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All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Observationally constrained analysis of sulfur cycle in the marine atmosphere with NASA ATom measurements and AeroCom model simulations

The atmospheric sulfur cycle plays a key role in air quality, climate, and ecosystems, such as pollution, radiative forcing, new particle formation, and acid rain. In this study, we compare the spatially and temporally resolved measurements from the NASA Atmospheric Tomography (ATom) mission with simulations from five AeroCom III models for four sulfur species (dimethyl sulfide (DMS), sulfur dioxide (SO 2 ), particulate methanesulfonate (MSA), and particulate sulfate (SO 4 )). We focus on remote regions over the Pacific, Atlantic, and Southern oceans from near the surface to ~12 km altitude range covering all four seasons. In general, the differences among model results can be greater than 1 order of magnitude. Comparing with observations, model-simulated SO 2 is generally low, whereas SO 4 is generally high. Simulated DMS concentrations near the sea surface exceed observed levels by a factor of 5 in most cases, suggesting potential overestimation of DMS emissions in all models. With GEOS model simulations of tagging emission from anthropogenic, biomass burning, volcanic, and oceanic sources, we find that anthropogenic emissions are the dominant source of sulfate aerosol (40 %–60 % of the total amount) in the ATom measurements at almost all altitudes, followed by volcanic emissions (18 %–32 %) and oceanic sources (16 %–32 %). Similar source contributions can also be derived at broad ocean basins and on monthly scales, indicating the representativeness of ATom measurements for global ocean. Our work presents the first assessment of AeroCom sulfur study using ATom measurements, providing directions for improving sulfate simulations, which remain the largest uncertainty in radiative forcing estimates in aerosol climate models.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Disentangling the mechanism of temperature and water vapor modulation on ozone under a warming climate

Temperature and water vapor have been considered as important factors affecting ozone concentrations, however, their synergistic effect on ozone, as well as its response to a warming climate remains unclear. Here, numerical experiments with different combinations of climate and emissions highlighted opposite changes of annual ozone over the contiguous U.S. under scenarios with high vs. low ozone precursor emissions in the future with warming. Comparing the occurrence of heat waves on higher vs. lower ozone days, we found significant suppression of the heat wave exacerbation of ozone by anthropogenic emissions reductions. Variations of ozone with temperature (T) and water vapor (Q) over the western U.S. and southeastern U.S. in the simulations are clearly revealed through the construction of an O 3 -T-Q diagram. Based on the diagram, we further identified a T-dominant regime at higher temperatures where ozone increases with temperature increase, and a Q-dominant regime at lower temperatures where ozone decreases with temperature increase due to the negative effect of water vapor. With larger anthropogenic emission reductions, ozone may increase at a lower rate with temperature in the T-dominant regime, or even decrease with temperature in the Q-dominant regime. Our results show that with large emission reductions, substantial ozone pollution due to warming and increasing heat waves may be counteracted by water vapor, partly turning the ‘climate penalty’ on ozone into ‘climate benefit’. Hence controlling anthropogenic emissions may be an increasingly important strategy in a warmer and wetter climate to improve air quality and public health.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Pan-Arctic seasonal cycles and long-term trends of aerosol properties from 10 observatories

