Tg Yr Research Articles

Dissolved Nitrous Oxide and Methane in the Taiwan Strait: Distribution, Seasonal Variation, and Emission

AbstractThe global ocean plays an important role in the overall budgets of nitrous oxide (N2O) and methane (CH4), especially in continental estuaries and shelf areas. Four cruises were conducted between 2021 and 2022, covering the spring, summer, and fall seasons, to study the spatial and seasonal characteristics of N2O and CH4 distributions and emissions in the Taiwan Strait (TWS). The surface N2O and CH4 concentrations gradually decreased from the coast to the open sea, with maximum values (14.3 and 15.6 nmol L−1) occurring near the Jiulong and Minjiang estuaries, respectively. The mean surface N2O concentration (8.2 nmol L−1) was highest in the spring and approximately the same in the summer as in the fall. The mean surface concentrations of CH4 (8.8 nmol L−1) were greater in summer than in spring and fall, probably because of the high freshwater input in summer. Except for several stations in fall, surface waters were oversaturated with N2O and CH4 relative to the atmosphere in other seasons, and the TWS was a net source of atmospheric N2O and CH4 in the spring, summer, and fall. In situ production is the main source of N2O and CH4 in the TWS, with nitrification being the dominant mechanism of N2O production in the TWS. In contrast, physical influences (riverine inputs and water mass mixing) reshape the distributions of N2O and CH4. The annual emissions of N2O and CH4 from the TWS were estimated to be 0.9 × 10−3 ± 2.9 × 10−3 Tg yr−1 and 1.6 × 10−3 ± 3.0 × 10−3 Tg yr−1, respectively. Taken together, the TWS accounts for 0.025% of the surface area of the world's oceans and 0.022% ± 0.07% and 0.017% ± 0.033% of global oceanic N2O and CH4 emissions, respectively.

Estimation of carbon sequestration potential and air quality impacts of biochar production from straw in China

Aiming to optimize straw resource utilization and to reduce air pollutant and greenhouse gas emissions in China, the environmental benefits of biochar production using straw and utilization need to be assessed. Two biochar production scenarios were studied: centralized production scenario (CPS) utilizing an industrialized production method with advanced air pollution control devices, and decentralized production scenario (DPS) based on a distributed production method of biochar at the village level, compared to an open-burning scenario (OBS). The potential GHG emission reductions under DPS, including the benefit of soil biochar application, were evaluated as 680 Tg CO2-eq yr-1, which was lower than the reductions under CPS (780 Tg CO2-eq yr-1). Although the attentional centralized production method of biochar has more potential environmental benefits, at present the distributed production method is more practical in China due to its convenience, management ease, and lower costs. Modeling on air quality in China showed that in comparison with OBS, DPS could reduce the average monthly PM2.5 concentration of key regions by 19%, and about 190 Tg yr-1 biochar could be produced with 150 Tg C yr-1 sequestered in biochar. Our findings support widespread biochar use in China for improved air quality and climate neutrality.

Identifying and filling critical knowledge gaps can optimize financial viability of blue carbon projects in tidal wetlands

One of the world’s largest “blue carbon” ecosystems, Louisiana’s tidal wetlands on the US Gulf of Mexico coast, is rapidly being lost. Louisiana’s strong legal, regulatory, and monitoring framework, developed for one of the world’s largest tidal wetland systems, provides an opportunity for a programmatic approach to blue carbon accreditation to support restoration of these ecologically and economically important tidal wetlands. Louisiana’s coastal wetlands span ∼1.4 million ha and accumulate 5.5–7.3 Tg yr−1 of blue carbon (organic carbon), ∼6%–8% of tidal marsh blue carbon accumulation globally. Louisiana has a favorable governance framework to advance blue carbon accreditation, due to centralized restoration planning, long term coastal monitoring, and strong legal and regulatory frameworks around carbon. Additional restoration efforts, planned through Louisiana’s Coastal Master Plan, over 50 years are projected to create, or avoid loss of, up to 81,000 ha of wetland. Current restoration funding, primarily from Deepwater Horizon oil spill settlements, will be fully committed by the early 2030s and additional funding sources are required. Existing accreditation methodologies have not been successfully applied to coastal Louisiana’s ecosystem restoration approaches or herbaceous tidal wetland types. Achieving financial viability for accreditation of these restoration and wetland types will require expanded application of existing blue carbon crediting methodologies. It will also require expanded approaches for predicting the future landscape without restoration, such as numerical modeling, to be validated. Additional methodologies (and/or standards) would have many common elements with those currently available but may be beneficial, depending on the goals and needs of both the state of Louisiana and potential purchasers of Louisiana tidal wetland carbon credits. This study identified twenty targeted needs that will address data and knowledge gaps to maximize financial viability of blue carbon accreditation for Louisiana’s tidal wetlands. Knowledge needs were identified in five categories: legislative and policy, accreditation methodologies and standards, soil carbon flux, methane flux, and lateral carbon flux. Due to the large spatial scale and diversity of tidal wetlands, it is expected that progress in coastal Louisiana has high potential to be generalized to similar wetland ecosystems across the northern Gulf of Mexico and globally.

