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DOE OSTI2025

The Observed and Projected Changes of Global Monsoons: Current Status and Future Perspectives

The global monsoon system, encompassing the Asian-Australian, African, and American monsoons, sustains two-thirds of the world’s population by regulating water resources and agriculture. Monsoon anomalies pose severe risks, including floods and droughts. Recent research associated with the implementation of the Global Monsoons Model Intercomparison Project under the umbrella of CMIP6 has advanced our understanding of its historical variability and driving mechanisms. Observational data reveal a 20th-century shift: increased rainfall pre-1950s, followed by aridification and partial recovery post-1980s, driven by both internal variability (e.g., Atlantic Multidecadal Oscillation) and external forcings (greenhouse gases, aerosols), while ENSO drives interannual variability through ocean-atmosphere interactions. Future projections under greenhouse forcing suggest long-term monsoon intensification, though regional disparities and model uncertainties persist. Models indicate robust trends but struggle to quantify extremes, where thermodynamic effects (warming-induced moisture rise) uniformly boost heavy rainfall, while dynamical shifts (circulation changes) create spatial heterogeneity. Volcanic eruptions and proposed solar radiation modification (SRM) further complicate predictions: tropical eruptions suppress monsoons, whereas high-latitude events alter cross-equatorial flows, highlighting unresolved feedbacks. The emergent constraint approach is booming in terms of correcting future projections and reducing uncertainty with respect to the global monsoons. Critical challenges remain. Model biases and sparse 20th-century observational data hinder accurate attribution. The interplay between natural variability and anthropogenic forcings, along with nonlinear extreme precipitation risks under warming, demands deeper mechanistic insights. Additionally, SRM’s regional impacts and hemispheric monsoon interactions require systematic evaluation. Addressing these gaps necessitates enhanced observational networks, refined climate models, and interdisciplinary efforts to disentangle multiscale drivers, ultimately improving resilience strategies for monsoon-dependent regions.

climate extreme events↗

DOE OSTI2020

Microbial functional genes commonly respond to elevated carbon dioxide

Atmospheric CO 2 concentration is increasing, largely due to anthropogenic activities. Previous studies of individual free-air CO 2 enrichment (FACE) experimental sites have shown significant impacts of elevated CO 2 (eCO 2 ) on soil microbial communities; however, no common microbial response patterns have yet emerged, challenging our ability to predict ecosystem functioning and sustainability in the future eCO 2 environment. Here we analyzed 66 soil microbial communities from five FACE sites, and showed common microbial response patterns to eCO 2 , especially for key functional genes involved in carbon and nitrogen fixation (e.g., pcc/acc for carbon fixation, nifH for nitrogen fixation), carbon decomposition (e.g., amyA and pulA for labile carbon decomposition, mnp and lcc for recalcitrant carbon decomposition), and greenhouse gas emissions (e.g., mcrA for methane production, norB for nitrous oxide production) across five FACE sites. Also, the relative abundance of those key genes was generally increased and directionally associated with increased biomass, soil carbon decomposition, and soil moisture. In addition, a further literature survey of more disparate FACE experimental sites indicated increased biomass, soil carbon decay, nitrogen fixation, methane and nitrous oxide emissions, plant and soil carbon and nitrogen under eCO 2 . A conceptual framework was developed to link commonly responsive functional genes with ecosystem processes, such as pcc/acc vs. soil carbon storage, amyA/pulA/mnp/lcc vs. soil carbon decomposition, and nifH vs. nitrogen availability, suggesting that such common responses of microbial functional genes may have the potential to predict ecosystem functioning and sustainability in the future eCO 2 environment.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2022

Reduced CO 2 uptake and growing nutrient sequestration from slowing overturning circulation

Current Earth system models (ESMs) project dramatic slowing (28–42% by 2100) of Atlantic Meridional Overturning Circulation and Southern Meridional Overturning Circulation (SMOC) across a range of climate scenarios, with a complete shutdown of SMOC possible by year 2300. Slowing meridional overturning circulation (MOC) differentially impacts the ocean biological and solubility carbon pumps, leaving the net impact on ocean carbon uptake uncertain. Here using a suite of ESMs, we show that slowing MOC reduces anthropogenic carbon uptake by the solubility pump but increases deep-ocean storage of carbon and nutrients by the biological pump. The net effect reduces ocean uptake of anthropogenic CO 2 . The deep-ocean nutrient sequestration will increasingly depress global-scale, marine net primary production over time. As a result, MOC slowdown represents a positive feedback that could extend or intensify peak-warmth climate conditions on multi-century timescales.

