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    Authors: X. Faïn; D. M. Etheridge; D. M. Etheridge; K. Fourteau; +20 Authors

    Abstract. Carbon monoxide (CO) is a naturally occurring atmospheric trace gas, a regulated pollutant, and one of the main components determining the oxidative capacity of the atmosphere. Evaluating climate–chemistry models under different conditions than today and constraining past CO sources requires a reliable record of atmospheric CO mixing ratios ([CO]) that includes data since preindustrial times. Here, we report the first continuous record of atmospheric [CO] for Southern Hemisphere (SH) high latitudes over the past 3 millennia. Our continuous record is a composite of three high-resolution Antarctic ice core gas records and firn air measurements from seven Antarctic locations. The ice core gas [CO] records were measured by continuous flow analysis (CFA), using an optical feedback cavity-enhanced absorption spectrometer (OF-CEAS), achieving excellent external precision (2.8–8.8 ppb; 2σ) and consistently low blanks (ranging from 4.1±1.2 to 7.4±1.4 ppb), thus enabling paleo-atmospheric interpretations. Six new firn air [CO] Antarctic datasets collected between 1993 and 2016 CE at the DE08-2, DSSW19K, DSSW20K, South Pole, Aurora Basin North (ABN), and Lock-In sites (and one previously published firn CO dataset at Berkner) were used to reconstruct the atmospheric history of CO from ∼1897 CE, using inverse modeling that incorporates the influence of gas transport in firn. Excellent consistency was observed between the youngest ice core gas [CO] and the [CO] from the base of the firn and between the recent firn [CO] and atmospheric [CO] measurements at Mawson station (eastern Antarctica), yielding a consistent and contiguous record of CO across these different archives. Our Antarctic [CO] record is relatively stable from −835 to 1500 CE, with mixing ratios within a 30–45 ppb range (2σ). There is a ∼5 ppb decrease in [CO] to a minimum at around 1700 CE during the Little Ice Age. CO mixing ratios then increase over time to reach a maximum of ∼54 ppb by ∼1985 CE. Most of the industrial period [CO] growth occurred between about 1940 to 1985 CE, after which there was an overall [CO] decrease, as observed in Greenland firn air and later at atmospheric monitoring sites and attributed partly to reduced CO emissions from combustion sources. Our Antarctic ice core gas CO observations differ from previously published records in two key aspects. First, our mixing ratios are significantly lower than reported previously, suggesting that previous studies underestimated blank contributions. Second, our new CO record does not show a maximum in the late 1800s. The absence of a [CO] peak around the turn of the century argues against there being a peak in Southern Hemisphere biomass burning at this time, which is in agreement with (i) other paleofire proxies such as ethane or acetylene and (ii) conclusions reached by paleofire modeling. The combined ice core and firn air [CO] history, spanning −835 to 1992 CE, extended to the present by the Mawson atmospheric record, provides a useful benchmark for future atmospheric chemistry modeling studies. International audience

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    Climate of the Past (CP)
    Article . 2023 . Peer-reviewed
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    https://doi.org/10.5194/cp-202...
    Preprint . 2023 . Peer-reviewed
    License: CC BY
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    Climate of the Past
    Article . 2023
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    Apollo
    Article . 2023
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    Climate of the Past (CP)
    Other literature type . 2023
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      Climate of the Past (CP)
      Article . 2023 . Peer-reviewed
      License: CC BY
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      https://doi.org/10.5194/cp-202...
      Preprint . 2023 . Peer-reviewed
      License: CC BY
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      Apollo
      Article . 2023
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      Climate of the Past (CP)
      Other literature type . 2023
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    Authors: Nuria Benavent; Anoop S. Mahajan; Qinyi Li; Carlos A. Cuevas; +30 Authors

    This study received funding from the European Research Council Executive Agency under the European Union’s Horizon 2020 Research and Innovation Program (project ERC‐2016‐COG 726349 CLIMAHAL and ERC-2016-STG 714621 GASPARCON) and the European Commission via the EMME-CARE project and was supported by the Consejo Superior de Investigaciones Científicas of Spain. This work was supported by the European Union’s Horizon 2020 Research and Innovation Programme under grant agreement no. 856612 and the Academy of Finland (project no. 334514). The Indian Institute of Tropical Meteorology is funded by the Ministry of Earth Sciences, Government of India. Ozone, CO, CH4 and AMS measurements were funded by the Swiss National Science Foundation (grant 200021_188478), the Swiss Polar Institute and U.S. National Science Foundation grants 1914781 and 1807163. J.S. holds the Ingvar Kamprad chair for extreme environments research, sponsored by Ferring Pharmaceuticals. Data reported in this manuscript were produced as part of the international MOSAiC expedition with tag MOSAiC20192020, with activities supported by Polarstern expedition AWI-PS122_00. H.S. was funded by the European ERA-PLANET projects iGOSP and iCUPE (consortium agreement no. 689443 for both projects). We thank FORMAS and the Swedish Polar Research Secretariat for support. We gratefully acknowledge funding by the Deutsche Forschungsgemeinschaft (project no. 268020496 – TRR 172) within the Transregional Collaborative Research Center ‘ArctiC Amplification: Climate Relevant Atmospheric and SurfaCe Processes, and Feedback Mechanisms (AC)3’ in subproject C03. We thank I. Bourgeois (NOAA/CIRES) for providing the ATom NOx data. Unlike bromine, the effect of iodine chemistry on the Arctic surface ozone budget is poorly constrained. We present ship-based measurements of halogen oxides in the high Arctic boundary layer from the sunlit period of March to October 2020 and show that iodine enhances springtime tropospheric ozone depletion. We find that chemical reactions between iodine and ozone are the second highest contributor to ozone loss over the study period, after ozone photolysis-initiated loss and ahead of bromine. 6 pags., 2 figs. Peer reviewed

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    Authors: C. H. Whaley; R. Mahmood; R. Mahmood; K. von Salzen; +57 Authors