Modeling the contribution of leads to sea spray aerosol in the high Arctic

Abstract. Elongated open-water areas in sea ice (leads) release sea spray particles to the atmosphere. However, there is limited knowledge on the amount, properties and drivers of sea spray emitted from leads, and no existing parameterization of this process is available for use in models. In this work, we use measurements of aerosol fluxes from Nilsson et al. (2001) to produce an estimate of the location, timing and amount of sea spray emissions from leads at the scale of the Arctic Ocean for 1 year. Lead fractions are derived using sea ice data sets from numerical models and satellite detection. The proposed parameterization estimates that leads account for 0.3 %–9.8 % of the annual sea salt aerosol number emissions in the Arctic Ocean regions where sea ice concentration is greater than 80 %. Assuming similar size distributions to those from emissions from the open ocean, leads account for 30 %–85 % of mass emissions in sea ice regions. The total annual mass of sea salt emitted from leads, 0.1–2.1 Tg yr−1, is comparable to the mass of sea salt aerosol transported above sea ice from the open ocean, according to the MERRA-2 reanalysis. In addition to providing the first estimates of possible upper and lower bounds of sea spray emissions from leads, the conceptual model developed in this work is implemented and tested in the regional atmospheric chemistry model WRF-Chem. Given the estimates obtained in this work, the impact of sea spray from leads on Arctic clouds and radiative budget needs to be further explored.

Ammonia emission estimates using CrIS satellite observations over Europe

Abstract. Over the past century, ammonia (NH3) emissions have increased with the growth of livestock and fertilizer usage. The abundant NH3 emissions lead to secondary fine particulate matter (PM2.5) pollution, climate change, and a reduction in biodiversity, and they affect human health. Up-to-date and spatially and temporally resolved information on NH3 emissions is essential to better quantify their impact. In this study we applied the existing Daily Emissions Constrained by Satellite Observations (DECSO) algorithm to NH3 observations from the Cross-track Infrared Sounder (CrIS) to estimate NH3 emissions. Because NH3 in the atmosphere is influenced by nitrogen oxides (NOx), we implemented DECSO to estimate NOx and NH3 emissions simultaneously. The emissions are derived over Europe for 2020 on a spatial resolution of 0.2°×0.2° using daily observations from both CrIS and the TROPOspheric Monitoring Instrument (TROPOMI; on the Sentinel-5 Precursor (S5P) satellite). Due to the limited number of daily satellite observations of NH3, monthly emissions of NH3 are reported. The total NH3 emissions derived from observations are about 8 Tg yr−1, with a precision of about 5 %–17 % per grid cell per year over the European domain (35–55° N, 10° W–30° E). The comparison of the satellite-derived NH3 emissions from DECSO with independent bottom-up inventories and in situ observations indicates a consistency in terms of magnitude on the country totals, with the results also being comparable regarding the temporal and spatial distributions. The validation of DECSO over Europe implies that we can use DECSO to quickly derive fairly accurate monthly emissions of NH3 over regions with limited local information on NH3 emissions.

Physical and practical constraints on atmospheric methane removal technologies

Abstract Despite their apparent utility in mitigating climate change, technologies for removing methane from air are in early stages of development. Here we evaluate the limiting physical constraints, for three types of systems: two- and three-dimensional infrastructure and atmospheric oxidation enhancement, focusing on removing low ( x CH4 < 1000 ppm) and ambient ( x CH4 < 2 ppm) methane from air. With the space velocities and removal efficiencies of current three-dimensional technologies, volumes of 7–350 km3 are required to remove 1 Tg CH4 yr−1. Two-dimensional solutions are limited by the transport rate of methane to a surface. If every molecule of methane that collides with the surface is removed, an area of 1130 km2 is needed to remove 1 Tg CH4 yr−1 at ambient concentration. However, research shows that per-collision reaction probabilities are < 10−8 requiring a surface area of 1010–1015 km2. Finally, we examine atmospheric oxidation enhancement, where 4.8 Tg yr−1 of Cl ⋅ or 8.8 Tg yr−1 of OH ⋅ is required to remove 1 Tg CH4 yr−1, with precursors such as H2O2 or O3. However, limitations arise concerning multiple environmental impacts. We conclude that the physical and practical constraints are considerable, and identify the main barriers that must be addressed.

