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  • 2013-2022
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  • Copernicus Publications
  • Atmospheric Chemistry and Physics (...
  • Aurora Universities Network

  • 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: Romero-Alvarez, Johana; Lupaşcu, Aurelia; Lowe, Douglas; Badia, Alba; +4 Authors

    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.

    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/ Copernicus Publicati...arrow_drop_down
    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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      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/ Copernicus Publicati...arrow_drop_down
      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/
    Authors: Stolzenburg, Dominik; Simon, Mario; Ranjithkumar, Ananth; Kürten, Andreas; +74 Authors

    In the present-day atmosphere, sulfuric acid is the most important vapour for aerosol particle formation and initial growth. However, the growth rates of nanoparticles (<10 nm) from sulfuric acid remain poorly measured. Therefore, the effect of stabilizing bases, the contribution of ions and the impact of attractive forces on molecular collisions are under debate. Here, we present precise growth rate measurements of uncharged sulfuric acid particles from 1.8 to 10 nm, performed under atmospheric conditions in the CERN (European Organization for Nuclear Research) CLOUD chamber. Our results show that the evaporation of sulfuric acid particles above 2 nm is negligible, and growth proceeds kinetically even at low ammonia concentrations. The experimental growth rates exceed the hard-sphere kinetic limit for the condensation of sulfuric acid. We demonstrate that this results from van der Waals forces between the vapour molecules and particles and disentangle it from charge–dipole interactions. The magnitude of the enhancement depends on the assumed particle hydration and collision kinetics but is increasingly important at smaller sizes, resulting in a steep rise in the observed growth rates with decreasing size. Including the experimental results in a global model, we find that the enhanced growth rate of sulfuric acid particles increases the predicted particle number concentrations in the upper free troposphere by more than 50 %.

    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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    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/
    Copernicus Publications
    Other ORP type . 2020
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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
      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/
      Copernicus Publications
      Other ORP type . 2020
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    Authors: Sellitto, Pasquale; Guermazi, Henda; Carboni, Elisa; Siddans, Richard; +1 Authors

    We developed an optimal-estimation algorithm to simultaneously retrieve, for the first time, coexisting volcanic gaseous SO2 and sulfate aerosols (SA) from ground-based Fourier transform infrared (FTIR) observations. These effluents, both linked to magmatic degassing process and subsequent atmospheric evolution processes, have overlapping spectral signatures leading to mutual potential interferences when retrieving one species without considering the other. We show that significant overestimations may be introduced in SO2 retrievals if the radiative impact of coexistent SA is not accounted for, which may have impacted existing SO2 long-term series, e.g. from satellite platforms. The method was applied to proximal observations at Masaya volcano, where SO2 and SA concentrations, and SA acidity, were retrieved. A gas-to-particle sulfur partitioning of 400 and a strong SA acidity (sulfuric acid concentration: 65 %) were found, consistent with past in situ observations at this volcano. This method is easily exportable to other volcanoes to monitor magma extraction processes and the atmospheric sulfur cycle in the case of ash-free plumes.

    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 Measurem...arrow_drop_down
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    Copernicus Publications
    Other ORP type . 2019
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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 Measurem...arrow_drop_down
      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/
      Copernicus Publications
      Other ORP type . 2019
  • 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: Frege, Carla; Ortega, Ismael K.; Rissanen, Matti P.; Praplan, Arnaud P.; +49 Authors

    It was recently shown by the CERN CLOUD experiment that biogenic highly oxygenated molecules (HOMs) form particles under atmospheric conditions in the absence of sulfuric acid, where ions enhance the nucleation rate by 1–2 orders of magnitude. The biogenic HOMs were produced from ozonolysis of α-pinene at 5 ∘C. Here we extend this study to compare the molecular composition of positive and negative HOM clusters measured with atmospheric pressure interface time-of-flight mass spectrometers (APi-TOFs), at three different temperatures (25, 5 and −25 ∘C). Most negative HOM clusters include a nitrate (NO3-) ion, and the spectra are similar to those seen in the nighttime boreal forest. On the other hand, most positive HOM clusters include an ammonium (NH4+) ion, and the spectra are characterized by mass bands that differ in their molecular weight by ∼ 20 C atoms, corresponding to HOM dimers. At lower temperatures the average oxygen to carbon (O : C) ratio of the HOM clusters decreases for both polarities, reflecting an overall reduction of HOM formation with decreasing temperature. This indicates a decrease in the rate of autoxidation with temperature due to a rather high activation energy as has previously been determined by quantum chemical calculations. Furthermore, at the lowest temperature (−25 ∘C), the presence of C30 clusters shows that HOM monomers start to contribute to the nucleation of positive clusters. These experimental findings are supported by quantum chemical calculations of the binding energies of representative neutral and charged clusters.