Even though the Arctic is remote, aerosol properties observed there are strongly influenced by anthropogenic emissions from outside the Arctic. This is particularly true for the so-called Arctic haze season (January through April). In summer (June through September), when atmospheric transport patterns change, and precipitation is more frequent, local Arctic sources, i.e., natural sources of aerosols and precursors, play an important role. Over the last few decades, significant reductions in anthropogenic emissions have taken place. At the same time a large body of literature shows evidence that the Arctic is undergoing fundamental environmental changes due to climate forcing, leading to enhanced emissions by natural processes that may impact aerosol properties. In this study, we analyze 9 aerosol chemical species and 4 particle optical properties from 10 Arctic observatories (Alert, Kevo, Pallas, Summit, Thule, Tiksi, Barrow/Utgiavik, Villum, and Gruvebadet and Zeppelin Observatory – both at Ny-Ålesund Research Station) to understand changes in anthropogenic and natural aerosol contributions. Variables include equivalent black carbon, particulate sulfate, nitrate, ammonium, methanesulfonic acid, sodium, iron, calcium and potassium, as well as scattering and absorption coefficients, single scattering albedo and scattering Ångström exponent. First, annual cycles are investigated, which despite anthropogenic emission reductions still show the Arctic haze phenomenon. Second, long-term trends are studied using the Mann–Kendall Theil–Sen slope method. We find in total 41 significant trends over full station records, i.e., spanning more than a decade, compared to 26 significant decadal trends. The majority of significantly declining trends is from anthropogenic tracers and occurred during the haze period, driven by emission changes between 1990 and 2000. For the summer period, no uniform picture of trends has emerged. Twenty-six percent of trends, i.e., 19 out of 73, are significant, and of those 5 are positive and 14 are negative. Negative trends include not only anthropogenic tracers such as equivalent black carbon at Kevo, but also natural indicators such as methanesulfonic acid and non-sea-salt calcium at Alert. Positive trends are observed for sulfate at Gruvebadet. No clear evidence of a significant change in the natural aerosol contribution can be observed yet. However, testing the sensitivity of the Mann–Kendall Theil–Sen method, we find that monotonic changes of around 5 % yr –1 in an aerosol property are needed to detect a significant trend within one decade. This highlights that long-term efforts well beyond a decade are needed to capture smaller changes. It is particularly important to understand the ongoing natural changes in the Arctic, where interannual variability can be high, such as with forest fire emissions and their influence on the aerosol population. To investigate the climate-change-induced influence on the aerosol population and the resulting climate feedback, long-term observations of tracers more specific to natural sources are needed, as well as of particle microphysical properties such as size distributions, which can be used to identify changes in particle populations which are not well captured by mass-oriented methods such as bulk chemical composition.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Utilizing Earth Observations of Soil Freeze/Thaw Data and Atmospheric Concentrations to Estimate Cold Season Methane Emissions in the Northern High Latitudes

The northern wetland methane emission estimates have large uncertainties. Inversion models are a qualified method to estimate the methane fluxes and emissions in northern latitudes but when atmospheric observations are sparse, the models are only as good as their a priori estimates. Thus, improving a priori estimates is a competent way to reduce uncertainties and enhance emission estimates in the sparsely sampled regions. Here, we use a novel way to integrate remote sensing soil freeze/thaw (F/T) status from SMOS satellite to better capture the seasonality of methane emissions in the northern high latitude. The SMOS F/T data provide daily information of soil freezing state in the northern latitudes, and in this study, the data is used to define the cold season in the high latitudes and, thus, improve our knowledge of the seasonal cycle of biospheric methane fluxes. The SMOS F/T data is implemented to LPX-Bern DYPTOP model estimates and the modified fluxes are used as a biospheric a priori in the inversion model CarbonTracker Europe-CH 4 . The implementation of the SMOS F/T soil state is shown to be beneficial in improving the inversion model’s cold season biospheric flux estimates. Our results show that cold season biospheric CH4 emissions in northern high latitudes are approximately 0.60 Tg lower than previously estimated, which corresponds to 17% reduction in the cold season biospheric emissions. This reduction is partly compensated by increased anthropogenic emissions in the same area (0.23 Tg), and the results also indicates that the anthropogenic emissions could have even larger contribution in cold season than estimated here.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Corrigendum to “The Emissions Model Intercomparison Project (Emissions-MIP): quantifying model sensitivity to emission characteristics” published in Atmos. Chem. Phys., 23, 14779–14799, 2023