Wet depositional fluxes of fossil fuel-derived carbon in East Asia: Dynamics of Brown carbon

Over the past 50 years, fossil fuel consumption has increased dramatically, rising approximately eight-fold since 1950 and doubling since 1980. This surge has led to increased emissions of brown carbon (BrC) into the atmosphere, which are subsequently deposited onto oceans and land through dry or wet deposition processes. However, the source-specific fluxes of atmospheric organic carbon (OC) and BrC into the ocean are not adequately represented in the global carbon cycle. For the first time, we calculated BrC concentration using the optical intensity of organic matter and determined the global wet depositional flux of fossil fuel-derived BrC. Using the ratio of humic-like substances to OC fluxes, we estimated the global wet deposition of fossil fuel-derived BrC to be 2.0 ± 0.6 Tg C yr−1. Of this amount, the flux into oceans (0.7 ± 0.2 Tg C yr−1) represents 1.6% of the production rate of refractory dissolved organic carbon (RDOC) in the ocean (43 Tg yr−1). Notably, an increase in the proportion of fossil fuel-derived BrC in atmospheric OC may change the composition of OC in precipitation, resulting in a more refractory composition, which deviates from previously established paradigms. Our findings indicate that the flux of fossil fuel-derived RDOC from the atmosphere into the ocean, which is inadequately represented in current global DOC cycling models, may play a significant role in oceanic carbon cycles. These findings necessitate reconsidering our understanding of oceanic carbon cycling and highlight the need to improve existing models to better account for these newly identified processes and their potential impacts on global carbon dynamics.

Long-term changes of methane emissions from rice cultivation during 2000 – 2060 in China: Trends, driving factors, predictions and policy implications

Regional budget assessments of methane (CH4) are critical for future climate and environmental management. CH4 emissions from rice cultivation (CH4-rice) constitute one of the most significant sources. However, previous studies mainly focus on historical emission estimates and lack consideration of future changes in CH4-rice under climate change or anthropogenic policy intervention, which hampers our understanding of long-term trends and the implementation of targeted emission reduction efforts. This study investigates the spatiotemporal variations of CH4-rice over the past two decades, using an integrated method to identify the major drivers and predict future emissions under climate change scenarios and policy perspectives. Results indicate that the CH4-rice emissions in China ranged between 6.21 and 6.57 Tg yr−1 over the past two decades, with a spatial distribution characterized by decreases in the south and increases in the north, associated with economic development, dietary shifts, technological advancements, and climate change. Factors such as the rate of straw added (RSA), fertilization, soil texture, temperature, and precipitation significantly influence CH4 emissions per unit rice production (CH4-urp), with RSA identified as the most significant tillage management factor, explaining 32 % of the variance. Lowering RSA to 8 % is beneficial for reducing CH4-urp. Scenario analysis indicates that under policies focusing on production or demand, CH4-rice is expected to increase by 0.3 % to 5.6 %, while adjusting RSA can reduce CH4-rice by 9.4 % to 10.0 %. Structural adjustments and regional cooperation serve as beneficial starting points for controlling and reducing CH4-rice in China, while optimizing industrial layouts contributes to regional development and CH4-rice control. Implementing policies related to maintaining field and crop yields can achieve a balance between rice supply and demand ahead of schedule. Dynamic adjustment of rice cultivation based on supply–demand balance can effectively reduce CH4-rice from excess rice production. By 2060, the reduction effect could reach 8.95 %–12.01 %. Introducing policy-driven tillage management measures as reference indicators facilitates the reduction of CH4-rice.

Glacial troughs as centres of organic carbon accumulation on the Norwegian continental margin

The role of continental margin sediments in the carbon cycle and the associated management potential for climate mitigation are currently poorly understood. Previous work has indicated that margin sediments store significant amounts of organic carbon, but few studies have quantified the rates at which organic carbon is accumulated. Here, we use machine learning to make spatial predictions of the organic carbon stocks and accumulation rates of sediments on the Norwegian continental margin. We show that surface sediments (upper 10 cm) store 814 Tg and accumulate 6 Tg yr−1 of organic carbon. Shelf-incised glacial troughs account for 39% of the stocks and 48% of the accumulation, with the main accumulation hotspot located in the Skagerrak. Continental margin sediments accumulate organic carbon at scales much larger than vegetated coastal ecosystems in Norway because of their larger extent. Future studies should explore to what extent management interventions could increase accumulation rates, e.g., by minimising anthropogenic disturbance of seafloor sediments.