58 GEOSCIENCES↗

DOE OSTI2023

Assessing the methane mitigation potential of innovative management in US rice production

Abstract Rice is an important global crop while also contributing significant anthropogenic methane (CH 4 ) emissions. To support the future of rice production, more information is needed on the impacts of sustainability-driven management used to grow rice with lower associated methane emissions. Recent support for the impacts of different growing practices in the US has prompted the application of a regional methodology (Tier 2) to estimate methane emissions in different rice growing regions. The methodology estimates rice methane emissions from the US Mid-South (MdS) and California (Cal) using region-specific scaling factors applied to a region-specific baseline flux. In our study, we leverage land cover data and soil clay content to estimate methane emissions using this approach, while also examining how changes in common production practices can affect overall emissions in the US. Our results indicated US rice cultivation produced between 0.32 and 0.45 Tg CH 4 annually, which were approximately 7% and 42% lower on average compared to Food and Agriculture Organization of the UN (FAO) and US Environmental Protection Agency (EPA) inventories, respectively. Our estimates were 63% greater on average compared to similar methods that lack regional context. Introducing aeration events into irrigation resulted in the greatest methane reductions across both regions. When accounting for differences between baseline and reduction scenarios, the US MdS typically had higher mitigation potential compared to Cal. The differences in cumulative mitigation potential across the 2008–2020 period were likely driven by lower production area clay content for the US MdS compared to Cal. The added spatial representation in the Tier 2 approach is useful in surveying how impactful methane-reducing practices might be within and across regions.

Environmental Sciences & Ecology↗

DOE OSTI2020

Rapid growth of anthropogenic organic nanoparticles greatly alters cloud lifecycle in the Amazon rainforest

Atmospheric nanoparticles can significantly influence Earth’s climate if they grow to sizes large enough to nucleate cloud droplets. While the contribution of extremely low volatility vapors to nanoparticle growth has been discussed extensively, the role of semivolatile organics has been largely overlooked. Here we examine the growth and impacts of air pollution nanoparticles from an isolated metropolis amidst the Amazon rainforest. Although extremely low volatility organics are necessary for the initial growth of nanoparticles, model analysis suggests that dynamic gas-particle partitioning of semivolatile oxidation products of anthropogenic and natural hydrocarbons is predominantly responsible for the observed rapid growth to 50 nm. Furthermore, cloud-resolving simulations demonstrate that the grown particles appreciably modify shallow cloud droplet size distribution, suppress precipitation, and enhance the transition to deep clouds. With condensable semivolatile organics typically formed in greater proportion, similar nanoparticle growth and impacts on clouds could likely occur in heavily urbanized forested regions globally.

Zaveri, Rahul A↗

DOE OSTI2020

DATASET: Rapid growth of anthropogenic organic nanoparticles greatly alters cloud lifecycle in the Amazon rainforest

