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22 Research products

  • European Marine Science
  • 2014-2023
  • GB
  • Atmospheric Chemistry and Physics (ACP)
  • Aurora Universities Network

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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: R. Wagner; L. Ickes; A. K. Bertram; N. Els; +5 Authors

    Sea spray aerosol particles are a recognised type of ice-nucleating particles under mixed-phase cloud conditions. Entities that are responsible for the heterogeneous ice nucleation ability include intact or fragmented cells of marine microorganisms as well as organic matter released by cell exudation. Only a small fraction of sea spray aerosol is transported to the upper troposphere, but there are indications from mass-spectrometric analyses of the residuals of sublimated cirrus particles that sea salt could also contribute to heterogeneous ice nucleation under cirrus conditions. Experimental studies on the heterogeneous ice nucleation ability of sea spray aerosol particles and their proxies at temperatures below 235 K are still scarce. In our article, we summarise previous measurements and present a new set of ice nucleation experiments at cirrus temperatures with particles generated from sea surface microlayer and surface seawater samples collected in three different regions of the Arctic and from a laboratory-grown diatom culture (Skeletonema marinoi). The particles were suspended in the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) cloud chamber and ice formation was induced by expansion cooling. We confirmed that under cirrus conditions, apart from the ice-nucleating entities mentioned above, also crystalline inorganic salt constituents can contribute to heterogeneous ice formation. This takes place at temperatures below 220 K, where we observed in all experiments a strong immersion freezing mode due to the only partially deliquesced inorganic salts. The inferred ice nucleation active surface site densities for this nucleation mode reached a maximum of about 5×1010 m−2 at an ice saturation ratio of 1.3. Much smaller densities in the range of 108–109 m−2 were observed at temperatures between 220 and 235 K, where the inorganic salts fully deliquesced and only the organic matter and/or algal cells and cell debris could contribute to heterogeneous ice formation. These values are 2 orders of magnitude smaller than those previously reported for particles generated from microlayer suspensions collected in temperate and subtropical zones. While this difference might simply underline the strong variability of the number of ice-nucleating entities in the sea surface microlayer across different geographical regions, we also discuss how instrumental parameters like the aerosolisation method and the ice nucleation measurement technique might affect the comparability of the results amongst different studies.

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    KITopen
    Article . 2021
    License: CC BY
    Data sources: KITopen
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    https://doi.org/10.5445/ir/100...
    Article . 2021
    License: CC BY
    Data sources: Datacite
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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/ Atmospheric Chemistr...arrow_drop_down
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      KITopen
      Article . 2021
      License: CC BY
      Data sources: KITopen
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      https://doi.org/10.5445/ir/100...
      Article . 2021
      License: CC BY
      Data sources: Datacite
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    Authors: Christo Buizert; Patricia Martinerie; Vasilii V. Petrenko; J. P. Severinghaus; +22 Authors

    Author(s): Buizert, C; Martinerie, P; Petrenko, VV; Severinghaus, JP; Trudinger, CM; Witrant, E; Rosen, JL; Orsi, AJ; Rubino, M; Etheridge, DM; Steele, LP; Hogan, C; Laube, JC; Sturges, WT; Levchenko, VA; Smith, AM; Levin, I; Conway, TJ; Dlugokencky, EJ; Lang, PM; Kawamura, K; Jenk, TM; White, JWC; Sowers, T; Schwander, J; Blunier, T

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    Atmospheric Chemistry and Physics (ACP)
    Article
    License: CC BY
    Data sources: UnpayWall
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    Atmospheric Chemistry and Physics (ACP)
    Article . 2014 . Peer-reviewed
    License: CC BY
    Data sources: Crossref
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      Atmospheric Chemistry and Physics (ACP)
      Article
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      Atmospheric Chemistry and Physics (ACP)
      Article . 2014 . Peer-reviewed
      License: CC BY
      Data sources: Crossref
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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: R. Hossaini; R. Hossaini; P. K. Patra; A. A. Leeson; +51 Authors