    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/ Copernicus Publicati...arrow_drop_down
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    Copernicus Publications
    Other ORP type . 2019
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      Copernicus Publications
      Other ORP type . 2019
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    Authors: Watson-Parris, Duncan; Schutgens, Nick; Reddington, Carly; Pringle, Kirsty J.; +5 Authors

    Despite ongoing efforts, the vertical distribution of aerosols globally is poorly understood. This in turn leads to large uncertainties in the contributions of the direct and indirect aerosol forcing on climate. Using the Global Aerosol Synthesis and Science Project (GASSP) database – the largest synthesised collection of in-situ aircraft measurements currently available, with more than 1000 flights from 37 campaigns from around the world – we investigate the vertical structure of sub-micron aerosols across a wide range of regions and environments. The application of this unique dataset to assess the vertical distributions of number size distribution and Cloud Condensation Nuclei (CCN) in the global aerosol-climate model ECHAM-HAM reveals that the model underestimates accumulation mode particles in the upper troposphere, especially in remote regions. The processes underlying this discrepancy are explored using different aerosol microphysical schemes and a process sensitivity analysis. These show that the biases are predominantly related to aerosol ageing and removal rather than emissions.

    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/ Copernicus Publicati...arrow_drop_down
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    Copernicus Publications
    Other ORP type . 2019
    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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      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/ Copernicus Publicati...arrow_drop_down
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      Copernicus Publications
      Other ORP type . 2019
      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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    Authors: Dumousseaud, C.; Achterberg, E. P.; Tyrrell, T.; Charalampopoulou, A.; +3 Authors

    Future climate change as a result of increasing atmospheric CO2 concentrations is expected to strongly affect the oceans, with shallower winter mixing and consequent reduction in primary production and oceanic carbon drawdown in low and mid-latitudinal oceanic regions. Here we test this hypothesis by examining the effects of cold and warm winters on the carbonate system in the surface waters of the Northeast Atlantic Ocean for the period between 2005 and 2007. Monthly observations were made between the English Channel and the Bay of Biscay using a ship of opportunity program. During the colder winter of 2005/2006, the maximum depth of the mixed layer reached up to 650 m in the Bay of Biscay, whilst during the warmer (by 2.6 ± 0.5 °C) winter of 2006/2007 the mixed layer depth reached only 300 m. The inter-annual differences in late winter concentrations of nitrate (2.8 ± 1.1 μmol l−1) and dissolved inorganic carbon (22 ± 6 μmol kg−1, with higher concentrations at the end of the colder winter (2005/2006), led to differences in the dissolved oxygen anomaly and the chlorophyll α-fluorescence data for the subsequent growing season. In contrast to model predictions, the calculated air-sea CO2 fluxes (ranging from +3.7 to −4.8 mmol m−2 d−1) showed an increased oceanic CO2 uptake in the Bay of Biscay following the warmer winter of 2006/2007 associated with wind speed and sea surface temperature differences.

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    Copernicus Publications
    Other ORP type . 2018
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      Copernicus Publications
      Other ORP type . 2018
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    Authors: Prestele, Reinhard; Arneth, Almut; Bondeau, Alberte; Noblet-Ducoudré, Nathalie; +4 Authors

    Land-use and land-cover change (LULCC) represents one of the key drivers of global environmental change. However, the processes and drivers of anthropogenic land-use activity are still overly simplistically implemented in terrestrial biosphere models (TBMs). The published results of these models are used in major assessments of processes and impacts of global environmental change, such as the reports of the Intergovernmental Panel on Climate Change (IPCC). Fully coupled models of climate, land use and biogeochemical cycles to explore land use–climate interactions across spatial scales are currently not available. Instead, information on land use is provided as exogenous data from the land-use change modules of integrated assessment models (IAMs) to TBMs. In this article, we discuss, based on literature review and illustrative analysis of empirical and modeled LULCC data, three major challenges of this current LULCC representation and their implications for land use–climate interaction studies: (I) provision of consistent, harmonized, land-use time series spanning from historical reconstructions to future projections while accounting for uncertainties associated with different land-use modeling approaches, (II) accounting for sub-grid processes and bidirectional changes (gross changes) across spatial scales, and (III) the allocation strategy of independent land-use data at the grid cell level in TBMs. We discuss the factors that hamper the development of improved land-use representation, which sufficiently accounts for uncertainties in the land-use modeling process. We propose that LULCC data-provider and user communities should engage in the joint development and evaluation of enhanced LULCC time series, which account for the diversity of LULCC modeling and increasingly include empirically based information about sub-grid processes and land-use transition trajectories, to improve the representation of land use in TBMs. Moreover, we suggest concentrating on the development of integrated modeling frameworks that may provide further understanding of possible land–climate–society feedbacks.