Zaveri, Rahul A↗

DOE OSTI2023

A Large Ensemble Global Dataset for Climate Impact Assessments

We present a self-consistent, large ensemble, high-resolution global dataset of long-term future climate, which accounts for the uncertainty in climate system response to anthropogenic emissions of greenhouse gases and in geographical patterns of climate change. The dataset is developed by applying an integrated spatial disaggregation (SD) - bias-correction (BC) method to climate projections from the MIT Integrated Global System Model (IGSM). Four emission scenarios are considered that represent energy and environmental policies and commitments of potential future pathways, namely, Reference, Paris Forever, Paris 2 °C and Paris 1.5 °C. The dataset contains nine key meteorological variables on a monthly scale from 2021 to 2100 at a spatial resolution of 0.5°x 0.5°, including precipitation, air temperature (mean, minimum and maximum), near-surface wind speed, shortwave and longwave radiation, specific humidity, and relative humidity. We demonstrate the dataset’s ability to represent climate-change responses across various regions of the globe. This dataset can be used to support regional-scale climate-related impact assessments of risk across different applications that include hydropower, water resources, ecosystem, agriculture, and sustainable development.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Earth's record-high greenness and its attributions in 2020

Terrestrial vegetation is a crucial component of Earth's biosphere, regulating global carbon and water cycles and contributing to human welfare. Despite an overall greening trend, terrestrial vegetation exhibits a significant inter-annual variability. The mechanisms driving this variability, particularly those related to climatic and anthropogenic factors, remain poorly understood, which hampers our ability to project the long-term sustainability of ecosystem services. Here, in this work, by leveraging diverse remote sensing measurements, we pinpointed 2020 as a historic landmark, registering as the greenest year in modern satellite records from 2001 to 2020. Using ensemble machine learning and Earth system models, we found this exceptional greening primarily stemmed from consistent growth in boreal and temperate vegetation, attributed to rising CO 2 levels, climate warming, and reforestation efforts, alongside a transient tropical green-up linked to the enhanced rainfall. Contrary to expectations, the COVID-19 pandemic lockdowns had a limited impact on this global greening anomaly. Our findings highlight the resilience and dynamic nature of global vegetation in response to diverse climatic and anthropogenic influences, offering valuable insights for optimizing ecosystem management and informing climate mitigation strategies.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Emerging Per- and Polyfluoroalkyl Substances in Tap Water from the American Healthy Homes Survey II

Humans experience widespread exposure to anthropogenic per- and polyfluoroalkyl substances (PFAS) through various media, which can lead to a wide range of negative health impacts. Tap water is an important source of exposure in communities with any degree of contamination but routine or large-scale PFAS monitoring often depends on targeted analytical methods limited to measuring specific PFAS. We analyzed 680 tap water samples from the American Healthy Homes Survey II for PFAS using non-targeted analysis (NTA) to expand the range of detectable PFAS. Based on detection frequency and relative abundance, about half of the identified PFAS were found only by NTA. We identified (with varying degrees of confidence) 75 distinct PFAS, including 57 exclusively detected by NTA. The identified PFAS are members of seven structural subclasses differentiated by their head groups and degree of fluorination. Clustering analysis categorized the PFAS into four coabundance groups dominated by specific PFAS subclasses. One group uniquely identified by NTA contains zwitterionic PFAS and other PFAS transformation products which are likely associated with aqueous firefighting foam contaminants in a small number of spatially correlated samples. These results help further characterize the scope of exposure to emerging PFAS experienced by the U.S. population via tap water and augment nationwide targeted-PFAS monitoring programs.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗

DOE OSTI2023

Climate responses in China to domestic and foreign aerosol changes due to clean air actions during 2013–2019

In recent years, to improve air quality, significant efforts have been made to reduce regional aerosols including China, Europe and North America, which have potential impacts on climate. In this study, fast and slow climate responses in China to changes in domestic and foreign anthropogenic emissions of aerosols and precursors from 2013 to 2019 are investigated using the Community Earth System Model version 1 (CESM1). Aerosol emissions changes, especially reductions in China, North America and Europe, during 2013–2019 resulted in surface air temperature increases across the Northern Hemisphere. Global aerosol changes induce a regional warming of 0.2 °C in China, equally contributed by domestic and foreign emissions changes. China’s domestic emission reductions lead to a regional average temperature rise of 0.1°C, primarily driven by rapid atmospheric adjustments over eastern China. Foreign aerosol changes, particularly reductions in North America and Europe, also contributed to a 0.1°C warming in China through slow oceanic processes. This warming in China induced by foreign aerosol changes is due to a teleconnection between the aerosol-induced anomalous regional warming in Eastern U.S.-North Atlantic Ocean-Europe and the downstream East Asian climate through anomalous wave trains propagation. The comparable influence of domestic and foreign aerosol changes on climate in China underscores the importance of international collaboration in climate mitigation endeavors.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Nitrogen Source Governs Community Carbon Metabolism in a Model Hypersaline Benthic Phototrophic Biofilm