    The first concerted multi-model intercomparison of halogenated very short-lived substances (VSLS) has been performed, within the framework of the ongoing Atmospheric Tracer Transport Model Intercomparison Project (TransCom). Eleven global models or model variants participated (nine chemical transport models and two chemistry-climate models) by simulating the major natural bromine VSLS, bromoform (CHBr3) and dibromomethane (CH2Br2), over a 20-year period (1993-2012). Except for three model simulations, all others were driven offline by (or nudged to) reanalysed meteorology. The overarching goal of TransCom-VSLS was to provide a reconciled model estimate of the stratospheric source gas injection (SGI) of bromine from these gases, to constrain the current measurement-derived range, and to investigate inter-model differences due to emissions and transport processes. Models ran with standardised idealised chemistry, to isolate differences due to transport, and we investigated the sensitivity of results to a range of VSLS emission inventories. Models were tested in their ability to reproduce the observed seasonal and spatial distribution of VSLS at the surface, using measurements from NOAA's long-term global monitoring network, and in the tropical troposphere, using recent aircraft measurements - including high-altitude observations from the NASA Global Hawk platform. The models generally capture the observed seasonal cycle of surface CHBr3 and CH2Br2 well, with a strong model-measurement correlation (r≥0.7) at most sites. In a given model, the absolute model-measurement agreement at the surface is highly sensitive to the choice of emissions. Large inter-model differences are apparent when using the same emission inventory, highlighting the challenges faced in evaluating such inventories at the global scale. Across the ensemble, most consistency is found within the tropics where most of the models (8 out of 11) achieve best agreement to surface CHBr3 observations using the lowest of the three CHBr3 emission inventories tested (similarly, 8 out of 11 models for CH2Br2). In general, the models reproduce observations of CHBr3 and CH2Br2 obtained in the tropical tropopause layer (TTL) at various locations throughout the Pacific well. Zonal variability in VSLS loading in the TTL is generally consistent among models, with CHBr3 (and to a lesser extent CH2Br2) most elevated over the tropical western Pacific during boreal winter. The models also indicate the Asian monsoon during boreal summer to be an important pathway for VSLS reaching the stratosphere, though the strength of this signal varies considerably among models. We derive an ensemble climatological mean estimate of the stratospheric bromine SGI from CHBr3 and CH2Br2 of 2.0 (1.2-2.5)ppt, ∼57% larger than the best estimate from the most recent World Meteorological Organization (WMO) Ozone Assessment Report. We find no evidence for a long-term, transport-driven trend in the stratospheric SGI of bromine over the simulation period. The transport-driven interannual variability in the annual mean bromine SGI is of the order of ±5%, with SGI exhibiting a strong positive correlation with the El Niño-Southern Oscillation (ENSO) in the eastern Pacific. Overall, our results do not show systematic differences between models specific to the choice of reanalysis meteorology, rather clear differences are seen related to differences in the implementation of transport processes in the models. Peer Reviewed

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    OceanRep
    Article . 2016 . Peer-reviewed
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    CORE (RIOXX-UK Aggregator)
    Article . 2016
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    Atmospheric Chemistry and Physics (ACP)
    Article . 2016 . Peer-reviewed
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    https://doi.org/10.5194/acp-20...
    Preprint . 2016 . Peer-reviewed
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    Cranfield CERES
    Article . 2016
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    Data sources: Cranfield CERES
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    Atmospheric Chemistry and Physics (ACP)
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    https://doi.org/10.5445/ir/100...
    Article . 2016
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    Article . 2016
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    Apollo
    Other literature type . 2016
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    Apollo
    Article . 2016
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      Atmospheric Chemistry and Physics (ACP)
      Article . 2016 . Peer-reviewed
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      https://doi.org/10.5194/acp-20...
      Preprint . 2016 . Peer-reviewed
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      Cranfield CERES
      Article . 2016
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      Atmospheric Chemistry and Physics (ACP)
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      https://doi.org/10.5445/ir/100...
      Article . 2016
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      Apollo
      Other literature type . 2016
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      Apollo
      Article . 2016
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    Authors: Benjamin Murray; Nora Els; Elena Gorokhova; Robert Wagner; +4 Authors