    Assessments from the Russian ship-based campaign were performed with the support of RFBR project no. 20-55-12001 and according to the development program of the Interdisciplinary Scientific and Educational School of M.V. Lomonosov Moscow State University “Future Planet and Global Environmental Change”. Development of the methodology for aethalometric data treatment was supported by RSF project no. 19-77-30004. The BC observations on R/V Mirai were supported by the Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan (Arctic Challenge for Sustainability (ArCS) project). Contributions by SMHI were funded by the Swedish Environmental Protection Agency under contract NV-03174-20 and the Swedish Climate and Clean Air Research program (SCAC) as well as partly by the Swedish National Space Board (NORD-SLCP, grant agreement ID: 94/16) and the EU Horizon 2020 project Integrated Arctic Observing System (INTAROS, grant agreement ID: 727890). Work on ACE-FTS analysis was supported by the Natural Sciences and Engineering Research Council of Canada (NSERC). Julia Schmale received funding from the Swiss National Science Foundation (project no. 200021_188478). Duncan Watson-Parris received funding from NERC projects NE/P013406/1 (A-CURE) and NE/S005390/1 (ACRUISE) as well as funding from the European Union's Horizon 2020 research and innovation program iMIRACLI under Marie Skłodowska-Curie grant agreement no. 860100. LATMOS has been supported by the EU iCUPE (Integrating and Comprehensive Understanding on Polar Environments) project (grant agreement no. 689443) under the European Network for Observing our Changing Planet (ERA-Planet), as well as access to IDRIS HPC resources (GENCI allocation A009017141) and the IPSL mesoscale computing center (CICLAD: Calcul Intensif pour le CLimat, l’Atmosphère et la Dynamique) for model simulations. Naga Oshima was supported by the Japan Society for the Promotion of Science KAKENHI (grant nos. JP18H03363, JP18H05292, and JP21H03582), the Environment Research and Technology Development Fund (grant nos. JPMEERF20202003 and JPMEERF20205001) of the Environmental Restoration and Conservation Agency of Japan, the Arctic Challenge for Sustainability II (ArCS II) under program grant no. JPMXD1420318865, and a grant for the Global Environmental Research Coordination System from the Ministry of the Environment, Japan (MLIT1753). The research with GISS-E2.1 has been supported by the Aarhus University Interdisciplinary Centre for Climate Change (iClimate) OH fund (no. 2020-0162731), the FREYA project funded by the Nordic Council of Ministers (grant agreement nos. MST-227-00036 and MFVM-2019-13476), and the EVAM-SLCF funded by the Danish Environmental Agency (grant agreement no. MST-112-00298). Jesper Christensen (for DEHM model) received funding from the Danish Environmental Protection Agency (DANCEA funds for Environmental Support to the Arctic Region project; grant no. 2019-7975). Maria Sand has been supported by the Research Council of Norway (grant 315195, ACCEPT). While carbon dioxide is the main cause for global warming, modeling short-lived climate forcers (SLCFs) such as methane, ozone, and particles in the Arctic allows us to simulate near-term climate and health impacts for a sensitive, pristine region that is warming at 3 times the global rate. Atmospheric modeling is critical for understanding the long-range transport of pollutants to the Arctic, as well as the abundance and distribution of SLCFs throughout the Arctic atmosphere. Modeling is also used as a tool to determine SLCF impacts on climate and health in the present and in future emissions scenarios. In this study, we evaluate 18 state-of-the-art atmospheric and Earth system models by assessing their representation of Arctic and Northern Hemisphere atmospheric SLCF distributions, considering a wide range of different chemical species (methane, tropospheric ozone and its precursors, black carbon, sulfate, organic aerosol, and particulate matter) and multiple observational datasets. Model simulations over 4 years (2008–2009 and 2014–2015) conducted for the 2022 Arctic Monitoring and Assessment Programme (AMAP) SLCF assessment report are thoroughly evaluated against satellite, ground, ship, and aircraft-based observations. The annual means, seasonal cycles, and 3-D distributions of SLCFs were evaluated using several metrics, such as absolute and percent model biases and correlation coefficients. The results show a large range in model performance, with no one particular model or model type performing well for all regions and all SLCF species. The multi-model mean (mmm) was able to represent the general features of SLCFs in the Arctic and had the best overall performance. For the SLCFs with the greatest radiative impact (CH4, O3, BC, and SO), the mmm was within ±25 % of the measurements across the Northern Hemisphere. Therefore, we recommend a multi-model ensemble be used for simulating climate and health impacts of SLCFs. Of the SLCFs in our study, model biases were smallest for CH4 and greatest for OA. For most SLCFs, model biases skewed from positive to negative with increasing latitude. Our analysis suggests that vertical mixing, long-range transport, deposition, and wildfires remain highly uncertain processes. These processes need better representation within atmospheric models to improve their simulation of SLCFs in the Arctic environment. As model development proceeds in these areas, we highly recommend that the vertical and 3-D distribution of SLCFs be evaluated, as that information is critical to improving the uncertain processes in models. "Article signat per més de 50 autors/es: Cynthia H. Whaley, Rashed Mahmood, Knut von Salzen, Barbara Winter, Sabine Eckhardt, Stephen Arnold, Stephen Beagley, Silvia Becagli, Rong-You Chien, Jesper Christensen, Sujay Manish Damani, Xinyi Dong, Konstantinos Eleftheriadis, Nikolaos Evangeliou, Gregory Faluvegi, Mark Flanner, Joshua S. Fu, Michael Gauss, Fabio Giardi, Wanmin Gong, Jens Liengaard Hjorth, Lin Huang, Ulas Im, Yugo Kanaya, Srinath Krishnan, Zbigniew Klimont, Thomas Kühn, Joakim Langner, Kathy S. Law, Louis Marelle, Andreas Massling, Dirk Olivié, Tatsuo Onishi, Naga Oshima, Yiran Peng, David A. Plummer, Olga Popovicheva, Luca Pozzoli, Jean-Christophe Raut, Maria Sand, Laura N. Saunders, Julia Schmale, Sangeeta Sharma, Ragnhild Bieltvedt Skeie, Henrik Skov, Fumikazu Taketani, Manu A. Thomas, Rita Traversi, Kostas Tsigaridis, Svetlana Tsyro, Steven Turnock, Vito Vitale, Kaley A. Walker, Minqi Wang, Duncan Watson-Parris, and Tahya Weiss-Gibbons " Peer Reviewed

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    NILU Brage
    Article . 2022
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    Atmospheric Chemistry and Physics
    Article . 2022
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    Recolector de Ciencia Abierta, RECOLECTA
    Article . 2022 . Peer-reviewed
    License: CC BY
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    Authors: Vaios Moschos; Katja Dzepina; Deepika Bhattu; Houssni Lamkaddam; +30 Authors

    Organic aerosols in the Arctic are predominantly fuelled by anthropogenic sources in winter and natural sources in summer, according to observations from eight sites across the Arctic Aerosols play an important yet uncertain role in modulating the radiation balance of the sensitive Arctic atmosphere. Organic aerosol is one of the most abundant, yet least understood, fractions of the Arctic aerosol mass. Here we use data from eight observatories that represent the entire Arctic to reveal the annual cycles in anthropogenic and biogenic sources of organic aerosol. We show that during winter, the organic aerosol in the Arctic is dominated by anthropogenic emissions, mainly from Eurasia, which consist of both direct combustion emissions and long-range transported, aged pollution. In summer, the decreasing anthropogenic pollution is replaced by natural emissions. These include marine secondary, biogenic secondary and primary biological emissions, which have the potential to be important to Arctic climate by modifying the cloud condensation nuclei properties and acting as ice-nucleating particles. Their source strength or atmospheric processing is sensitive to nutrient availability, solar radiation, temperature and snow cover. Our results provide a comprehensive understanding of the current pan-Arctic organic aerosol, which can be used to support modelling efforts that aim to quantify the climate impacts of emissions in this sensitive region. Peer reviewed