Increasing anthropogenic inputs of fixed nitrogen are leading to greater eutrophication of aquatic environments, but it is unclear how this impacts the flux and fate of carbon in lacustrine and riverine systems. Here, we present evidence that the form of nitrogen governs the partitioning of carbon among members in a genome-sequenced, model phototrophic biofilm of 20 members. Consumption of NO 3 – as the sole nitrogen source unexpectedly resulted in more rapid transfer of carbon to heterotrophs than when NH 4 + was also provided, suggesting alterations in the form of carbon exchanged. The form of nitrogen dramatically impacted net community nitrogen, but not carbon, uptake rates. Furthermore, this alteration in nitrogen form caused very large but focused alterations to community structure, strongly impacting the abundance of only two species within the biofilm and modestly impacting a third member species. Our data suggest that nitrogen metabolism may coordinate coupled carbon-nitrogen biogeochemical cycling in benthic biofilms and, potentially, in phototroph-heterotroph consortia more broadly. It further indicates that the form of nitrogen inputs may significantly impact the contribution of these communities to carbon partitioning across the terrestrial-aquatic interface.

carbon cycling↗

DOE OSTI2020

Climate smart agriculture and global food-crop production

Most business-as-usual scenarios for farming under changing climate regimes project that the agriculture sector will be significantly impacted from increased temperatures and shifting precipitation patterns. Perhaps ironically, agricultural production contributes substantially to the problem with yearly greenhouse gas (GHG) emissions of about 11% of total anthropogenic GHG emissions, not including land use change. It is partly because of this tension that Climate Smart Agriculture (CSA) has attracted interest given its promise to increase agricultural productivity under a changing climate while reducing emissions. Considerable resources have been mobilized to promote CSA globally even though the potential effects of its widespread adoption have not yet been studied. Here we show that a subset of agronomic practices that are often included under the rubric of CSA can contribute to increasing agricultural production under unfavorable climate regimes while contributing to the reduction of GHG. However, for CSA to make a significant impact important investments and coordination are required and its principles must be implemented widely across the entire sector.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Low Temperature Activation of Methane on Metal-Oxides and Complex Interfaces: Insights from Surface Science

The abundance of inexpensive, natural gas has transformed the energy landscape, whereby revealing new possibilities for sustainable chemical technologies or impacting those that have relied on traditional fossil fuels. The primary component, methane, is underutilized and wastefully exhausted, leading to anthropogenic global warming. Historically, the manipulation of methane remained “ clavis aurea ,” an insurmountable yet rewarding challenge and thus the focus of intense research. This is primarily due to an inability to dissociate C–H bonds in methane selectively, which requires a high energy penalty and is an essential prerequisite for the direct conversion of methane into a large set of value-added products. The discovery of such processes would promise an energy gainful use of natural gas benefiting several essential chemical processes associated with C1 chemistry. This first C–H bond dissociation step of the methane molecule appears in numerous catalytic mechanisms as the rate-determining step or most essential barrier sequence for all subsequent steps that follow in the production of C–C, C–O, or C x –H y –O z bonds found in value added products. A main goal is to catalytically reduce the energy barrier for the first C–H bond dissociation to be able to achieve the activation of methane at low or moderate temperatures. As such there is great value in understanding the fundamental nature of the active sites responsible for bond breaking or formation and thus be able to facilitate better control of this chemistry, leading to the development of new technologies for fuel production and chemical conversion. Surface science studies offer enhanced perspectives for a careful manipulation of bonds over the last layer atoms of catalyst surfaces, an essential factor for the design of atomically precise catalysts and unravelling of the reaction mechanism. With the advent of new surface imaging, spectroscopy, and in situ tools, it has been possible to decipher the surface chemistry of complex materials systems and further our understanding of atomic active sites on the surfaces of metals, oxides, and carbides or metal–oxide and metal–carbide interfaces. The once considered near impossible step of C–H bond activation is now observed at low temperatures with high propensity over a collection of oxide, metal–oxide, and metal–carbide systems in a conventional or inverse configuration (oxide or carbide on metal). The enabling of C–H activation at low temperature has opened interesting possibilities for the specific production of chemicals such as methanol directly from methane, a step toward facile synthesis of liquid fuels. We highlight the most recent of these results and present the key aspects of active site configurations engineered from surface science studies which enable such a simple reactive event through careful manipulation of the last surface layer of atoms found in the catalyst structure. New concepts which help in the activation and conversion of methane are discussed.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Assessing the sensitivity of aerosol mass budget and effective radiative forcing to horizontal grid spacing in E3SMv1 using a regional refinement approach