Anthropogenic emissions of aerosols and precursor compounds are known to significantly affect the energy balance of the Earth–atmosphere system, alter the formation of clouds and precipitation, and have a substantial impact on human health and the environment. Global models are an essential tool for examining the impacts of these emissions. In this study, we examine the sensitivity of model results to the assumed height of SO 2 injection, seasonality of SO 2 and black carbon (BC) particulate emissions, and the assumed fraction of SO 2 emissions that is injected into the atmosphere as particulate phase sulfate (SO 4 ) in 11 climate and chemistry models, including both chemical transport models and the atmospheric component of Earth system models. We find large variation in atmospheric lifetime across models for SO 2 , SO 4 , and BC, with a particularly large relative variation for SO 2 , which indicates that fundamental aspects of atmospheric sulfur chemistry remain uncertain. Of the perturbations examined in this study, the assumed height of SO 2 injection had the largest overall impacts, particularly on global mean net radiative flux (maximum difference of -0.35?W?m-2), SO2 lifetime over Northern Hemisphere land (maximum difference of 0.8?d), surface SO 2 concentration (up to 59?% decrease), and surface sulfate concentration (up to 23?% increase). Emitting SO 2 at height consistently increased SO 2 and SO 4 column burdens and shortwave cooling, with varying magnitudes, but had inconsistent effects across models on the sign of the change in implied cloud forcing. The assumed SO 4 emission fraction also had a significant impact on net radiative flux and surface sulfate concentration. Because these properties are not standardized across models this is a source of inter-model diversity typically neglected in model intercomparisons. These results imply a need to ensure that anthropogenic emission injection height and SO 4 emission fraction are accurately and consistently represented in global models.

Ahsan, Hamza [Pacific Northwest National Laborator↗
DOE OSTI2021

Industrial emission inventories of iron and phosphorus for past, present and future

Global emission inventories of aerosol iron by species, and of phosphorus, were developed for inclusion in Earth system modeling that includes atmospheric transport. The time period covered was 1850-2010 to evaluate human influence. A variety of approaches to compare measured and modeled values of aerosol iron was synthesized to estimate how well anthropogenic emissions are known. Anthropogenic emissions are constrained within a factor of two and if there is a bias, it is an overestimation. The exception is shipping emissions, which may be underestimated. Direct radiative forcing by iron aerosol is small in the global average (0.02 W m -2 ) but reaches 0.25 W m -2 around source regions. Regions of high direct radiative forcing are poorly constrained by observations. The central value of change in oceanic net primary productivity due to iron deposition is about 0.26 PgC yr -1 , also highly localized. This leads to a decrease in atmospheric CO2 accumulation that corresponds to a forcing of 0.008 W m -2 since 1850 (0.003-0.18 W m -2 ). Emissions of particulate matter to 2050 were estimated in response to different policy scenarios, including the need for renewable energy installations under decarbonization scenarios. Under the business-as-usual scenario, the total metal demand is 195 Mt/yr in 2020, peaking at 270 Mt/yr in years 2040-2045; under the Rapid Decarbonization scenario, total metal demand is nearly doubled at its peak: 480 Mt/yr in year 2040. Primary particulate matter emissions attributable to processing metals for renewable energy are also amplified under rapid decarbonization, but total atmospheric emissions are much lower because of the shift away from combustion.

58 GEOSCIENCES↗
DOE OSTI2022

Atmospheric Radiative and Oceanic Biological Productivity Responses to Increasing Anthropogenic Combustion‐Iron Emission in the 1850–2010 Period

Abstract Anthropogenic emission is an important component of the present‐day iron cycle yet its long‐term impacts on climate are poorly understood. Iron mineralogy strongly affects its radiative and oceanic interactions and was unrepresented in previous studies. We perform simulations using a mineralogy‐based inventory and an atmospheric transport model and estimate the 1850–2010 global mean direct radiative forcing (DRF) to be +0.02 to +0.10 W/m 2 . We estimate that the CO 2 sequestration of 0.2–13 ppmv over the last 150 years due to enhanced phytoplankton productivity by anthropogenic iron deposition causes an avoided CO 2 forcing of −0.002 to −0.16 W/m 2 . While globally small, these impacts can be higher in specific regions; the anthropogenic DRF is +0.5 W/m 2 over areas with more coal combustion and metal smelting, and anthropogenic soluble iron sustains >10% of marine net primary productivity in the high‐latitude North Pacific Ocean, a region vulnerable to stratification due to climate change.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

A comprehensive and synthetic dataset for global, regional, and national greenhouse gas emissions by sector 1970–2018 with an extension to 2019

