net carbon source. This assessment, based on in situ observations and models, improves our understanding of the high-latitude carbon status and also indicates a continued need for integrated site-to-regional assessments to monitor the vulnerability of these ecosystems to climate change.

Volatile chemical products (VCPs) and other non-combustion-related sources have become important for urban air quality, and bottom-up calculations report emissions of a variety of functionalized compounds that remain understudied and uncertain in emissions estimates. Using a new instrumental configuration, we present online measurements of oxygenated organic compounds in a US megacity over a 10 d wintertime sampling period, when biogenic sources and photochemistry were less active. Measurements were conducted at a rooftop observatory in upper Manhattan, New York City, USA using a Vocus chemical ionization time-of-flight mass spectrometer, with ammonium (NH4+) as the reagent ion operating at 1 Hz. The range of observations spanned volatile, intermediate-volatility, and semi-volatile organic compounds, with targeted analyses of ∼150 ions, whose likely assignments included a range of functionalized compound classes such as glycols, glycol ethers, acetates, acids, alcohols, acrylates, esters, ethanolamines, and ketones that are found in various consumer, commercial, and industrial products. Their concentrations varied as a function of wind direction, with enhancements over the highly populated areas of the Bronx, Manhattan, and parts of New Jersey, and included abundant concentrations of acetates, acrylates, ethylene glycol, and other commonly used oxygenated compounds. The results provide top-down constraints on wintertime emissions of these oxygenated and functionalized compounds, with ratios to common anthropogenic marker compounds and comparisons of their relative abundances to two regionally resolved emissions inventories used in urban air quality models.

Understanding the sources and sinks of methane (CH4) is critical to both predicting and mitigating future climate change. There are large uncertainties in the global budget of atmospheric CH4, but natural emissions are estimated to be of a similar magnitude to anthropogenic emissions. To understand CH4 flux from biogenic sources in the United States (US) of America, a multi-scale CH4 observation network focused on CH4 flux rates, processes, and scaling methods is required. This can be achieved with a network of ground-based observations that are distributed based on climatic regions and land cover. To determine the gaps in physical infrastructure for developing this network, we need to understand the landscape representativeness of the current infrastructure. We focus here on eddy covariance (EC) flux towers because they are essential for a bottom-up framework that bridges the gap between point-based chamber measurements and airborne or satellite platforms that inform policy decisions and global climate agreements. Using dissimilarity, multidimensional scaling, and cluster analysis, the US was divided into 10 clusters distributed across temperature and precipitation gradients. We evaluated dissimilarity within each cluster for research sites with active CH4 EC towers to identify gaps in existing infrastructure that limit our ability to constrain the contribution of US biogenic CH4 emissions to the global budget. Through our analysis using climate, land cover, and location variables, we identified priority areas for research infrastructure to provide a more complete understanding of the CH4 flux potential of ecosystem types across the US. Clusters corresponding to Alaska and the Rocky Mountains, which are inherently difficult to capture, are the most poorly represented, and all clusters require a greater representation of vegetation types.

Climate change is causing an intensification in tundra fires across the Arctic, including the unprecedented 2015 fires in the Yukon-Kuskokwim (YK) Delta. The YK Delta contains extensive surface waters (∼33% cover) and significant quantities of organic carbon, much of which is stored in vulnerable permafrost. Inland aquatic ecosystems act as hot-spots for landscape CO2 and CH4 emissions and likely represent a significant component of the Arctic carbon balance, yet aquatic fluxes of CO2 and CH4 are also some of the most uncertain. We measured dissolved CH4 and CO2 concentrations (n = 364), in surface waters from different types of waterbodies during summers from 2016 to 2019. We used Sentinel-2 multispectral imagery to classify landcover types and area burned in contributing watersheds. We develop a model using machine learning to assess how waterbody properties (size, shape, and landscape properties), environmental conditions (O2, temperature), and surface water chemistry (dissolved organic carbon composition, nutrient concentrations) help predict in situ observations of CH4 and CO2 concentrations across deltaic waterbodies. CO2 concentrations were negatively related to waterbody size and positively related to waterbody edge effects. CH4 concentrations were primarily related to organic matter quantity and composition. Waterbodies in burned watersheds appeared to be less carbon limited and had longer soil water residence times than in unburned watersheds. Our results illustrate the importance of small lakes for regional carbon emissions and demonstrate the need for a mechanistic understanding of the drivers of greenhouse gasses in small waterbodies.