Abstract. Atmospheric aerosols have important impacts on air quality and the Earth–atmospheric energy balance. However, as computing power is limited, Earth system models generally use coarse spatial grids and parameterize finer-scale atmospheric processes. These parameterizations and the simulation of atmospheric aerosols are often sensitive to model horizontal resolutions. Understanding the sensitivities is necessary for the development of Earth system models at higher resolutions with the deployment of more powerful supercomputers. Using the Energy Exascale Earth System Model (E3SM) version 1, this study investigates the impact of horizontal grid spacing on the simulated aerosol mass budget, aerosol–cloud interactions, and the effective radiative forcing of anthropogenic aerosols (ERFaer) over the contiguous United States. We examine the resolution sensitivity by comparing the nudged simulation results for 2016 from the low-resolution model (LR) and the regional refinement model (RRM). As expected, the simulated emissions of natural dust, sea salt, and marine organic matter are substantially higher in the RRM than in the LR. In addition, RRM simulates stronger aqueous-phase production of sulfate through the enhanced oxidation of sulfur dioxide by hydrogen peroxide due to increased cloud liquid water content. In contrast, the gas-phase chemical production of sulfate is slightly suppressed. The RRM resolves more large-scale precipitation and produces less convective precipitation than the LR, leading to increased (decreased) aerosol wet scavenging by large-scale (convective) precipitation. Regarding aerosol effects on clouds, RRM produces larger temporal variabilities in the large-scale liquid cloud fractions than LR, resulting in increased microphysical cloud processing of aerosols (more interstitial aerosols are converted to cloud-borne aerosols via aerosol activation) in RRM. Water vapor condensation is also enhanced in RRM compared to LR. Consequently, the RRM simulation produces more cloud droplets, a larger cloud droplet radius, a higher liquid water path, and a larger cloud optical depth than the LR simulation. A comparison of the present-day and pre-industrial simulations indicates that, for this contiguous United States domain, the higher-resolution increases ERFaer at the top of the model by about 12 %, which is mainly attributed to the strengthened indirect effect associated with aerosol–cloud interactions.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Assessing Adaptive Irrigation Impacts on Water Scarcity in Nonstationary Environments—A Multi‐Agent Reinforcement Learning Approach

Abstract One major challenge in water resource management is to balance the uncertain and nonstationary water demands and supplies caused by the changing anthropogenic and hydroclimate conditions. To address this issue, we developed a reinforcement learning agent‐based modeling (RL‐ABM) framework where agents (agriculture water users) are able to learn and adjust water demands based on their interactions with the water systems. The intelligent agents are created by a reinforcement learning algorithm adapted from the Q‐learning algorithm. We illustrated this framework in a case study where the RL‐ABM is two‐way coupled with the Colorado River Simulation System (CRSS), a long‐term planning model used for the administration of the Colorado River Basin, for assessing agriculture water uses impacts on water scarcity. Seventy‐eight intelligent agents are simulated, which can be grouped into three categories based on their parameter values: the “aggressive” (swift actions; low regrets), the “forward‐looking conservative” (mild actions; high regrets; fast learning), and the “myopic conservative” (mild actions; median regrets; slow learning). The ABM‐CRSS results showed that the major reservoirs in the Upper Colorado Basin might experience more frequent water shortages due to the increasing water uses compared to the original CRSS results. If the drought continues, the case study also demonstrates that agents can learn and adjust their demands.