Increasing Methane Emissions and Widespread Cold‐Season Release From High‐Arctic Regions Detected Through Atmospheric Measurements

AbstractRising Arctic temperatures pose a threat to the large carbon stores trapped in Arctic permafrost. To assess methane emissions in high‐Arctic regions, we analyzed atmospheric data from Alaska and Siberia using two methods: (a) a wind sector approach to calculate emission changes based on concentration enhancements using wind direction, and (b) an inversion method utilizing a high‐resolution atmospheric transport model. Incorporating data after 2015, we observed a significant rise in methane emissions (0.018 ± 0.005 Tg yr−2 from 2000 to 2021) from Alaska's North Slope, indicating a shift from previous analyses. We find 34%–50% of yearly emissions occurred in the late season (September–December) consistently across multiple years and regions, which is historically underestimated in models and inventories. Our findings reveal significant changes occurring in the Arctic, highlighting the crucial role of long‐term atmospheric measurements in monitoring the region, especially during the cold season.

Importance of microphysical settings for climate forcing by stratospheric SO2 injections as modeled by SOCOL-AERv2

Abstract. Solar radiation modification by a sustained deliberate source of SO2 into the stratosphere (strat-SRM) has been proposed as an option for climate intervention. Global interactive aerosol–chemistry–climate models are often used to investigate the potential cooling efficiencies and associated side effects of hypothesized strat-SRM scenarios. A recent model intercomparison study for composition–climate models with interactive stratospheric aerosol suggests that the modeled climate response to a particular assumed injection strategy depends on the type of aerosol microphysical scheme used (e.g., modal or sectional representation) alongside host model resolution and transport. Compared to short-duration volcanic SO2 emissions, the continuous SO2 injections in strat-SRM scenarios may pose a greater challenge to the numerical implementation of microphysical processes such as nucleation, condensation, and coagulation. This study explores how changing the time steps and sequencing of microphysical processes in the sectional aerosol–chemistry–climate model SOCOL-AERv2 (40 mass bins) affects model-predicted climate and ozone layer impacts considering strat-SRM by SO2 injections of 5 and 25 Tg(S) yr−1 at 20 km altitude between 30° S and 30° N. The model experiments consider the year 2040 to be the boundary conditions for ozone-depleting substances and greenhouse gases (GHGs). We focus on the length of the microphysical time step and the call sequence of nucleation and condensation, the two competing sink processes for gaseous H2SO4. Under stratospheric background conditions, we find no effect of the microphysical setup on the simulated aerosol properties. However, at the high sulfur loadings reached in the scenarios injecting 25 Tg(S) yr−1 of SO2 with a default microphysical time step of 6 min, changing the call sequence from the default “condensation first” to “nucleation first” leads to a massive increase in the number densities of particles in the nucleation mode (R<0.01 µm) and a small decrease in coarse-mode particles (R>1 µm). As expected, the influence of the call sequence becomes negligible when the microphysical time step is reduced to a few seconds, with the model solutions converging to a size distribution with a pronounced nucleation mode. While the main features and spatial patterns of climate forcing by SO2 injections are not strongly affected by the microphysical configuration, the absolute numbers vary considerably. For the extreme injection with 25 Tg(S) yr−1, the simulated net global radiative forcing ranges from −2.3 to −5.3 W m−2, depending on the microphysical configuration. Nucleation first shifts the size distribution towards radii better suited for solar scattering (0.3 µm <R< 0.4 µm), enhancing the intervention efficiency. The size distribution shift, however, generates more ultrafine aerosol particles, increasing the surface area density and resulting in 10 DU (Dobson units) less ozone (about 3 % of the total column) in the northern mid-latitudes and 20 DU less ozone (6 %) over the polar caps compared to the condensation first approach. Our results suggest that a reasonably short microphysical time step of 2 min or less must be applied to accurately capture the magnitude of the H2SO4 supersaturation resulting from SO2 injection scenarios or volcanic eruptions. Taken together, these results underscore how structural aspects of model representation of aerosol microphysical processes become important under conditions of elevated stratospheric sulfur in determining atmospheric chemistry and climate impacts.