    Abstract. Sea spray aerosol particles are a recognised type of ice-nucleating particles under mixed-phase cloud conditions. Entities that are responsible for the heterogeneous ice nucleation ability include intact or fragmented cells of marine microorganisms as well as organic matter released by cell exudation. Only a small fraction of sea spray aerosol is transported to the upper troposphere, but there are indications from mass-spectrometric analyses of the residuals of sublimated cirrus particles that sea salt could also contribute to heterogeneous ice nucleation under cirrus conditions. Experimental studies on the heterogeneous ice nucleation ability of sea spray aerosol particles and their proxies at temperatures below 235 K are still scarce. In our article, we summarise previous measurements and present a new set of ice nucleation experiments at cirrus temperatures with particles generated from sea surface microlayer and surface seawater samples collected in three different regions of the Arctic and from a laboratory-grown diatom culture (Skeletonema marinoi). The particles were suspended in the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) cloud chamber and ice formation was induced by expansion cooling. We confirmed that under cirrus conditions, apart from the ice-nucleating entities mentioned above, also crystalline inorganic salt constituents can contribute to heterogeneous ice formation. This takes place at temperatures below 220 K, where we observed in all experiments a strong immersion freezing mode due to the only partially deliquesced inorganic salts. The inferred ice nucleation active surface site densities for this nucleation mode reached a maximum of about 5×1010 m−2 at an ice saturation ratio of 1.3. Much smaller densities in the range of 108–109 m−2 were observed at temperatures between 220 and 235 K, where the inorganic salts fully deliquesced and only the organic matter and/or algal cells and cell debris could contribute to heterogeneous ice formation. These values are 2 orders of magnitude smaller than those previously reported for particles generated from microlayer suspensions collected in temperate and subtropical zones. While this difference might simply underline the strong variability of the number of ice-nucleating entities in the sea surface microlayer across different geographical regions, we also discuss how instrumental parameters like the aerosolisation method and the ice nucleation measurement technique might affect the comparability of the results amongst different studies.

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    Atmospheric Chemistry and Physics (ACP)
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    Atmospheric Chemistry and Physics (ACP); OpenAPC Global Initiative
    Article . Conference object . 2021 . Peer-reviewed
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      Atmospheric Chemistry and Physics (ACP); OpenAPC Global Initiative
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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: Saunois, Marielle; Bousquet, Philippe; Poulter, Ben; Peregon, Anna; +68 Authors