Hung, Fengwei↗

DOE OSTI2025

Compounding effects of climate change and WUI expansion quadruple the likelihood of extreme-impact wildfires in California

Previous research has examined individual factors contributing to wildfire risk, but the compounding effects of these factors remain underexplored. Here, we introduce the “Integrated Human-centric Wildfire Risk Index (IHWRI)” to quantify the compounding effects of fire-weather intensification and anthropogenic factors—including ignitions and human settlement into wildland—on wildfire risk. While climatic trends increased the frequency of high-risk fire-weather by 2.5-fold, the combination of this trend with wildland-urban interface expansion led to a 4.1-fold increase in the frequency of conditions conducive to extreme-impact wildfires from 1990 to 2022 across California. More than three-quarters of extreme-impact wildfires—defined as the top 20 largest, most destructive, or deadliest events on record—originated within 1 km from the wildland-urban interface. The deadliest and most destructive wildfires—90% of which were human-caused—primarily occurred in the fall, while the largest wildfires—56% of which were human-caused—mostly took place in the summer. By integrating human activity and climate change impacts, we provide a holistic understanding of human-centric wildfire risk, crucial for policy development.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Influence of sea-ice anomalies on Antarctic precipitation using source attribution in the Community Earth System Model

Abstract. We conduct sensitivity experiments using a general circulation model that has an explicit water source tagging capability forced by prescribed composites of pre-industrial sea-ice concentrations (SICs) and corresponding sea surface temperatures (SSTs) to understand the impact of sea-ice anomalies on regional evaporation, moisture transport and source–receptor relationships for Antarctic precipitation in the absence of anthropogenic forcing. Surface sensible heat fluxes, evaporation and column-integrated water vapor are larger over Southern Ocean (SO) areas with lower SICs. Changes in Antarctic precipitation and its source attribution with SICs have a strong spatial variability. Among the tagged source regions, the Southern Ocean (south of 50° S) contributes the most (40 %) to the Antarctic total precipitation, followed by more northerly ocean basins, most notably the South Pacific Ocean (27%), southern Indian Ocean (16 %) and South Atlantic Ocean (11 %). Comparing two experiments prescribed with high and low pre-industrial SICs, respectively, the annual mean Antarctic precipitation is about 150 Gt yr-1 (or 6 %) more in the lower SIC case than in the higher SIC case. This difference is larger than the model-simulated interannual variability in Antarctic precipitation (99 Gt yr-1). The contrast in contribution from the Southern Ocean, 102 Gt yr-1, is even more significant compared to the interannual variability of 35 Gt yr-1 in Antarctic precipitation that originates from the Southern Ocean. The horizontal transport pathways from individual vapor source regions to Antarctica are largely determined by large-scale atmospheric circulation patterns. Vapor from lower-latitude source regions takes elevated pathways to Antarctica. In contrast, vapor from the Southern Ocean moves southward within the lower troposphere to the Antarctic continent along moist isentropes that are largely shaped by local ambient conditions and coastal topography. This study also highlights the importance of atmospheric dynamics in affecting the thermodynamic impact of sea-ice anomalies associated with natural variability on Antarctic precipitation. Our analyses of the seasonal contrast in changes of basin-scale evaporation, moisture flux and precipitation suggest that the impact of SIC anomalies on regional Antarctic precipitation depends on dynamic changes that arise from SIC–SST perturbations along with internal variability. The latter appears to have a more significant effect on the moisture transport in austral winter than in summer.

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↗