Quantifying CH4 emissions from coal mine aggregation areas in Shanxi, China, using TROPOMI observations and the wind-assigned anomaly method

Abstract. China stands out as a major contributor to anthropogenic methane (CH4) emissions, with coal mine methane (CMM) playing a crucial role. To control and reduce CH4 emissions, China has made a dedicated commitment and formulated an ambitious mitigation plan. To verify the progress made, the consistent acquisition of independent CH4 emission data is required. This paper aims to implement a wind-assigned anomaly method for the precise determination of regional-scale CMM emissions within the coal-rich Shanxi province. We use the TROPOspheric Monitoring Instrument (TROPOMI) CH4 observations from May 2018 to May 2023, coupled with ERA5 wind and a bottom-up inventory dataset based on the IPCC (Intergovernmental Panel on Climate Change) Tier 2 approach covering the Changzhi, Jincheng, and Yangquan regions of the Shanxi province. The derived emission strengths are 8.4 × 1026 molec. s−1 (0.706 Tg yr−1, ±25 %), 1.4 × 1027 molec. s−1 (1.176 Tg yr−1, ±20 %), and 4.9 × 1026 molec. s−1 (0.412 Tg yr−1, ±21 %), respectively. Our results exhibit biases of −18 %, 8 %, and 14 %, respectively, when compared to the IPCC Tier 2 bottom-up inventory. Larger discrepancies are found when comparing the estimates to the Copernicus Atmosphere Monitoring Service global anthropogenic emissions (CAMS-GLOB-ANT) and Emissions Database for Global Atmospheric Research (EDGARv7.0) inventories (64 %–176 %), suggesting that the two inventories may be overestimating CH4 emissions from the studied coal mining regions. Our estimates provide a comprehensive characterization of the regions within the Shanxi province, contribute to the validation of emission inventories, and provide additional insights into CMM emission mitigation.

Dependency of the impacts of geoengineering on the stratospheric sulfur injection strategy – Part 2: How changes in the hydrological cycle depend on the injection rate and model used

Abstract. This is the second of two papers in which we study the dependency of the impacts of stratospheric sulfur injections on the model and injection strategy used. Here, aerosol optical properties from simulated stratospheric aerosol injections using two aerosol models (modal scheme M7 and sectional scheme SALSA), as described in Part 1 (Laakso et al., 2022), are implemented consistently into the EC-Earth, MPI-ESM and CESM Earth system models (ESMs) to simulate the climate impacts of different injection rates ranging from 2 to 100 Tg(S) yr−1. Two sets of simulations were run with the three ESMs: (1) regression simulations, in which an abrupt change in CO2 concentration or stratospheric aerosols over pre-industrial conditions was applied to quantify global mean fast temperature-independent climate responses and quasi-linear dependence on temperature, and (2) equilibrium simulations, in which radiative forcing of aerosol injections with various magnitudes compensated for the corresponding radiative forcing of CO2 enhancement to study the dependence of precipitation on the injection magnitude. The latter also allow one to explore the regional climatic responses. Large differences in SALSA- and M7-simulated radiative forcing in Part 1 translated into large differences in the estimated surface temperature and precipitation changes in ESM simulations; for example, an injection rate of 20 Tg(S) yr−1 in CESM using M7-simulated aerosols led to only 2.2 K global mean cooling, while EC-Earth–SALSA combination produced a 5.2 K change. In equilibrium simulations, where aerosol injections were utilized to offset the radiative forcing caused by an atmospheric CO2 concentration of 500 ppm, the decrease in global mean precipitation varied among models, ranging from −0.7 % to −2.4 % compared with the pre-industrial climate. These precipitation changes can be explained by the fast precipitation response due to radiation changes caused by the stratospheric aerosols and CO2, as the global mean fast precipitation response is shown to be negatively correlated with global mean atmospheric absorption. Our study shows that estimating the impact of stratospheric aerosol injection on climate is not straightforward. This is because the simulated capability of the sulfate layer to reflect solar radiation and absorb long-wave radiation is sensitive to the injection rate as well as the aerosol model used to simulate the aerosol field. These findings emphasize the necessity for precise simulation of aerosol microphysics to accurately estimate the climate impacts of stratospheric sulfur intervention. This study also reveals gaps in our understanding and uncertainties that still exist related to these controversial techniques.