Arctic warming is affecting snow cover and soil hydrology, with consequences for carbon sequestration in tundra ecosystems. The scarcity of observations in the Arctic has limited our understanding of the impact of covarying environmental drivers on the carbon balance of tundra ecosystems. In this study, we address some of these uncertainties through a novel record of 119 site-years of summer data from eddy covariance towers representing dominant tundra vegetation types located on continuous permafrost in the Arctic. Here we found that earlier snowmelt was associated with more tundra net CO2 sequestration and higher gross primary productivity (GPP) only in June and July, but with lower net carbon sequestration and lower GPP in August. Although higher evapotranspiration (ET) can result in soil drying with the progression of the summer, we did not find significantly lower soil moisture with earlier snowmelt, nor evidence that water stress affected GPP in the late growing season. Our results suggest that the expected increased CO2 sequestration arising from Arctic warming and the associated increase in growing season length may not materialize if tundra ecosystems are not able to continue sequestering CO2 later in the season.

The Southern Ocean plays an important role in determining atmospheric carbon dioxide (CO2), yet estimates of air-sea CO2 flux for the region diverge widely. In this study, we constrained Southern Ocean air-sea CO2 exchange by relating fluxes to horizontal and vertical CO2 gradients in atmospheric transport models and applying atmospheric observations of these gradients to estimate fluxes. Aircraft-based measurements of the vertical atmospheric CO2 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 CO2 (PCO2)–based products, but our data indicate stronger annual mean uptake than suggested by recent interpretations of profiling float observations.

The northern high latitude (NHL, 40°N to 90°N) is where the second peak region of gross primary productivity (GPP) other than the tropics. The summer NHL GPP is about 80% of the tropical peak, but both regions are still highly uncertain (Norton et al. 2019, https://doi.org/10.5194/bg-16-3069-2019). Carbonyl sulfide (OCS) provides an important proxy for photosynthetic carbon uptake. Here we optimize the OCS plant uptake fluxes across the NHL by fitting atmospheric concentration simulation with the GEOS-CHEM global transport model to the aircraft profiles acquired over Alaska during NASA's Carbon in Arctic Reservoirs Vulnerability Experiment (2012-2015). We use the empirical biome-specific linear relationship between OCS plant uptake flux and GPP to derive the six plant uptake OCS fluxes from different GPP data. Such GPP-based fluxes are used to drive the concentration simulations. We evaluate the simulations against the independent observations at two ground sites of Alaska. The optimized OCS fluxes suggest the NHL plant uptake OCS flux of -247 Gg S year

Understanding the sources and sinks of CH4 is critical to both predicting and mitigating future climate change. There are large uncertainties in the global budget of atmospheric CH4, but natural emissions are estimated to be of a similar magnitude to total anthropogenic emissions. The largest sources of uncertainty in scaling bottom-up CH4 estimates stem from limited ground-based measurements and the misalignment between drivers of CH4 fluxes and current land use classifications. To understand the CH4 flux potential of natural ecosystems and agricultural lands in the United States (US) of America, a multi-scale CH4 observation network focused on CH4 flux rates, processes, and scaling methods is required. This can be achieved with a network of ground-based observations that are distributed based on climatic regions and landcover. To determine the gaps in physical infrastructure for developing this network, we need to understand the representativeness of current measurements. We focus here on eddy covariance (EC) flux towers because they are essential for a bottom-up framework that bridges the gap between point-based chamber measurements and airborne or satellite platforms, informing the remote sensing and modelling communities and policy decisions, all the way to IPCC reports. Using multidimensional scaling and a cluster analysis, the US was divided into 10 clusters that were distributed across temperature and wetness gradients. We evaluated the distance to the medoid condition within each cluster for research sites with EC tower infrastructure to identify the gaps in existing infrastructure that limit our ability to constrain the contribution of US biogenic CH4 emissions to the global budget. These gaps occurred across all EC flux tower networks and independently managed sites as well as in some environmental clusters. Through our analysis using climate, land cover, and location variables, we have identified priority areas to target for research infrastructure to provide a more complete understanding of the CH4 flux potential of ecosystem types across the US.