    Source at https://doi.org/10.5194/acp-17-11135-2017 Following the recent Global Carbon Project (GCP) synthesis of the decadal methane (CH4 budget over 2000– 2012 (Saunois et al., 2016), we analyse here the same dataset with a focus on quasi-decadal and inter-annual variability in CH4 emissions. The GCP dataset integrates results from topdown studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models (including process-based models for estimating land surface emissions and atmospheric chemistry), inventories of anthropogenic emissions, and data-driven approaches. The annual global methane emissions from top-down studies, which by construction match the observed methane growth rate within their uncertainties, all show an increase in total methane emissions over the period 2000–2012, but this increase is not linear over the 13 years. Despite differences between individual studies, the mean emission anomaly of the top-down ensemble shows no significant trend in total methane emissions over the period 2000–2006, during the plateau of atmospheric methane mole fractions, and also over the period 2008–2012, during the renewed atmospheric methane increase. However, the top-down ensemble mean produces an emission shift between 2006 and 2008, leading to 22 [16–32] Tg CH4yr-1 higher methane emissions over the period 2008–2012 compared to 2002–2006. This emission increase mostly originated from the tropics, with a smaller contribution from mid-latitudes and no significant change from boreal regions. The regional contributions remain uncertain in top-down studies. Tropical South America and South and East Asia seem to contribute the most to the emission increase in the tropics. However, these two regions have only limited atmospheric measurements and remain therefore poorly constrained. The sectorial partitioning of this emission increase between the periods 2002–2006 and 2008–2012 differs from one atmospheric inversion study to another. However, all topdown studies suggest smaller changes in fossil fuel emissions (from oil, gas, and coal industries) compared to the mean of the bottom-up inventories included in this study. This difference is partly driven by a smaller emission change in China from the top-down studies compared to the estimate in the Emission Database for Global Atmospheric Research (EDGARv4.2) inventory, which should be revised to smaller values in a near future. We apply isotopic signatures to the emission changes estimated for individual studies based on five emission sectors and find that for six individual top-down studies (out of eight) the average isotopic signature of the emission changes is not consistent with the observed change in atmospheric 13CH4. However, the partitioning in emission change derived from the ensemble mean is consistent with this isotopic constraint. At the global scale, the top-down ensemble mean suggests that the dominant contribution to the resumed atmospheric CH4 growth after 2006 comes from microbial sources (more from agriculture and waste sectors than from natural wetlands), with an uncertain but smaller contribution from fossil CH4 emissions. In addition, a decrease in biomass burning emissions (in agreement with the biomass burning emission databases) makes the balance of sources consistent with atmospheric 13CH4 observations. In most of the top-down studies included here, OH concentrations are considered constant over the years (seasonal variations but without any inter-annual variability). As a result, the methane loss (in particular through OH oxidation) varies mainly through the change in methane concentrations and not its oxidants. For these reasons, changes in the methane loss could not be properly investigated in this study, although it may play a significant role in the recent atmospheric methane changes as briefly discussed at the end of the paper.

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    Article . 2017
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    https://doi.org/10.5194/acp-20...
    Preprint . 2017
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    Article . 2017
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    https://www.atmos-chem-phys.ne...
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    https://doi.org/10.7892/boris....
    Other literature type . 2017
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      https://doi.org/10.5194/acp-20...
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      https://www.atmos-chem-phys.ne...
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      https://doi.org/10.7892/boris....
      Other literature type . 2017
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    Authors: Keeble, James; Hassler, Birgit; Banerjee, Antara; Checa-Garcia, Ramiro; +27 Authors

    Stratospheric ozone and water vapour are key components of the Earth system, and past and future changes to both have important impacts on global and regional climate. Here, we evaluate long-term changes in these species from the pre-industrial period (1850) to the end of the 21st century in Coupled Model Intercomparison Project phase 6 (CMIP6) models under a range of future emissions scenarios. There is good agreement between the CMIP multi-model mean and observations for total column ozone (TCO), although there is substantial variation between the individual CMIP6 models. For the CMIP6 multi-model mean, global mean TCO has increased from ∼ 300 DU in 1850 to ∼ 305 DU in 1960, before rapidly declining in the 1970s and 1980s following the use and emission of halogenated ozone-depleting substances (ODSs). TCO is projected to return to 1960s values by the middle of the 21st century under the SSP2-4.5, SSP3-7.0, SSP4-3.4, SSP4-6.0, and SSP5-8.5 scenarios, and under the SSP3-7.0 and SSP5-8.5 scenarios TCO values are projected to be ∼ 10 DU higher than the 1960s values by 2100. However, under the SSP1-1.9 and SSP1-1.6 scenarios, TCO is not projected to return to the 1960s values despite reductions in halogenated ODSs due to decreases in tropospheric ozone mixing ratios. This global pattern is similar to regional patterns, except in the tropics where TCO under most scenarios is not projected to return to 1960s values, either through reductions in tropospheric ozone under SSP1-1.9 and SSP1-2.6, or through reductions in lower stratospheric ozone resulting from an acceleration of the Brewer–Dobson circulation under other Shared Socioeconomic Pathways (SSPs). In contrast to TCO, there is poorer agreement between the CMIP6 multi-model mean and observed lower stratospheric water vapour mixing ratios, with the CMIP6 multi-model mean underestimating observed water vapour mixing ratios by ∼ 0.5 ppmv at 70 hPa. CMIP6 multi-model mean stratospheric water vapour mixing ratios in the tropical lower stratosphere have increased by ∼ 0.5 ppmv from the pre-industrial to the present-day period and are projected to increase further by the end of the 21st century. The largest increases (∼ 2 ppmv) are simulated under the future scenarios with the highest assumed forcing pathway (e.g. SSP5-8.5). Tropical lower stratospheric water vapour, and to a lesser extent TCO, shows large variations following explosive volcanic eruptions.