Regional to global distributions, trends, and drivers of biogenic volatile organic compound emission from 2001 to 2020

Abstract. Biogenic volatile organic compounds (BVOCs) are important precursors to ozone and secondary organic aerosols in the atmosphere, affecting air quality, clouds, and climate. However, the trend in BVOC emissions and driving factors for the emission changes in different geographic regions over the past 2 decades has remained unclear. Here, regional to global changes in BVOC emissions during 2001–2020 are simulated using the latest Model of Emission of Gases and Aerosols from Nature (MEGANv3.2) with the input of time-varying satellite-retrieved vegetation and reanalysis meteorology data. Comparison of model simulations with the site observations shows that the model can reasonably reproduce the magnitude of isoprene and monoterpene emission fluxes. The spatial distribution of the modeled isoprene emissions is generally comparable to the satellite retrievals. The estimated annual average global BVOC emissions are 835.4 Tg yr−1 with the emissions from isoprene, monoterpenes, sesquiterpenes, and other BVOC comprised of 347.7, 184.8, 23.3, and 279.6 Tg yr−1, respectively. We find that the decrease in global isoprene emissions (−0.07 % per year) caused by the increase in CO2 concentrations (−0.20 % per year) is stronger than that caused by changes in vegetation (−0.03 % per year) and meteorological factors (0.15 % per year). However, regional disparities are large. Isoprene emissions increase significantly in Europe, East Asia, and South Asia (0.37 % per year–0.66 % per year). Half of the increasing trend is contributed by increased leaf area index (LAI) (maximum over 0.02 m2 m−2 yr−1) and tree cover. Changes in meteorological factors contribute to another half, with elevated temperature dominating in Europe and increased soil moisture dominating in East and South Asia. In contrast, in South America and Southeast Asia, shifts in vegetation type associated with the BVOC emission capacity, which partly results from the deforestation and agricultural expansion, decrease the BVOC emission and offset nearly half of the emission increase caused by changes in meteorological factors. Overall, isoprene emission increases by 0.35 % per year and 0.25 % per year in South America and Southeast Asia, respectively. In Central Africa, a decrease in temperature dominates the negative emission trend (−0.74 % per year). Global monoterpene emissions show a significantly increasing trend (0.34 % per year, 0.6 Tg yr−1) compared to that of isoprene (−0.07 % per year, −0.2 Tg yr−1), especially in strong greening hotspots. This is mainly because the monoterpene emissions are more sensitive to changes in LAI and are not subject to the inhibition effect of CO2. The findings highlight the important roles of vegetation cover and biomass, temperature, and soil moisture in modulating the temporal variations of global BVOC emissions in the past 2 decades.

European CH4 inversions with ICON-ART coupled to the CarbonTracker Data Assimilation Shell

Abstract. We present the first application of the ICOsahedral Nonhydrostatic model with Aerosols and Reactive Trace gases (ICON-ART) in inverse modeling in inverse modeling of greenhouse gas fluxes with an ensemble Kalman smoother. For this purpose, we extended ICON-ART to efficiently handle gridded emissions, generate an ensemble of perturbed emissions during runtime and use nudging on selected variables to keep the simulations close to analyzed meteorology. We show that the system can optimize total and anthropogenic European CH4 fluxes on a national scale in an idealized setup using pseudo-observations from a realistic network of measurement stations. However, we were unable to constrain the sum of the natural emission sources of comparatively low magnitude. Also regions with low emissions and regions with low observational coverage could not be optimized individually for lack of observational constraints. Furthermore, we investigated the sensitivities towards different inversion parameters and design choices with 15 sensitivity runs using the same idealized setup, demonstrating the robustness of the approach when regarding some minimal requirements of the setup (e.g., number of ensemble members). Subsequently, we applied the system to real in situ observations from 28 European stations for three years, 2008, 2013 and 2018. We used a priori anthropogenic fluxes from the EDGARv6 inventory and a priori natural fluxes from peatlands and mineral soils, inland waters, the ocean, biofuels and biomass burning, and geology. Our results for the year 2018 indicate that anthropogenic emissions may be underestimated in EDGARv6 by ca. 25 % in the Benelux countries and, to a smaller degree, in northwestern France and southern England. In the rest of the domain, anthropogenic fluxes are corrected downwards by the inversion, suggesting an overestimation in the a priori. For most countries, this means that the a posteriori country-total anthropogenic emissions are closer to the values reported to the United Nations Framework Convention on Climate Change (UNFCCC) than the a priori emissions from EDGARv6. Aggregating the a posteriori emissions across the EU27 + UK results in a total of 17.4 Tg yr−1, while the a priori emissions were 19.9 Tg yr−1. Our a posteriori is close to the total reported to the UNFCCC of 17.8 Tg yr−1. Natural emissions are reduced from their a priori magnitude almost everywhere, especially over Italy and Romania–Moldova, where a priori geological emissions are high, and over the United Kingdom and Scandinavia, where emissions from peatlands and wetlands were possibly unusually low during the hot and dry summer of 2018. Our a posteriori anthropogenic emissions for the EU27 + UK fall within the range estimated by global top-down studies but are lower than most other regional inversions. However, many of these studies have used observations from different measurement stations or satellite observations. The spatial pattern of the emission increments in our results, especially the increase in the Benelux countries, also agrees well with other regional inversions.