To track progress towards keeping global warming well below 2 °C or even 1.5 °C, as agreed in the Paris Agreement, comprehensive up-to-date and reliable information on anthropogenic emissions and removals of greenhouse gas (GHG) emissions is required. Here we compile a new synthetic dataset on anthropogenic GHG emissions for 1970–2018 with a fast-track extension to 2019. Our dataset is global in coverage and includes CO 2 emissions, CH 4 emissions, N 2 O emissions, as well as those from fluorinated gases (F-gases: HFCs, PFCs, SF 6 , NF 3 ) and provides country and sector details. We build this dataset from the version 6 release of the Emissions Database for Global Atmospheric Research (EDGAR v6) and three bookkeeping models for CO 2 emissions from land use, land-use change, and forestry (LULUCF). We assess the uncertainties of global greenhouse gases at the 90 % confidence interval (5th–95th percentile range) by combining statistical analysis and comparisons of global emissions inventories and top-down atmospheric measurements with an expert judgement informed by the relevant scientific literature. We identify important data gaps for F-gas emissions. The agreement between our bottom-up inventory estimates and top-down atmospheric-based emissions estimates is relatively close for some F-gas species (~ 10 % or less), but estimates can differ by an order of magnitude or more for others. Our aggregated F-gas estimate is about 10 % lower than top-down estimates in recent years. However, emissions from excluded F-gas species such as chlorofluorocarbons (CFCs) or hydrochlorofluorocarbons (HCFCs) are cumulatively larger than the sum of the reported species. Using global warming potential values with a 100-year time horizon from the Sixth Assessment Report by the Intergovernmental Panel on Climate Change (IPCC), global GHG emissions in 2018 amounted to 58 ± 6.1 GtCO 2 eq. consisting of CO 2 from fossil fuel combustion and industry (FFI) 38 ± 3.0 GtCO 2 , CO 2 -LULUCF 5.7 ± 4.0 GtCO 2 , CH 4 10 ± 3.1 GtCO 2 eq., N2O 2.6 ± 1.6 GtCO 2 eq., and F-gases 1.3 ± 0.40 GtCO 2 eq. Initial estimates suggest further growth of 1.3 GtCO 2 eq. in GHG emissions to reach 59 ± 6.6 GtCO 2 eq. by 2019. Our analysis of global trends in anthropogenic GHG emissions over the past 5 decades (1970–2018) highlights a pattern of varied but sustained emissions growth. There is high confidence that global anthropogenic GHG emissions have increased every decade, and emissions growth has been persistent across the different (groups of) gases. There is also high confidence that global anthropogenic GHG emissions levels were higher in 2009–2018 than in any previous decade and that GHG emissions levels grew throughout the most recent decade. While the average annual GHG emissions growth rate slowed between 2009 and 2018 (1.2 % yr –1 ) compared to 2000–2009 (2.4 % yr –1 ), the absolute increase in average annual GHG emissions by decade was never larger than between 2000–2009 and 2009–2018. Our analysis further reveals that there are no global sectors that show sustained reductions in GHG emissions. There are a number of countries that have reduced GHG emissions over the past decade, but these reductions are comparatively modest and outgrown by much larger emissions growth in some developing countries such as China, India, and Indonesia. There is a need to further develop independent, robust, and timely emissions estimates across all gases. As such, tracking progress in climate policy requires substantial investments in independent GHG emissions accounting and monitoring as well as in national and international statistical infrastructures. The data associated with this article (Minx et al., 2021) can be found at https://doi.org/10.5281/zenodo.5566761.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Properties and Controlling Processes of Aerosol and Cloud Condensation Nuclei in Marine Boundary Layer Over Eastern North Atlantic (Final Report)

Remote marine low cloud systems have large spatial and temporal coverages. Because of their relatively low optical thickness and background aerosol concentrations, marine low clouds are particularly susceptible to perturbations in aerosols associated with anthropogenic emissions. Recent studies show that a large fraction of the global aerosol indirect forcing can be attributed to changes in marine low clouds, despite their relatively long distance from most anthropogenic sources. Currently, there remain large uncertainties in the magnitude of the global aerosol indirect radiative forcing. One major contribution to this large uncertainty derives from poor understanding of the aerosols under natural conditions, the perturbation by anthropogenic emissions, and the processes that drive them. In this project, we took advantage of the comprehensive, multi-dimensional characterization of meteorological parameters, trace gases, aerosol, cloud, and drizzle fields during the Aerosol and Cloud Experiments in Eastern North Atlantic (ACE-ENA) and the long-term measurements at the Atmospheric Radiation Measurement (ARM) Eastern North Atlantic (ENA) site on Graciosa Island. By synergistically combining in situ measurements, remote sensing retrievals, and model simulations, we quantified aerosol properties in the ENA, their vertical profiles, and variations with season, synoptic state, and airmass. We investigated key aerosol processes, including entrainment of free troposphere aerosol into marine boundary layer, new particle formation, growth of Aitken mode particles, and the influences of these processes on the cloud condensation nuclei (CCN) population in marine boundary layer. The representation of key aerosol processes in the Energy Exascale Earth System Model (E3SM) was evaluated using the observations. This project has led to 26 publications, which are listed at the end of this report.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