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    Nature Geoscience
    Other literature type . Article . 2022 . Peer-reviewed
    License: CC BY
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    Nature Geoscience
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    NILU Brage
    Article . 2022
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      image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/ Flore (Florence Rese...arrow_drop_down
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      Nature Geoscience
      Other literature type . Article . 2022 . Peer-reviewed
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      NILU Brage
      Article . 2022
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    Authors: De Vito-Francesco, Elisabetta; Farinelli, Alessandro; Yang, Qiuyue; Nagar, Bhawna; +7 Authors

    Smart monitoring has been studied and developed in recent years to create faster, cheaper, and more user-friendly on-site methods. The present study describes an innovative technology for investigative monitoring of heavy metal pollution (Cu and Pb) in surface water. It is composed of an autonomous surface vehicle capable of semiautonomous driving and equipped with a microfluidic device for detection of heavy metals. Detection is based on the method of square wave anodic stripping voltammetry using carbon-based screen-printed electrodes (SPEs). The focus of this work was to validate the ability of the integrated system to perform on-site detection of heavy metal pollution plumes in river catchments. This scenario was simulated in laboratory experiments. The main performance characteristics of the system, which was evaluated based on ISO 15839 were measurement bias (Pb 75%, Cu 65%), reproducibility (in terms of relative standard deviation: Pb 11–18%, Cu 6–10%) and the limit of detection (4 µg/L for Pb and 7 µg/L for Cu). The lowest detectable change (LDC), which is an important performance characteristic for this application, was estimated to be 4–5 µg/L for Pb and 6–7 µg/L for Cu. The life span of an SPE averaged 39 measurements per day, which is considered sufficient for intended monitoring campaigns. This work demonstrated the suitability of the integrated system for on-site detection of Pb and Cu emissions from large and medium urban areas discharging into small water bodies. Open access funding provided by University of Natural Resources and Life Sciences Vienna (BOKU). The research leading to the presented results received funding from the research project INTCATCH 2020, “Development and application of Novel, Integrated Tools for monitoring and managing Catchments” supported by the European Union’s Horizon 2020 research and innovation programme, under the grant agreement No. 689341. The ICN2 is funded by the CERCA Programme/Generalitat de Catalunya. The ICN2 is supported by the Severo Ochoa program of the Spanish Ministry of Economy, Industry, and Competitiveness (MINECO, Grant No. SEV-2017–0706).

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    Environmental Monitoring and Assessment
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      image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/ Europe PubMed Centra...arrow_drop_down
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      Environmental Monitoring and Assessment
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    Authors: Wünsch, Robin;

    Micropollutants (MP) such as residues of pharmaceuticals, industrial chemicals or pesticides can be detected in almost all water resources. Various processes can be used to abate them in drinking water treatment, e.g., ozonation, advanced oxidation processes (AOP), adsorption on activated carbon or membrane filtration. The selection of a suitable process combination is a complex task for water suppliers. This thesis compares two process chains in the context of a multi-barrier system including managed aquifer recharge (MAR). To protect soils and aquifers from MP in the future, an additional barrier against MP upstream of the MAR was investigated: (1) a full-stream treatment using the AOP UV/H2O2, and (2) a side-stream treatment with low-pressure reverse osmosis (LPRO) or nanofiltration (NF) and ozonation of the retentate to treat the concentrated MPs. Pilot-scale experiments were conducted to determine the relative abatements of MP by UV/H2O2 treatment and by a subsequent soil column treatment. Compared to a soil column fed with water without UV/H2O2 pretreatment, the performance of the combined process (UV/H2O2 + soil column) was more efficient. However, this could be explained by an additive effect of the individual processes. Relative abatements in the UV/H2O2 process are mainly based on the introduced UV fluence and hydroxyl radical exposure. These parameters could be calculated with a model based on the measured relative abatements of two MPs (probe compounds) and their kinetic data (second-order rate constants for the reactions with hydroxyl radical, absorbance and quantum yield). With this information, the relative abatements of other MPs could be predicted with an accuracy of ±20%. A sensitivity analysis of the model showed that the relative abatements of the selected probe compounds should be >50%. In this case, the accuracy of the calculated parameters depends mainly on the precision of the kinetic data. In the case of membrane-based treatment of water by LPRO or NF, a concentrate is produced. Ozonation to treat MP in the concentrate is accompanied by a formation of the possibly carcinogenic bromate by oxidation of bromide. To achieve the highest possible MP abatement with simultaneously low bromate formation, both membrane selection and subsequent concentrate ozonation were investigated. In laboratory tests with standardized concentrates, neither the water source nor the membrane type caused a change in bromate yield for similar relative MP abatements. However, NF membranes have lower relative retentions of bromide and MP than LPRO membranes, making NF concentrates more suitable for ozonation with limited bromate formation. A comparison of UV/H2O2 with membrane treatment showed that full-stream treatment with UV/H2O2 has about four times lower costs and an about five times lower environmental impact. In addition it achieves significantly higher disinfection. In contrast, side-stream treatment with LPRO causes up to two times lower impacts for the environment when the electrical energy source is wind or hydropower. This study thus contributes technical, economic, and environmental aspects to a holistic evaluation of the two process options.

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    https://doi.org/10.5075/epfl-t...
    Other literature type . 2022
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      https://doi.org/10.5075/epfl-t...
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    Authors: Moschos, Vaios; Schmale, Julia; Aas, Wenche; Becagli, Silvia; +23 Authors

    The Arctic is warming two to three times faster than the global average, and the role of aerosols is not well constrained. Aerosol number concentrations can be very low in remote environments, rendering local cloud radiative properties highly sensitive to available aerosol. The composition and sources of the climate-relevant aerosols, affecting Arctic cloud formation and altering their microphysics, remain largely elusive due to a lack of harmonized concurrent multi-component, multi-site, and multi-season observations. Here, we present a dataset on the overall chemical composition and seasonal variability of the Arctic total particulate matter (with a size cut at 10 mu m, PM10, or without any size cut) at eight observatories representing all Arctic sectors. Our holistic observational approach includes the Russian Arctic, a significant emission source area with less dedicated aerosol monitoring, and extends beyond the more traditionally studied summer period and black carbon/sulfate or fine-mode pollutants. The major airborne Arctic PM components in terms of dry mass are sea salt, secondary (non-sea-salt, nss) sulfate, and organic aerosol (OA), with minor contributions from elemental carbon (EC) and ammonium. We observe substantial spatiotemporal variability in component ratios, such as EC/OA, ammonium/nss-sulfate and OA/nss-sulfate, and fractional contributions to PM. When combined with component-specific back-trajectory analysis to identify marine or terrestrial origins, as well as the companion study by Moschos et al 2022 Nat. Geosci. focusing on OA, the composition analysis provides policy-guiding observational insights into sector-based differences in natural and anthropogenic Arctic aerosol sources. In this regard, we first reveal major source regions of inner-Arctic sea salt, biogenic sulfate, and natural organics, and highlight an underappreciated wintertime source of primary carbonaceous aerosols (EC and OA) in West Siberia, potentially associated with the oil and gas sector. The presented dataset can assist in reducing uncertainties in modelling pan-Arctic aerosol-climate interactions, as the major contributors to yearly aerosol mass can be constrained. These models can then be used to predict the future evolution of individual inner-Arctic atmospheric PM components in light of current and emerging pollution mitigation measures and improved region-specific emission inventories. Peer reviewed