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    Other literature type . Article . 2021 . Peer-reviewed
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    Atmospheric Chemistry and Physics (ACP)
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    Apollo
    Article . 2021
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    Apollo
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      Apollo
      Article . 2021
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      Article . 2021
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    Authors: Outi Meinander; Pavla Dagsson-Waldhauserova; Pavel Amosov; Elena Aseyeva; +52 Authors

    Dust particles from high latitudes have a potentially large local, regional, and global significance to climate and the environment as short-lived climate forcers, air pollutants, and nutrient sources. Identifying the locations of local dust sources and their emission, transport, and deposition processes is important for understanding the multiple impacts of high-latitude dust (HLD) on the Earth's systems. Here, we identify, describe, and quantify the source intensity (SI) values, which show the potential of soil surfaces for dust emission scaled to values 0 to 1 concerning globally best productive sources, using the Global Sand and Dust Storms Source Base Map (G-SDS-SBM). This includes 64 HLD sources in our collection for the northern (Alaska, Canada, Denmark, Greenland, Iceland, Svalbard, Sweden, and Russia) and southern (Antarctica and Patagonia) high latitudes. Activity from most of these HLD sources shows seasonal character. It is estimated that high-latitude land areas with higher (SI ≥0.5), very high (SI ≥0.7), and the highest potential (SI ≥0.9) for dust emission cover >1 670 000 km2, >560 000 km2, and >240 000 km2, respectively. In the Arctic HLD region (≥60∘ N), land area with SI ≥0.5 is 5.5 % (1 035 059 km2), area with SI ≥0.7 is 2.3 % (440 804 km2), and area with SI ≥0.9 is 1.1 % (208 701 km2). Minimum SI values in the northern HLD region are about 3 orders of magnitude smaller, indicating that the dust sources of this region greatly depend on weather conditions. Our spatial dust source distribution analysis modeling results showed evidence supporting a northern HLD belt, defined as the area north of 50∘ N, with a “transitional HLD-source area” extending at latitudes 50–58∘ N in Eurasia and 50–55∘ N in Canada and a “cold HLD-source area” including areas north of 60∘ N in Eurasia and north of 58∘ N in Canada, with currently “no dust source” area between the HLD and low-latitude dust (LLD) dust belt, except for British Columbia. Using the global atmospheric transport model SILAM, we estimated that 1.0 % of the global dust emission originated from the high-latitude regions. About 57 % of the dust deposition in snow- and ice-covered Arctic regions was from HLD sources. In the southern HLD region, soil surface conditions are favorable for dust emission during the whole year. Climate change can cause a decrease in the duration of snow cover, retreat of glaciers, and an increase in drought, heatwave intensity, and frequency, leading to the increasing frequency of topsoil conditions favorable for dust emission, which increases the probability of dust storms. Our study provides a step forward to improve the representation of HLD in models and to monitor, quantify, and assess the environmental and climate significance of HLD.