The acidity of atmospheric particles and clouds

Acidity, defined as pH, is a central component of aqueous chemistry. In the atmosphere, the acidity of condensed phases (aerosol particles, cloud water, and fog droplets) governs the phase partitioning of semivolatile gases such as HNO 3 , NH 3 , HCl, and organic acids and bases as well as chemical reaction rates. It has implications for the atmospheric lifetime of pollutants, deposition, and human health. Despite its fundamental role in atmospheric processes, only recently has this field seen a growth in the number of studies on particle acidity. Even with this growth, many fine-particle pH estimates must be based on thermodynamic model calculations since no operational techniques exist for direct measurements. Current information indicates acidic fine particles are ubiquitous, but observationally constrained pH estimates are limited in spatial and temporal coverage. Clouds and fogs are also generally acidic, but to a lesser degree than particles, and have a range of pH that is quite sensitive to anthropogenic emissions of sulfur and nitrogen oxides, as well as ambient ammonia. Historical measurements indicate that cloud and fog droplet pH has changed in recent decades in response to controls on anthropogenic emissions, while the limited trend data for aerosol particles indicate acidity may be relatively constant due to the semivolatile nature of the key acids and bases and buffering in particles. This paper reviews and synthesizes the current state of knowledge on the acidity of atmospheric condensed phases, specifically particles and cloud droplets. It includes recommendations for estimating acidity and pH, standard nomenclature, a synthesis of current pH estimates based on observations, and new model calculations on the local and global scale.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA)

With their extensive coverage, marine low clouds greatly impact global climate. Presently, marine low clouds are poorly represented in global climate models, and the response of marine low clouds to changes in atmospheric greenhouse gases and aerosols remains the major source of uncertainty in climate simulations. The Eastern North Atlantic (ENA) is a region of persistent but diverse subtropical marine boundary layer clouds, whose albedo and precipitation are highly susceptible to perturbations in aerosol properties. In addition, the ENA is periodically impacted by continental aerosols, making it an excellent location to study the cloud condensation nuclei (CCN) budget in a remote marine region periodically perturbed by anthropogenic emissions, and to investigate the impacts of long-range transport of aerosols on remote marine clouds. The Aerosol and Cloud Experiments in Eastern North Atlantic (ACE-ENA) campaign was motivated by the need of comprehensive in-situ measurements for improving the understanding of marine boundary layer CCN budget, cloud and drizzle microphysics, and the impact of aerosol on marine low cloud and precipitation. The airborne deployments took place from June 21 to July 20, 2017 and January 15 to February 18, 2018 in the Azores. The flights were designed to maximize the synergy between in-situ airborne measurements and ongoing long-term observations at a ground site. Here we present measurements, observation strategy, meteorological conditions during the campaign, and preliminary findings. Lastly, we discuss future analyses and modeling studies that improve the understanding and representation of marine boundary layer aerosols, clouds, precipitation, and the interactions among them.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Global Methane Budget 2000–2020