Molecular analysis of secondary organic aerosol and brown carbon from the oxidation of indole

Abstract. Indole (ind) is a nitrogen-containing heterocyclic volatile organic compound commonly emitted from animal husbandry and from different plants like maize with global emissions of 0.1 Tg yr−1. The chemical composition and optical properties of indole secondary organic aerosol (SOA) and brown carbon (BrC) are still not well understood. To address this, environmental chamber experiments were conducted to investigate the oxidation of indole at atmospherically relevant concentrations of selected oxidants (OH radicals and O3) with or without NO2. In the presence of NO2, the SOA yields decreased by more than a factor of 2, but the mass absorption coefficient at 365 nm (MAC365) of ind-SOA was 4.3 ± 0.4 m2 g−1, which was 5 times higher than that in experiments without NO2. In the presence of NO2, C8H6N2O2 (identified as 3-nitroindole) contributed 76 % to all organic compounds detected by a chemical ionization mass spectrometer, contributing ∼ 50 % of the light absorption at 365 nm (Abs365). In the absence of NO2, the dominating chromophore was C8H7O3N, contributing to 20 %–30 % of Abs365. Indole contributes substantially to the formation of secondary BrC and its potential impact on the atmospheric radiative transfer is further enhanced in the presence of NO2, as it significantly increases the specific light absorption of ind-SOA by facilitating the formation of 3-nitroindole. This work provides new insights into an important process of brown carbon formation by interaction of two pollutants, NO2 and indole, mainly emitted by anthropogenic activities.

Country-level methane emissions and their sectoral trends during 2009–2020 estimated by high-resolution inversion of GOSAT and surface observations

Considering the significant role of global methane emissions in the Earth’s radiative budget, global or regionally persistent increasing trends in its emission are of great concern. Understanding the regional contributions of various emissions sectors to the growth rate thus has policy relevance. We used a high-resolution global methane inverse model to independently optimize sectoral emissions using GOSAT and ground-based observations for 2009–2020. Annual emission trends were calculated for top-emitting countries, and the sectoral contributions to the total anthropogenic trend were studied. Global total posterior emissions show a growth rate of 2.6 Tg yr−2 (p < 0.05), with significant contributions from waste (1.1 Tg yr−2) and agriculture (0.9 Tg yr−2). Country-level aggregated sectoral emissions showed statistically significant (p < 0.1) trends in total posterior emissions for China (0.56 Tg yr−2), India (0.22 Tg yr−2), United States (0.65 Tg yr−2), Pakistan (0.22 Tg yr−2) and Indonesia (0.28 Tg yr−2) among the top methane emitters. Emission sectors contributing to the above country-level emission trend are, China (waste 0.35; oil and gas 0.07 Tg yr−2), India (agriculture 0.09; waste 0.11 Tg yr−2), United States (oil and gas 1.0; agriculture 0.07; coal −0.15 Tg yr−2), Brazil (waste 0.09; agriculture 0.08 Tg yr−2), Russia (waste 0.04; biomass burning 0.15; coal 0.11; oil and gas −0.42 Tg yr−2), Indonesia (coal 0.28 Tg yr−2), Canada (oil and gas 0.08 Tg yr−2), Pakistan (agriculture 0.15; waste 0.03 Tg yr−2) and Mexico (waste 0.04 Tg yr−2). Additionally, our analysis showed that methane emissions from wetlands in Russia (0.24 Tg yr−2) and central African countries such as Congo (0.09 Tg yr−2), etc. have a positive trend with a considerably large increase after 2017, whereas Bolivia (−0.09 Tg yr−2) have a declining trend. Our results reveal some key emission sectors to be targeted on a national level for designing methane emission mitigation efforts.