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    https://doi.org/10.5445/ir/100...
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    https://doi.org/10.17169/refub...
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      https://doi.org/10.5445/ir/100...
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    Authors: Robert Mulvaney; Max Thomas; Jan Kaiser; Patricia Martinerie; +1 Authors

    Abstract. We present novel measurements of the carbon isotope composition of CFC-11 (CCl 3 F), CFC-12 (CCl 2 F 2 ), and CFC-113 (CF 2 ClCFCl 2 ), three atmospheric trace gases that are important for both stratospheric ozone depletion and global warming. These measurements were carried out on air samples collected in the stratosphere – the main sink region for these gases – and on air extracted from deep polar firn snow. We quantify, for the first time, the apparent isotopic fractionation, ϵapp(13C) , for these gases as they are destroyed in the high- and mid-latitude stratosphere: ϵapp (CFC-12, high-latitude) = ( - 20.2 ± 4.4 ) ‰, and ϵapp (CFC-113, high-latitude) = ( - 9.4 ± 4.4 ) ‰, ϵapp (CFC-12, mid-latitude) = ( - 30.3 ± 10.7 ) ‰, and ϵapp (CFC-113, mid-latitude) = ( - 34.4 ± 9.8 ) ‰. Our CFC-11 measurements were not sufficient to calculate ϵapp (CFC-11), so we instead used previously reported photolytic fractionation for CFC-11 and CFC-12 to scale our ϵapp (CFC-12), resulting in ϵapp (CFC-11, high-latitude) = ( - 7.8 ± 1.7 ) ‰ and ϵapp (CFC-11, mid-latitude) = ( - 11.7 ± 4.2 ) ‰. Measurements of firn air were used to construct histories of the tropospheric isotopic composition, δT(13C) , for CFC-11 (1950s to 2009), CFC-12 (1950s to 2009), and CFC-113 (1970s to 2009), with δT(13C) increasing for each gas. We used ϵapp (high-latitude), which was derived from more data, and a constant isotopic composition of emissions, δE(13C) , to model δT ( 13C , CFC-11), δT ( 13C , CFC-12), and δT ( 13C , CFC-113). For CFC-11 and CFC-12, modelled δT(13C) was consistent with measured δT(13C) for the entire period covered by the measurements, suggesting that no dramatic change in δE ( 13C , CFC-11) or δE ( 13C , CFC-12) has occurred since the 1950s. For CFC-113, our modelled δT ( 13C , CFC-113) did not agree with our measurements earlier than 1980. This discrepancy may be indicative of a change in δE ( 13C , CFC-113). However, this conclusion is based largely on a single sample and only just significant outside the 95 % confidence interval. Therefore more work is needed to independently verify this temporal trend in the global tropospheric 13 C isotopic composition of CFC-113. Our modelling predicts increasing δT ( 13C , CFC-11), δT ( 13C , CFC-12), and δT ( 13C , CFC-113) into the future. We investigated the effect of recently reported new CFC-11 emissions on background δT ( 13C , CFC-11) by fixing model emissions after 2012 and comparing δT ( 13C , CFC-11) in this scenario to the model base case. The difference in δT ( 13C , CFC-11) between these scenarios was 1.4 ‰ in 2050. This difference is smaller than our model uncertainty envelope and would therefore require improved modelling and measurement precision as well as better quantified isotopic source compositions to detect.

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    Atmospheric Chemistry and Physics (ACP)
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    Atmospheric Chemistry and Physics (ACP); OpenAPC Global Initiative
    Article . Conference object . 2021 . Peer-reviewed
    License: CC BY
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      Atmospheric Chemistry and Physics (ACP)
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      Atmospheric Chemistry and Physics (ACP); OpenAPC Global Initiative
      Article . Conference object . 2021 . Peer-reviewed
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    Authors: Markus M. Frey; Howard K. Roscoe; Alexandre Kukui; Joel Savarino; +3 Authors