Abstract. Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. CH4 is the second most important human-influenced greenhouse gas in terms of climate forcing after carbon dioxide (CO2), and both emissions and atmospheric concentrations of CH4 have continued to increase since 2007 after a temporary pause. The relative importance of CH4 emissions compared to those of CO2 for temperature change is related to its shorter atmospheric lifetime, stronger radiative effect, and acceleration in atmospheric growth rate over the past decade, the causes of which are still debated. Two major challenges in quantifying the factors responsible for the observed atmospheric growth rate arise from diverse, geographically overlapping CH4 sources and from the uncertain magnitude and temporal change in the destruction of CH4 by short-lived and highly variable hydroxyl radicals (OH). To address these challenges, we have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to improve, synthesise, and update the global CH4 budget regularly and to stimulate new research on the methane cycle. Following Saunois et al. (2016, 2020), we present here the third version of the living review paper dedicated to the decadal CH4 budget, integrating results of top-down CH4 emission estimates (based on in situ and Greenhouse Gases Observing SATellite (GOSAT) atmospheric observations and an ensemble of atmospheric inverse-model results) and bottom-up estimates (based on process-based models for estimating land surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations). We present a budget for the most recent 2010–2019 calendar decade (the latest period for which full data sets are available), for the previous decade of 2000–2009 and for the year 2020. The revision of the bottom-up budget in this 2025 edition benefits from important progress in estimating inland freshwater emissions, with better counting of emissions from lakes and ponds, reservoirs, and streams and rivers. This budget also reduces double counting across freshwater and wetland emissions and, for the first time, includes an estimate of the potential double counting that may exist (average of 23 Tg CH4 yr−1). Bottom-up approaches show that the combined wetland and inland freshwater emissions average 248 [159–369] Tg CH4 yr−1 for the 2010–2019 decade. Natural fluxes are perturbed by human activities through climate, eutrophication, and land use. In this budget, we also estimate, for the first time, this anthropogenic component contributing to wetland and inland freshwater emissions. Newly available gridded products also allowed us to derive an almost complete latitudinal and regional budget based on bottom-up approaches. For the 2010–2019 decade, global CH4 emissions are estimated by atmospheric inversions (top-down) to be 575 Tg CH4 yr−1 (range 553–586, corresponding to the minimum and maximum estimates of the model ensemble). Of this amount, 369 Tg CH4 yr−1 or ∼ 65 % is attributed to direct anthropogenic sources in the fossil, agriculture, and waste and anthropogenic biomass burning (range 350–391 Tg CH4 yr−1 or 63 %–68 %). For the 2000–2009 period, the atmospheric inversions give a slightly lower total emission than for 2010–2019, by 32 Tg CH4 yr−1 (range 9–40). The 2020 emission rate is the highest of the period and reaches 608 Tg CH4 yr−1 (range 581–627), which is 12 % higher than the average emissions in the 2000s. Since 2012, global direct anthropogenic CH4 emission trends have been tracking scenarios that assume no or minimal climate mitigation policies proposed by the Intergovernmental Panel on Climate Change (shared socio-economic pathways SSP5 and SSP3). Bottom-up methods suggest 16 % (94 Tg CH4 yr−1) larger global emissions (669 Tg CH4 yr−1, range 512–849) than top-down inversion methods for the 2010–2019 period. The discrepancy between the bottom-up and the top-down budgets has been greatly reduced compared to the previous differences (167 and 156 Tg CH4 yr−1 in Saunois et al. (2016, 2020) respectively), and for the first time uncertainties in bottom-up and top-down budgets overlap. Although differences have been reduced between inversions and bottom-up, the most important source of uncertainty in the global CH4 budget is still attributable to natural emissions, especially those from wetlands and inland freshwaters. The tropospheric loss of methane, as the main contributor to methane lifetime, has been estimated at 563 [510–663] Tg CH4 yr−1 based on chemistry–climate models. These values are slightly larger than for 2000–2009 due to the impact of the rise in atmospheric methane and remaining large uncertainty (∼ 25 %). The total sink of CH4 is estimated at 633 [507–796] Tg CH4 yr−1 by the bottom-up approaches and at 554 [550–567] Tg CH4 yr−1 by top-down approaches. However, most of the top-down models use the same OH distribution, which introduces less uncertainty to the global budget than is likely justified. For 2010–2019, agriculture and waste contributed an estimated 228 [213–242] Tg CH4 yr−1 in the top-down budget and 211 [195–231] Tg CH4 yr−1 in the bottom-up budget. Fossil fuel emissions contributed 115 [100–124] Tg CH4 yr−1 in the top-down budget and 120 [117–125] Tg CH4 yr−1 in the bottom-up budget. Biomass and biofuel burning contributed 27 [26–27] Tg CH4 yr−1 in the top-down budget and 28 [21–39] Tg CH4 yr−1 in the bottom-up budget. We identify five major priorities for improving the CH4 budget: (i) producing a global, high-resolution map of water-saturated soils and inundated areas emitting CH4 based on a robust classification of different types of emitting ecosystems; (ii) further development of process-based models for inland-water emissions; (iii) intensification of CH4 observations at local (e.g. FLUXNET-CH4 measurements, urban-scale monitoring, satellite imagery with pointing capabilities) to regional scales (surface networks and global remote sensing measurements from satellites) to constrain both bottom-up models and atmospheric inversions; (iv) improvements of transport models and the representation of photochemical sinks in top-down inversions; and (v) integration of 3D variational inversion systems using isotopic and/or co-emitted species such as ethane as well as information in the bottom-up inventories on anthropogenic super-emitters detected by remote sensing (mainly oil and gas sector but also coal, agriculture, and landfills) to improve source partitioning. The data presented here can be downloaded from https://doi.org/10.18160/GKQ9-2RHT (Martinez et al., 2024).