    image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/ Flore (Florence Rese...arrow_drop_down
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    NILU Brage
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    image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
    image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
    image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
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    Environmental Research Letters
    Article . 2022
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      Environmental Research Letters
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    Authors: Beatriz Ferreira Araujo; Stefan Osterwalder; Natalie Szponar; Domenica Lee; +19 Authors

    During Arctic springtime, halogen radicals oxidize atmospheric elemental mercury (Hg-0), which deposits to the cryosphere. This is followed by a summertime atmospheric Hg-0 peak that is thought to result mostly from terrestrial Hg inputs to the Arctic Ocean, followed by photoreduction and emission to air. The large terrestrial Hg contribution to the Arctic Ocean and global atmosphere has raised concern over the potential release of permafrost Hg, via rivers and coastal erosion, with Arctic warming. Here we investigate Hg isotope variability of Arctic atmospheric, marine, and terrestrial Hg. We observe highly characteristic Hg isotope signatures during the summertime peak that reflect re-emission of Hg deposited to the cryosphere during spring. Air mass back trajectories support a cryospheric Hg emission source but no major terrestrial source. This implies that terrestrial Hg inputs to the Arctic Ocean remain in the marine ecosystem, without substantial loss to the global atmosphere, but with possible effects on food webs.Arctic warming thaws permafrost, leading to enhanced soil mercury transport to the Arctic Ocean. Mercury isotope signatures in arctic rivers, ocean and atmosphere suggest that permafrost mercury is buried in marine sediment and not emitted to the global atmosphere Peer reviewed

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    Nature Communications
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    Research Collection
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    Authors: Leinonen, Ville; Kokkola, Harri; Yli-Juuti, Taina; Mielonen, Tero; +32 Authors

    Despite a large number of studies, out of all drivers of radiative forcing, the effect of aerosols has the largest uncertainty in global climate model radiative forcing estimates. There have been studies of aerosol optical properties in climate models, but the effects of particle number size distribution need a more thorough inspection. We investigated the trends and seasonality of particle number concentrations in nucleation, Aitken, and accumulation modes at 21 measurement sites in Europe and the Arctic. For 13 of those sites, with longer measurement time series, we compared the field observations with the results from five climate models, namely EC-Earth3, ECHAM-M7, ECHAM-SALSA, NorESM1.2, and UKESM1. This is the first extensive comparison of detailed aerosol size distribution trends between in situ observations from Europe and five earth system models (ESMs). We found that the trends of particle number concentrations were mostly consistent and decreasing in both measurements and models. However, for many sites, climate models showed weaker decreasing trends than the measurements. Seasonal variability in measured number concentrations, quantified by the ratio between maximum and minimum monthly number concentration, was typically stronger at northern measurement sites compared to other locations. Models had large differences in their seasonal representation, and they can be roughly divided into two categories: for EC-Earth and NorESM, the seasonal cycle was relatively similar for all sites, and for other models the pattern of seasonality varied between northern and southern sites. In addition, the variability in concentrations across sites varied between models, some having relatively similar concentrations for all sites, whereas others showed clear differences in concentrations between remote and urban sites. To conclude, although all of the model simulations had identical input data to describe anthropogenic mass emissions, trends in differently sized particles vary among the models due to assumptions in emission sizes and differences in how models treat size-dependent aerosol processes. The inter-model variability was largest in the accumulation mode, i.e. sizes which have implications for aerosol-cloud interactions. Our analysis also indicates that between models there is a large variation in efficiency of long-range transportation of aerosols to remote locations. The differences in model results are most likely due to the more complex effect of different processes instead of one specific feature (e.g. the representation of aerosol or emission size distributions). Hence, a more detailed characterization of microphysical processes and deposition processes affecting the long-range transport is needed to understand the model variability. Peer reviewed

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    NILU Brage
    Article . 2022
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      NILU Brage
      Article . 2022
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    Authors: Shupe, Matthew D.; Rex, Markus; Blomquist, Byron; Persson, P. Ola G.; +110 Authors

    With the Arctic rapidly changing, the needs to observe, understand, and model the changes are essential. To support these needs, an annual cycle of observations of atmospheric properties, processes, and interactions were made while drifting with the sea ice across the central Arctic during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition from October 2019 to September 2020. An international team designed and implemented the comprehensive program to document and characterize all aspects of the Arctic atmospheric system in unprecedented detail, using a variety of approaches, and across multiple scales. These measurements were coordinated with other observational teams to explore crosscutting and coupled interactions with the Arctic Ocean, sea ice, and ecosystem through a variety of physical and biogeochemical processes. This overview outlines the breadth and complexity of the atmospheric research program, which was organized into 4 subgroups: atmospheric state, clouds and precipitation, gases and aerosols, and energy budgets. Atmospheric variability over the annual cycle revealed important influences from a persistent large-scale winter circulation pattern, leading to some storms with pressure and winds that were outside the interquartile range of past conditions suggested by long-term reanalysis. Similarly, the MOSAiC location was warmer and wetter in summer than the reanalysis climatology, in part due to its close proximity to the sea ice edge.The comprehensiveness of the observational program for characterizing and analyzing atmospheric phenomena is demonstrated via a winter case study examining air mass transitions and a summer case study examining vertical atmospheric evolution. Overall, the MOSAiC atmospheric program successfully met its objectives and was the most comprehensive atmospheric measurement program to date conducted over the Arctic sea ice. The obtained data will support a broad range of coupled-system scientific research and provide an important foundation for advancing multiscale modeling capabilities in the Arctic. International audience

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    NARCIS; Research@WUR
    Article . 2022
    License: CC BY
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    Elementa: Science of the Anthropocene
    Article
    License: CC BY
    Data sources: UnpayWall
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    Hyper Article en Ligne
    Other literature type . 2022
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  • image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
    Authors: X. Faïn; D. M. Etheridge; D. M. Etheridge; K. Fourteau; +20 Authors