    Abstract. Mixing ratios of the atmospheric nitrogen oxides NO and NO2 were measured as part of the OPALE (Oxidant Production in Antarctic Lands & Export) campaign at Dome C, East Antarctica (75.1° S, 123.3° E, 3233 m), during December 2011 to January 2012. Profiles of NOx mixing ratios of the lower 100 m of the atmosphere confirm that, in contrast to the South Pole, air chemistry at Dome C is strongly influenced by large diurnal cycles in solar irradiance and a sudden collapse of the atmospheric boundary layer in the early evening. Depth profiles of mixing ratios in firn air suggest that the upper snowpack at Dome C holds a significant reservoir of photolytically produced NO2 and is a sink of gas-phase ozone (O3). First-time observations of bromine oxide (BrO) at Dome C show that mixing ratios of BrO near the ground are low, certainly less than 5 pptv, with higher levels in the free troposphere. Assuming steady state, observed mixing ratios of BrO and RO2 radicals are too low to explain the large NO2 : NO ratios found in ambient air, possibly indicating the existence of an unknown process contributing to the atmospheric chemistry of reactive nitrogen above the Antarctic Plateau. During 2011–2012, NOx mixing ratios and flux were larger than in 2009–2010, consistent with also larger surface O3 mixing ratios resulting from increased net O3 production. Large NOx mixing ratios at Dome C arise from a combination of continuous sunlight, shallow mixing height and significant NOx emissions by surface snow (FNOx). During 23 December 2011–12 January 2012, median FNOx was twice that during the same period in 2009–2010 due to significantly larger atmospheric turbulence and a slightly stronger snowpack source. A tripling of FNOx in December 2011 was largely due to changes in snowpack source strength caused primarily by changes in NO3− concentrations in the snow skin layer, and only to a secondary order by decrease of total column O3 and associated increase in NO3− photolysis rates. A source of uncertainty in model estimates of FNOx is the quantum yield of NO3− photolysis in natural snow, which may change over time as the snow ages.

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    Atmospheric Chemistry and Physics (ACP)
    Article . 2015 . Peer-reviewed
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    Atmospheric Chemistry and Physics (ACP)
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      Atmospheric Chemistry and Physics (ACP)
      Article . 2015 . Peer-reviewed
      License: CC BY
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      Atmospheric Chemistry and Physics (ACP)
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    Authors: Johana Romero-Alvarez; Aurelia Lupaşcu; Douglas Lowe; Alba Badia; +4 Authors

    Abstract. Tropospheric ozone (O3) concentrations depend on a combination of hemispheric, regional, and local-scale processes. Estimates of how much O3 is produced locally vs. transported from further afield are essential in air quality management and regulatory policies. Here, a tagged-ozone mechanism within the Weather Research and Forecasting model coupled with chemistry (WRF-Chem) is used to quantify the contributions to surface O3 in the UK from anthropogenic nitrogen oxide (NOx) emissions from inside and outside the UK during May–August 2015. The contribution of the different source regions to three regulatory O3 metrics is also examined. It is shown that model simulations predict the concentration and spatial distribution of surface O3 with a domain-wide mean bias of −3.7 ppbv. Anthropogenic NOx emissions from the UK and Europe account for 13 % and 16 %, respectively, of the monthly mean surface O3 in the UK, as the majority (71 %) of O3 originates from the hemispheric background. Hemispheric O3 contributes the most to concentrations in the north and the west of the UK with peaks in May, whereas European and UK contributions are most significant in the east, south-east, and London, i.e. the UK's most populated areas, intensifying towards June and July. Moreover, O3 from European sources is generally transported to the UK rather than produced in situ. It is demonstrated that more stringent emission controls over continental Europe, particularly in western Europe, would be necessary to improve the health-related metric MDA8 O3 above 50 and 60 ppbv. Emission controls over larger areas, such as the Northern Hemisphere, are instead required to lessen the impacts on ecosystems as quantified by the AOT40 metric.

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    IASSpublic
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    IASSpublic
    Article . 2022
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    https://doi.org/10.17169/refub...
    Other literature type . 2022
    License: CC BY
    Data sources: Datacite
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