Salinity causes widespread restriction of methane emissions from small inland waters

Inland waters are one of the largest natural sources of methane (CH4), a potent greenhouse gas, but emissions models and estimates were developed for solute-poor ecosystems and may not apply to salt-rich inland waters. Here we combine field surveys and eddy covariance measurements to show that salinity constrains microbial CH4 cycling through complex mechanisms, restricting aquatic emissions from one of the largest global hardwater regions (the Canadian Prairies). Existing models overestimated CH4 emissions from ponds and wetlands by up to several orders of magnitude, with discrepancies linked to salinity. While not significant for rivers and larger lakes, salinity interacted with organic matter availability to shape CH4 patterns in small lentic habitats. We estimate that excluding salinity leads to overestimation of emissions from small Canadian Prairie waterbodies by at least 81% ( ~ 1 Tg yr−1 CO2 equivalent), a quantity comparable to other major national emissions sources. Our findings are consistent with patterns in other hardwater landscapes, likely leading to an overestimation of global lentic CH4 emissions. Widespread salinization of inland waters may impact CH4 cycling and should be considered in future projections of aquatic emissions.

Weekly derived top-down volatile-organic-compound fluxes over Europe from TROPOMI HCHO data from 2018 to 2021

Abstract. Volatile organic compounds (VOCs) are key precursors of particulate matter and tropospheric ozone. Although the terrestrial biosphere is by far the largest source of VOCs into the atmosphere, the emissions of biogenic VOCs remain poorly constrained at the regional scale. In this work, we derive top-down biogenic emissions over Europe using weekly averaged TROPOMI formaldehyde (HCHO) data from 2018 to 2021. The systematic bias of the TROPOMI HCHO columns is characterized and corrected for based on comparisons with FTIR data at seven European stations. The top-down fluxes of biogenic, pyrogenic, and anthropogenic VOC sources are optimized using an inversion framework based on the MAGRITTEv1.1 chemistry transport model and its adjoint. The inversion leads to strongly increased isoprene emissions with respect to the MEGAN–MOHYCAN inventory over the model domain (from 8.1 to 18.5 Tg yr−1), which is driven by the high observed TROPOMI HCHO columns in southern Europe. The impact of the inversion on biomass burning VOCs (+13 %) and anthropogenic VOCs (−17 %) is moderate. An evaluation of the optimized HCHO distribution against ground-based remote sensing (FTIR and MAX-DOAS) and in situ data provides generally improved agreement at stations below about 50∘ N but indicates overestimated emissions in northern Scandinavia. Sensitivity inversions show that the top-down emissions are robust with respect to changes in the inversion settings and in the model chemical mechanism, leading to differences of up to 10 % in the total emissions. However, the top-down emissions are very sensitive to the bias correction of the observed columns, as the biogenic emissions are 3 times lower when the correction is not applied. Furthermore, the use of different a priori biogenic emissions has a significant impact on the inversion results due to large differences among bottom-up inventories. The sensitivity run using CAMS-GLOB-BIOv3.1 as a priori emissions in the inversion results in 30 % lower emissions with respect to the optimization using MEGAN–MOHYCAN. In regions with large temperature and cloud cover variations, there is strong week-to-week variability in the observed HCHO columns. The top-down emissions, which are optimized at weekly increments, have a much improved capability of representing these large fluctuations than an inversion using monthly increments.

Enhanced dataset of global marine isoprene emissions from biogenic and photochemical processes for the period 2001–2020

Abstract. Isoprene is a crucial non-methane biogenic volatile organic compound (BVOC) that exhibits the largest emissions globally. It is chemically reactive in the atmosphere and serves as the primary source of generating secondary organic aerosols (SOA) in terrestrial and remote marine regions. However, a comprehensive estimation of marine isoprene emissions is currently lacking. Here we built a module to present a 20-year (2001–2020) global hourly dataset for marine isoprene emissions, including phytoplankton-generated biological emissions (BIO emissions) and photochemistry-generated emissions in the sea surface microlayer (SML emissions) based on the latest advancements in biological, physical, and chemical processes, with high spatial resolutions. Our dataset suggests the annual global marine isoprene emissions amount to 1.097±0.009 Tg yr−1. Among these, the BIO emissions are 0.481±0.008 Tg yr−1 while SML emissions contribute 0.616±0.003 Tg yr−1. The ability of this module to estimate marine isoprene emissions was evaluated through comparison with a series of observations of marine isoprene concentrations and emission fluxes. The annual total isoprene emissions across the tropical ocean show a declining trend from 2001 to 2020. Most ocean regions exhibit a 1-year emission period, whereas a significant intraseasonal period is found in the tropical ocean. This dataset can be employed as input for the simulation of marine SOA formation in earth system models. This work provides the foundation for further studies into the impact of the air–sea system on marine SOA formation and its climate effect. The DOI link for the dataset is https://doi.org/10.11888/Atmos.tpdc.300521 (Cui and Zhu, 2023).