    Abstract. Carbon monoxide (CO) is a naturally occurring atmospheric trace gas, a regulated pollutant, and one of the main components determining the oxidative capacity of the atmosphere. Evaluating climate–chemistry models under different conditions than today and constraining past CO sources requires a reliable record of atmospheric CO mixing ratios ([CO]) that includes data since preindustrial times. Here, we report the first continuous record of atmospheric [CO] for Southern Hemisphere (SH) high latitudes over the past 3 millennia. Our continuous record is a composite of three high-resolution Antarctic ice core gas records and firn air measurements from seven Antarctic locations. The ice core gas [CO] records were measured by continuous flow analysis (CFA), using an optical feedback cavity-enhanced absorption spectrometer (OF-CEAS), achieving excellent external precision (2.8–8.8 ppb; 2σ) and consistently low blanks (ranging from 4.1±1.2 to 7.4±1.4 ppb), thus enabling paleo-atmospheric interpretations. Six new firn air [CO] Antarctic datasets collected between 1993 and 2016 CE at the DE08-2, DSSW19K, DSSW20K, South Pole, Aurora Basin North (ABN), and Lock-In sites (and one previously published firn CO dataset at Berkner) were used to reconstruct the atmospheric history of CO from ∼1897 CE, using inverse modeling that incorporates the influence of gas transport in firn. Excellent consistency was observed between the youngest ice core gas [CO] and the [CO] from the base of the firn and between the recent firn [CO] and atmospheric [CO] measurements at Mawson station (eastern Antarctica), yielding a consistent and contiguous record of CO across these different archives. Our Antarctic [CO] record is relatively stable from −835 to 1500 CE, with mixing ratios within a 30–45 ppb range (2σ). There is a ∼5 ppb decrease in [CO] to a minimum at around 1700 CE during the Little Ice Age. CO mixing ratios then increase over time to reach a maximum of ∼54 ppb by ∼1985 CE. Most of the industrial period [CO] growth occurred between about 1940 to 1985 CE, after which there was an overall [CO] decrease, as observed in Greenland firn air and later at atmospheric monitoring sites and attributed partly to reduced CO emissions from combustion sources. Our Antarctic ice core gas CO observations differ from previously published records in two key aspects. First, our mixing ratios are significantly lower than reported previously, suggesting that previous studies underestimated blank contributions. Second, our new CO record does not show a maximum in the late 1800s. The absence of a [CO] peak around the turn of the century argues against there being a peak in Southern Hemisphere biomass burning at this time, which is in agreement with (i) other paleofire proxies such as ethane or acetylene and (ii) conclusions reached by paleofire modeling. The combined ice core and firn air [CO] history, spanning −835 to 1992 CE, extended to the present by the Mawson atmospheric record, provides a useful benchmark for future atmospheric chemistry modeling studies. International audience

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    Climate of the Past (CP)
    Article . 2023 . Peer-reviewed
    License: CC BY
    Data sources: Crossref
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    https://doi.org/10.5194/cp-202...
    Preprint . 2023 . Peer-reviewed
    License: CC BY
    Data sources: Crossref
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    Climate of the Past
    Article . 2023
    Data sources: DOAJ
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    Apollo
    Article . 2023
    License: CC BY
    Data sources: Apollo
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    Climate of the Past (CP)
    Other literature type . 2023
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      Climate of the Past (CP)
      Article . 2023 . Peer-reviewed
      License: CC BY
      Data sources: Crossref
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      https://doi.org/10.5194/cp-202...
      Preprint . 2023 . Peer-reviewed
      License: CC BY
      Data sources: Crossref
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      Climate of the Past
      Article . 2023
      Data sources: DOAJ
      image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
      Apollo
      Article . 2023
      License: CC BY
      Data sources: Apollo
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      Climate of the Past (CP)
      Other literature type . 2023
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    Authors: Nuria Benavent; Anoop S. Mahajan; Qinyi Li; Carlos A. Cuevas; +30 Authors

    This study received funding from the European Research Council Executive Agency under the European Union’s Horizon 2020 Research and Innovation Program (project ERC‐2016‐COG 726349 CLIMAHAL and ERC-2016-STG 714621 GASPARCON) and the European Commission via the EMME-CARE project and was supported by the Consejo Superior de Investigaciones Científicas of Spain. This work was supported by the European Union’s Horizon 2020 Research and Innovation Programme under grant agreement no. 856612 and the Academy of Finland (project no. 334514). The Indian Institute of Tropical Meteorology is funded by the Ministry of Earth Sciences, Government of India. Ozone, CO, CH4 and AMS measurements were funded by the Swiss National Science Foundation (grant 200021_188478), the Swiss Polar Institute and U.S. National Science Foundation grants 1914781 and 1807163. J.S. holds the Ingvar Kamprad chair for extreme environments research, sponsored by Ferring Pharmaceuticals. Data reported in this manuscript were produced as part of the international MOSAiC expedition with tag MOSAiC20192020, with activities supported by Polarstern expedition AWI-PS122_00. H.S. was funded by the European ERA-PLANET projects iGOSP and iCUPE (consortium agreement no. 689443 for both projects). We thank FORMAS and the Swedish Polar Research Secretariat for support. We gratefully acknowledge funding by the Deutsche Forschungsgemeinschaft (project no. 268020496 – TRR 172) within the Transregional Collaborative Research Center ‘ArctiC Amplification: Climate Relevant Atmospheric and SurfaCe Processes, and Feedback Mechanisms (AC)3’ in subproject C03. We thank I. Bourgeois (NOAA/CIRES) for providing the ATom NOx data. Unlike bromine, the effect of iodine chemistry on the Arctic surface ozone budget is poorly constrained. We present ship-based measurements of halogen oxides in the high Arctic boundary layer from the sunlit period of March to October 2020 and show that iodine enhances springtime tropospheric ozone depletion. We find that chemical reactions between iodine and ozone are the second highest contributor to ozone loss over the study period, after ozone photolysis-initiated loss and ahead of bromine. 6 pags., 2 figs. Peer reviewed

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    Authors: C. H. Whaley; R. Mahmood; R. Mahmood; K. von Salzen; +57 Authors