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Long-term trends of impacts of global gasoline and diesel emissions on ambient PM 2.5 and O 3 pollution and the related health burden for 2000–2015

Global economic development and urbanization during the past two decades have driven the increases in demand of personal and commercial vehicle fleets, especially in developing countries, which has likely resulted in changes in year-to-year vehicle tailpipe emissions associated with aerosols and trace gases. However, long-term trends of impacts of global gasoline and diesel emissions on air quality and human health are not clear. In this study, we employ the Community Earth System Model in conjunction with the newly developed Community Emissions Data System as anthropogenic emission inventory to quantify the long-term trends of impacts of global gasoline and diesel emissions on ambient air quality and human health for the period of 2000–2015. Global gasoline and diesel emissions contributed to regional increases in annual mean surface PM 2.5 (particulate matter with aerodynamic diameters ≤2.5 μm) concentrations by up to 17.5 and 13.7 µg m –3 , and surface ozone (O 3 ) concentrations by up to 7.1 and 7.2 ppbv, respectively, for 2000–2015. However, we also found substantial declines of surface PM 2.5 and O 3 concentrations over Europe, the US, Canada, and China for the same period, which suggested the co-benefits of air quality and human health from improving gasoline and diesel fuel quality and tightening vehicle emissions standards. Globally, we estimate the mean annual total PM 2.5- and O 3 -induced premature deaths are 139 700–170 700 for gasoline and 205 200–309 300 for diesel, with the corresponding years of life lost of 2.74–3.47 and 4.56–6.52 million years, respectively. Diesel and gasoline emissions create health-effect disparities between the developed and developing countries, which are likely to aggravate afterwards.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Global source apportionment of aerosols into major emission regions and sectors over 1850–2017

Anthropogenic emissions of aerosols and precursor gases have changed significantly in the past few decades around the world. In this study, the Explicit Aerosol Source Tagging (EAST) system is merged into the Energy Exascale Earth System Model version 1 (E3SMv1) to quantify the variations in anthropogenic aerosol concentrations, source contributions, and their subsequent radiative impact in four major emission regions across the globe during 1850–1980, 1980–2010, and 2010–2017. In North America and Europe, changes in anthropogenic PM 2.5 were mainly caused by changes in emissions from local energy and industrial sectors. The local industrial sector caused the largest increase in PM 2.5 in East Asia during 1980–2010 and decrease during 2010–2017. In South Asia, the increase in energy-related emissions dominated the rise in PM 2.5 levels during 1980–2017. During 1850–1980, the increases in emissions from North America contributed to the increase in the European PM 2.5 burden by 1.7 mg m -2 and the sources from the Europe were also responsible for the PM 2.5 burden increase in East Asia and South Asia by about 1.0 mg m -2 . During 1980–2010, East Asia contributed to an increase of 0.4–0.6 mg m -2 in the PM 2.5 burden in North America and Europe, while South Asia contributed about 0.3 mg m -2 . During 2010–2017, the contributions from East Asia to the PM 2.5 burdens in the North America, Europe, and South Asia declined by 0.3–0.6 mg m -2 due to the clean air actions in China, while the contributions from South Asia still increased due to the continuous increase in emissions in South Asia. The historical changes in aerosols had an impact on effective radiative forcing through aerosol–radiation interactions (ERF ari ). During 1980–2010, a decline in North American aerosols resulted in a positive ERF ari change (warming effect) in Europe and a decline in aerosols in Europe caused a warming effect in Russia and northern China. The changes in ERF ari from the increase and decrease in aerosols in China during 1980–2010 and 2010–2017, respectively, are comparable in magnitude. The continuous aerosol increases in South Asia from 1980 to 2017 resulted in negative ERF ari (cooling) changes in South Asia, Southeast Asia, and southern China.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