    Assessments from the Russian ship-based campaign were performed with the support of RFBR project no. 20-55-12001 and according to the development program of the Interdisciplinary Scientific and Educational School of M.V. Lomonosov Moscow State University “Future Planet and Global Environmental Change”. Development of the methodology for aethalometric data treatment was supported by RSF project no. 19-77-30004. The BC observations on R/V Mirai were supported by the Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan (Arctic Challenge for Sustainability (ArCS) project). Contributions by SMHI were funded by the Swedish Environmental Protection Agency under contract NV-03174-20 and the Swedish Climate and Clean Air Research program (SCAC) as well as partly by the Swedish National Space Board (NORD-SLCP, grant agreement ID: 94/16) and the EU Horizon 2020 project Integrated Arctic Observing System (INTAROS, grant agreement ID: 727890). Work on ACE-FTS analysis was supported by the Natural Sciences and Engineering Research Council of Canada (NSERC). Julia Schmale received funding from the Swiss National Science Foundation (project no. 200021_188478). Duncan Watson-Parris received funding from NERC projects NE/P013406/1 (A-CURE) and NE/S005390/1 (ACRUISE) as well as funding from the European Union's Horizon 2020 research and innovation program iMIRACLI under Marie Skłodowska-Curie grant agreement no. 860100. LATMOS has been supported by the EU iCUPE (Integrating and Comprehensive Understanding on Polar Environments) project (grant agreement no. 689443) under the European Network for Observing our Changing Planet (ERA-Planet), as well as access to IDRIS HPC resources (GENCI allocation A009017141) and the IPSL mesoscale computing center (CICLAD: Calcul Intensif pour le CLimat, l’Atmosphère et la Dynamique) for model simulations. Naga Oshima was supported by the Japan Society for the Promotion of Science KAKENHI (grant nos. JP18H03363, JP18H05292, and JP21H03582), the Environment Research and Technology Development Fund (grant nos. JPMEERF20202003 and JPMEERF20205001) of the Environmental Restoration and Conservation Agency of Japan, the Arctic Challenge for Sustainability II (ArCS II) under program grant no. JPMXD1420318865, and a grant for the Global Environmental Research Coordination System from the Ministry of the Environment, Japan (MLIT1753). The research with GISS-E2.1 has been supported by the Aarhus University Interdisciplinary Centre for Climate Change (iClimate) OH fund (no. 2020-0162731), the FREYA project funded by the Nordic Council of Ministers (grant agreement nos. MST-227-00036 and MFVM-2019-13476), and the EVAM-SLCF funded by the Danish Environmental Agency (grant agreement no. MST-112-00298). Jesper Christensen (for DEHM model) received funding from the Danish Environmental Protection Agency (DANCEA funds for Environmental Support to the Arctic Region project; grant no. 2019-7975). Maria Sand has been supported by the Research Council of Norway (grant 315195, ACCEPT). While carbon dioxide is the main cause for global warming, modeling short-lived climate forcers (SLCFs) such as methane, ozone, and particles in the Arctic allows us to simulate near-term climate and health impacts for a sensitive, pristine region that is warming at 3 times the global rate. Atmospheric modeling is critical for understanding the long-range transport of pollutants to the Arctic, as well as the abundance and distribution of SLCFs throughout the Arctic atmosphere. Modeling is also used as a tool to determine SLCF impacts on climate and health in the present and in future emissions scenarios. In this study, we evaluate 18 state-of-the-art atmospheric and Earth system models by assessing their representation of Arctic and Northern Hemisphere atmospheric SLCF distributions, considering a wide range of different chemical species (methane, tropospheric ozone and its precursors, black carbon, sulfate, organic aerosol, and particulate matter) and multiple observational datasets. Model simulations over 4 years (2008–2009 and 2014–2015) conducted for the 2022 Arctic Monitoring and Assessment Programme (AMAP) SLCF assessment report are thoroughly evaluated against satellite, ground, ship, and aircraft-based observations. The annual means, seasonal cycles, and 3-D distributions of SLCFs were evaluated using several metrics, such as absolute and percent model biases and correlation coefficients. The results show a large range in model performance, with no one particular model or model type performing well for all regions and all SLCF species. The multi-model mean (mmm) was able to represent the general features of SLCFs in the Arctic and had the best overall performance. For the SLCFs with the greatest radiative impact (CH4, O3, BC, and SO), the mmm was within ±25 % of the measurements across the Northern Hemisphere. Therefore, we recommend a multi-model ensemble be used for simulating climate and health impacts of SLCFs. Of the SLCFs in our study, model biases were smallest for CH4 and greatest for OA. For most SLCFs, model biases skewed from positive to negative with increasing latitude. Our analysis suggests that vertical mixing, long-range transport, deposition, and wildfires remain highly uncertain processes. These processes need better representation within atmospheric models to improve their simulation of SLCFs in the Arctic environment. As model development proceeds in these areas, we highly recommend that the vertical and 3-D distribution of SLCFs be evaluated, as that information is critical to improving the uncertain processes in models. "Article signat per més de 50 autors/es: Cynthia H. Whaley, Rashed Mahmood, Knut von Salzen, Barbara Winter, Sabine Eckhardt, Stephen Arnold, Stephen Beagley, Silvia Becagli, Rong-You Chien, Jesper Christensen, Sujay Manish Damani, Xinyi Dong, Konstantinos Eleftheriadis, Nikolaos Evangeliou, Gregory Faluvegi, Mark Flanner, Joshua S. Fu, Michael Gauss, Fabio Giardi, Wanmin Gong, Jens Liengaard Hjorth, Lin Huang, Ulas Im, Yugo Kanaya, Srinath Krishnan, Zbigniew Klimont, Thomas Kühn, Joakim Langner, Kathy S. Law, Louis Marelle, Andreas Massling, Dirk Olivié, Tatsuo Onishi, Naga Oshima, Yiran Peng, David A. Plummer, Olga Popovicheva, Luca Pozzoli, Jean-Christophe Raut, Maria Sand, Laura N. Saunders, Julia Schmale, Sangeeta Sharma, Ragnhild Bieltvedt Skeie, Henrik Skov, Fumikazu Taketani, Manu A. Thomas, Rita Traversi, Kostas Tsigaridis, Svetlana Tsyro, Steven Turnock, Vito Vitale, Kaley A. Walker, Minqi Wang, Duncan Watson-Parris, and Tahya Weiss-Gibbons " Peer Reviewed

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    NILU Brage
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    Recolector de Ciencia Abierta, RECOLECTA
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    Authors: Vaios Moschos; Katja Dzepina; Deepika Bhattu; Houssni Lamkaddam; +30 Authors

    Organic aerosols in the Arctic are predominantly fuelled by anthropogenic sources in winter and natural sources in summer, according to observations from eight sites across the Arctic Aerosols play an important yet uncertain role in modulating the radiation balance of the sensitive Arctic atmosphere. Organic aerosol is one of the most abundant, yet least understood, fractions of the Arctic aerosol mass. Here we use data from eight observatories that represent the entire Arctic to reveal the annual cycles in anthropogenic and biogenic sources of organic aerosol. We show that during winter, the organic aerosol in the Arctic is dominated by anthropogenic emissions, mainly from Eurasia, which consist of both direct combustion emissions and long-range transported, aged pollution. In summer, the decreasing anthropogenic pollution is replaced by natural emissions. These include marine secondary, biogenic secondary and primary biological emissions, which have the potential to be important to Arctic climate by modifying the cloud condensation nuclei properties and acting as ice-nucleating particles. Their source strength or atmospheric processing is sensitive to nutrient availability, solar radiation, temperature and snow cover. Our results provide a comprehensive understanding of the current pan-Arctic organic aerosol, which can be used to support modelling efforts that aim to quantify the climate impacts of emissions in this sensitive region. Peer reviewed

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    Nature Geoscience
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      Nature Geoscience
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      Article . 2022
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    Authors: De Vito-Francesco, Elisabetta; Farinelli, Alessandro; Yang, Qiuyue; Nagar, Bhawna; +7 Authors

    Smart monitoring has been studied and developed in recent years to create faster, cheaper, and more user-friendly on-site methods. The present study describes an innovative technology for investigative monitoring of heavy metal pollution (Cu and Pb) in surface water. It is composed of an autonomous surface vehicle capable of semiautonomous driving and equipped with a microfluidic device for detection of heavy metals. Detection is based on the method of square wave anodic stripping voltammetry using carbon-based screen-printed electrodes (SPEs). The focus of this work was to validate the ability of the integrated system to perform on-site detection of heavy metal pollution plumes in river catchments. This scenario was simulated in laboratory experiments. The main performance characteristics of the system, which was evaluated based on ISO 15839 were measurement bias (Pb 75%, Cu 65%), reproducibility (in terms of relative standard deviation: Pb 11–18%, Cu 6–10%) and the limit of detection (4 µg/L for Pb and 7 µg/L for Cu). The lowest detectable change (LDC), which is an important performance characteristic for this application, was estimated to be 4–5 µg/L for Pb and 6–7 µg/L for Cu. The life span of an SPE averaged 39 measurements per day, which is considered sufficient for intended monitoring campaigns. This work demonstrated the suitability of the integrated system for on-site detection of Pb and Cu emissions from large and medium urban areas discharging into small water bodies. Open access funding provided by University of Natural Resources and Life Sciences Vienna (BOKU). The research leading to the presented results received funding from the research project INTCATCH 2020, “Development and application of Novel, Integrated Tools for monitoring and managing Catchments” supported by the European Union’s Horizon 2020 research and innovation programme, under the grant agreement No. 689341. The ICN2 is funded by the CERCA Programme/Generalitat de Catalunya. The ICN2 is supported by the Severo Ochoa program of the Spanish Ministry of Economy, Industry, and Competitiveness (MINECO, Grant No. SEV-2017–0706).

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    Environmental Monitoring and Assessment
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      Environmental Monitoring and Assessment
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    Authors: Wünsch, Robin;

    Micropollutants (MP) such as residues of pharmaceuticals, industrial chemicals or pesticides can be detected in almost all water resources. Various processes can be used to abate them in drinking water treatment, e.g., ozonation, advanced oxidation processes (AOP), adsorption on activated carbon or membrane filtration. The selection of a suitable process combination is a complex task for water suppliers. This thesis compares two process chains in the context of a multi-barrier system including managed aquifer recharge (MAR). To protect soils and aquifers from MP in the future, an additional barrier against MP upstream of the MAR was investigated: (1) a full-stream treatment using the AOP UV/H2O2, and (2) a side-stream treatment with low-pressure reverse osmosis (LPRO) or nanofiltration (NF) and ozonation of the retentate to treat the concentrated MPs. Pilot-scale experiments were conducted to determine the relative abatements of MP by UV/H2O2 treatment and by a subsequent soil column treatment. Compared to a soil column fed with water without UV/H2O2 pretreatment, the performance of the combined process (UV/H2O2 + soil column) was more efficient. However, this could be explained by an additive effect of the individual processes. Relative abatements in the UV/H2O2 process are mainly based on the introduced UV fluence and hydroxyl radical exposure. These parameters could be calculated with a model based on the measured relative abatements of two MPs (probe compounds) and their kinetic data (second-order rate constants for the reactions with hydroxyl radical, absorbance and quantum yield). With this information, the relative abatements of other MPs could be predicted with an accuracy of ±20%. A sensitivity analysis of the model showed that the relative abatements of the selected probe compounds should be >50%. In this case, the accuracy of the calculated parameters depends mainly on the precision of the kinetic data. In the case of membrane-based treatment of water by LPRO or NF, a concentrate is produced. Ozonation to treat MP in the concentrate is accompanied by a formation of the possibly carcinogenic bromate by oxidation of bromide. To achieve the highest possible MP abatement with simultaneously low bromate formation, both membrane selection and subsequent concentrate ozonation were investigated. In laboratory tests with standardized concentrates, neither the water source nor the membrane type caused a change in bromate yield for similar relative MP abatements. However, NF membranes have lower relative retentions of bromide and MP than LPRO membranes, making NF concentrates more suitable for ozonation with limited bromate formation. A comparison of UV/H2O2 with membrane treatment showed that full-stream treatment with UV/H2O2 has about four times lower costs and an about five times lower environmental impact. In addition it achieves significantly higher disinfection. In contrast, side-stream treatment with LPRO causes up to two times lower impacts for the environment when the electrical energy source is wind or hydropower. This study thus contributes technical, economic, and environmental aspects to a holistic evaluation of the two process options.

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    https://doi.org/10.5075/epfl-t...
    Other literature type . 2022
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      https://doi.org/10.5075/epfl-t...
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    Authors: Moschos, Vaios; Schmale, Julia; Aas, Wenche; Becagli, Silvia; +23 Authors

    The Arctic is warming two to three times faster than the global average, and the role of aerosols is not well constrained. Aerosol number concentrations can be very low in remote environments, rendering local cloud radiative properties highly sensitive to available aerosol. The composition and sources of the climate-relevant aerosols, affecting Arctic cloud formation and altering their microphysics, remain largely elusive due to a lack of harmonized concurrent multi-component, multi-site, and multi-season observations. Here, we present a dataset on the overall chemical composition and seasonal variability of the Arctic total particulate matter (with a size cut at 10 mu m, PM10, or without any size cut) at eight observatories representing all Arctic sectors. Our holistic observational approach includes the Russian Arctic, a significant emission source area with less dedicated aerosol monitoring, and extends beyond the more traditionally studied summer period and black carbon/sulfate or fine-mode pollutants. The major airborne Arctic PM components in terms of dry mass are sea salt, secondary (non-sea-salt, nss) sulfate, and organic aerosol (OA), with minor contributions from elemental carbon (EC) and ammonium. We observe substantial spatiotemporal variability in component ratios, such as EC/OA, ammonium/nss-sulfate and OA/nss-sulfate, and fractional contributions to PM. When combined with component-specific back-trajectory analysis to identify marine or terrestrial origins, as well as the companion study by Moschos et al 2022 Nat. Geosci. focusing on OA, the composition analysis provides policy-guiding observational insights into sector-based differences in natural and anthropogenic Arctic aerosol sources. In this regard, we first reveal major source regions of inner-Arctic sea salt, biogenic sulfate, and natural organics, and highlight an underappreciated wintertime source of primary carbonaceous aerosols (EC and OA) in West Siberia, potentially associated with the oil and gas sector. The presented dataset can assist in reducing uncertainties in modelling pan-Arctic aerosol-climate interactions, as the major contributors to yearly aerosol mass can be constrained. These models can then be used to predict the future evolution of individual inner-Arctic atmospheric PM components in light of current and emerging pollution mitigation measures and improved region-specific emission inventories. Peer reviewed