The Global Methane Budget 2000–2017

Understanding and quantifying the global methane (CH 4 ) budget is important for assessing realistic pathways to mitigate climate change. Atmospheric emissions and concentrations of CH 4 are continuing to increase, making CH 4 the second most important human-influenced greenhouse gas in terms of climate forcing, after carbon dioxide (CO 2 ). Assessing the relative importance of CH 4 in comparison to CO 2 is complicated by its shorter atmospheric lifetime, stronger warming potential, and atmospheric growth rate variations over the past decade, the causes of which are still debated. Two major difficulties in reducing uncertainties arise from the variety of geographically overlapping CH 4 sources and from the destruction of CH 4 by short-lived hydroxyl radicals (OH). To address these difficulties, we have established a consortium of multi-disciplinary 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).

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2025

Model America - 2022 Arizona Building Energy Simulation Results from ORNL's AutoBEM

This dataset contains energy simulation outputs using ORNL's AutoBEM, covering the summer months (June 1st to August 31st) (named by "county_name.csv") and full-year periods (in output_all_year.zip) for each county in Arizona, USA. The data package includes simulation results such as basic energy metrics and anthropogenic emissions estimates. Files are provided in .csv. These data were generated to analyze the impact of weather conditions on energy use and emissions across urban and rural environments in Arizona, aiming to support research on urban heat islands, energy efficiency, and building retrofitting strategies. The source data for this work include NASA POWER weather datasets and computational models run using AutoBEM (i.e., an automated, large-scale energy simulation tool leveraging OpenStudio/EnergyPlus). This dataset can assist researchers, urban planners, and policymakers in developing climate-resilient energy systems and understanding anthropogenic contributions to local environments.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Persistent high PM 2.5 pollution driven by unfavorable meteorological conditions during the COVID-19 lockdown period in the Beijing-Tianjin-Hebei region, China

Lockdown measures to curtail the COVID-19 pandemic in China halted most nonessential activities on January 23, 2020. Despite significant reductions in anthropogenic emissions, the Beijing-Tianjin-Hebei (BTH) region still experienced high air pollution concentrations. In this work, employing two emissions reduction scenarios, the Community Multiscale Air Quality (CMAQ) model was used to investigate the PM 2.5 concentrations change in this region. The model using the scenario (C3) with greater traffic reductions performed better compared to the observed PM 2.5 . Compared with the no reductions base-case (scenario C1), PM 2.5 reductions with scenario C3 were 2.70, 2.53, 2.90, 2.98, 3.30, 2.81, 2.82, 2.98, 2.68, and 2.83 µg/m 3 in Beijing, Tianjin, Shijiazhuang, Baoding, Cangzhou, Chengde, Handan, Hengshui, Tangshan, and Xingtai, respectively. During high-pollution days in scenario C3, the percentage reductions in PM 2.5 concentrations in Beijing, Tianjin, Shijiazhuang, Baoding, Cangzhou, Chengde, Handan, Hengshui, Tangshan, and Xingtai were 3.76, 3.54, 3.28, 3.22, 3.57, 3.56, 3.47, 6.10, 3.61, and 3.67%, respectively. However, significant increases caused by unfavorable meteorological conditions counteracted the emissions reduction effects resulting in high air pollution in BTH region during the lockdown period. This study shows that effective air pollution control strategies incorporating these results are urgently required in BTH to avoid severe pollution.

54 ENVIRONMENTAL SCIENCES↗