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    NILU Brage
    Article . 2022
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    image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
    Environmental Research Letters
    Article . 2022
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    image/svg+xml Jakob Voss, based on art designer at PLoS, modified by Wikipedia users Nina and Beao Closed Access logo, derived from PLoS Open Access logo. This version with transparent background. http://commons.wikimedia.org/wiki/File:Closed_Access_logo_transparent.svg Jakob Voss, based on art designer at PLoS, modified by Wikipedia users Nina and Beao
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      image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
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      Environmental Research Letters
      Article . 2022
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      image/svg+xml Jakob Voss, based on art designer at PLoS, modified by Wikipedia users Nina and Beao Closed Access logo, derived from PLoS Open Access logo. This version with transparent background. http://commons.wikimedia.org/wiki/File:Closed_Access_logo_transparent.svg Jakob Voss, based on art designer at PLoS, modified by Wikipedia users Nina and Beao
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    Authors: Beatriz Ferreira Araujo; Stefan Osterwalder; Natalie Szponar; Domenica Lee; +19 Authors

    During Arctic springtime, halogen radicals oxidize atmospheric elemental mercury (Hg-0), which deposits to the cryosphere. This is followed by a summertime atmospheric Hg-0 peak that is thought to result mostly from terrestrial Hg inputs to the Arctic Ocean, followed by photoreduction and emission to air. The large terrestrial Hg contribution to the Arctic Ocean and global atmosphere has raised concern over the potential release of permafrost Hg, via rivers and coastal erosion, with Arctic warming. Here we investigate Hg isotope variability of Arctic atmospheric, marine, and terrestrial Hg. We observe highly characteristic Hg isotope signatures during the summertime peak that reflect re-emission of Hg deposited to the cryosphere during spring. Air mass back trajectories support a cryospheric Hg emission source but no major terrestrial source. This implies that terrestrial Hg inputs to the Arctic Ocean remain in the marine ecosystem, without substantial loss to the global atmosphere, but with possible effects on food webs.Arctic warming thaws permafrost, leading to enhanced soil mercury transport to the Arctic Ocean. Mercury isotope signatures in arctic rivers, ocean and atmosphere suggest that permafrost mercury is buried in marine sediment and not emitted to the global atmosphere Peer reviewed

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    Authors: Leinonen, Ville; Kokkola, Harri; Yli-Juuti, Taina; Mielonen, Tero; +32 Authors

    Despite a large number of studies, out of all drivers of radiative forcing, the effect of aerosols has the largest uncertainty in global climate model radiative forcing estimates. There have been studies of aerosol optical properties in climate models, but the effects of particle number size distribution need a more thorough inspection. We investigated the trends and seasonality of particle number concentrations in nucleation, Aitken, and accumulation modes at 21 measurement sites in Europe and the Arctic. For 13 of those sites, with longer measurement time series, we compared the field observations with the results from five climate models, namely EC-Earth3, ECHAM-M7, ECHAM-SALSA, NorESM1.2, and UKESM1. This is the first extensive comparison of detailed aerosol size distribution trends between in situ observations from Europe and five earth system models (ESMs). We found that the trends of particle number concentrations were mostly consistent and decreasing in both measurements and models. However, for many sites, climate models showed weaker decreasing trends than the measurements. Seasonal variability in measured number concentrations, quantified by the ratio between maximum and minimum monthly number concentration, was typically stronger at northern measurement sites compared to other locations. Models had large differences in their seasonal representation, and they can be roughly divided into two categories: for EC-Earth and NorESM, the seasonal cycle was relatively similar for all sites, and for other models the pattern of seasonality varied between northern and southern sites. In addition, the variability in concentrations across sites varied between models, some having relatively similar concentrations for all sites, whereas others showed clear differences in concentrations between remote and urban sites. To conclude, although all of the model simulations had identical input data to describe anthropogenic mass emissions, trends in differently sized particles vary among the models due to assumptions in emission sizes and differences in how models treat size-dependent aerosol processes. The inter-model variability was largest in the accumulation mode, i.e. sizes which have implications for aerosol-cloud interactions. Our analysis also indicates that between models there is a large variation in efficiency of long-range transportation of aerosols to remote locations. The differences in model results are most likely due to the more complex effect of different processes instead of one specific feature (e.g. the representation of aerosol or emission size distributions). Hence, a more detailed characterization of microphysical processes and deposition processes affecting the long-range transport is needed to understand the model variability. Peer reviewed

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    Authors: Shupe, Matthew D.; Rex, Markus; Blomquist, Byron; Persson, P. Ola G.; +110 Authors

    With the Arctic rapidly changing, the needs to observe, understand, and model the changes are essential. To support these needs, an annual cycle of observations of atmospheric properties, processes, and interactions were made while drifting with the sea ice across the central Arctic during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition from October 2019 to September 2020. An international team designed and implemented the comprehensive program to document and characterize all aspects of the Arctic atmospheric system in unprecedented detail, using a variety of approaches, and across multiple scales. These measurements were coordinated with other observational teams to explore crosscutting and coupled interactions with the Arctic Ocean, sea ice, and ecosystem through a variety of physical and biogeochemical processes. This overview outlines the breadth and complexity of the atmospheric research program, which was organized into 4 subgroups: atmospheric state, clouds and precipitation, gases and aerosols, and energy budgets. Atmospheric variability over the annual cycle revealed important influences from a persistent large-scale winter circulation pattern, leading to some storms with pressure and winds that were outside the interquartile range of past conditions suggested by long-term reanalysis. Similarly, the MOSAiC location was warmer and wetter in summer than the reanalysis climatology, in part due to its close proximity to the sea ice edge.The comprehensiveness of the observational program for characterizing and analyzing atmospheric phenomena is demonstrated via a winter case study examining air mass transitions and a summer case study examining vertical atmospheric evolution. Overall, the MOSAiC atmospheric program successfully met its objectives and was the most comprehensive atmospheric measurement program to date conducted over the Arctic sea ice. The obtained data will support a broad range of coupled-system scientific research and provide an important foundation for advancing multiscale modeling capabilities in the Arctic. International audience

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    Elementa: Science of the Anthropocene
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