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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: Leedham, E. C.; Hughes, C.; Keng, F. S. L.; Phang, S.-M.; +2 Authors

    Current estimates of global halocarbon emissions highlight the tropical coastal environment as an important source of very short-lived (VSL) biogenic halocarbons to the troposphere and stratosphere, due to a combination of assumed high primary productivity in tropical coastal waters and the prevalence of deep convective transport, potentially capable of rapidly lifting surface emissions to the upper troposphere/lower stratosphere. However, despite this perceived importance, direct measurements of tropical coastal biogenic halocarbon emissions, notably from macroalgae (seaweeds), have not been made. In light of this, we provide the first dedicated study of halocarbon production by a range of 15 common tropical macroalgal species and compare these results to those from previous studies of polar and temperate macroalgae. Variation between species was substantial; CHBr3 production rates, measured at the end of a 24 h incubation, varied from 1.4 to 1129 pmol g FW−1 h−1 (FW = fresh weight of sample). We used our laboratory-determined emission rates to estimate emissions of CHBr3 and CH2Br2 (the two dominant VSL precursors of stratospheric bromine) from the coastlines of Malaysia and elsewhere in South East Asia (SEA). We compare these values to previous top-down model estimates of emissions from these regions and, by using several emission scenarios, we calculate an annual CHBr3 emission of 40 (6–224 Mmol Br−1 yr), a value that is lower than previous estimates. The contribution of tropical aquaculture to current emission budgets is also considered. Whilst the current aquaculture contribution to halocarbon emissions in this regional is small, the potential exists for substantial increases in aquaculture to make a significant contribution to regional halocarbon budgets.

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    Authors: Myriokefalitakis, Stelios; Nenes, Athanasios; Baker, Alex R.; Mihalopoulos, Nikolaos; +1 Authors

    The atmospheric cycle of phosphorus (P) is parameterized here in a state-of-the-art global 3-D chemistry transport model, taking into account primary emissions of total P (TP) and soluble P (DP) associated with mineral dust, combustion particles from natural and anthropogenic sources, bioaerosols, sea spray and volcanic aerosols. For the present day, global TP emissions are calculated to be roughly 1.33 Tg-P yr−1, with the mineral sources contributing more than 80 % to these emissions. The P solubilization from mineral dust under acidic atmospheric conditions is also parameterized in the model and is calculated to contribute about one-third (0.14 Tg-P yr−1) of the global DP atmospheric source. To our knowledge, a unique aspect of our global study is the explicit modeling of the evolution of phosphorus speciation in the atmosphere. The simulated present-day global annual DP deposition flux is 0.45 Tg-P yr−1 (about 40 % over oceans), showing a strong spatial and temporal variability. Present-day simulations of atmospheric P aerosol concentrations and deposition fluxes are satisfactory compared with available observations, indicating however an underestimate of about 70 % on current knowledge of the sources that drive the P atmospheric cycle. Sensitivity simulations using preindustrial (year 1850) anthropogenic and biomass burning emission scenarios showed a present-day increase of 75 % in the P solubilization flux from mineral dust, i.e., the rate at which P is converted into soluble forms, compared to preindustrial times, due to increasing atmospheric acidity over the last 150 years. Future reductions in air pollutants due to the implementation of air-quality regulations are expected to decrease the P solubilization flux from mineral dust by about 30 % in the year 2100 compared to the present day. Considering, however, that all the P contained in bioaerosols is readily available for uptake by marine organisms, and also accounting for all other DP sources, a total bioavailable P flux of about 0.17 Tg-P yr−1 to the oceans is derived. Our calculations further show that in some regions more than half of the bioavailable P deposition flux to the ocean can originate from biological particles, while this contribution is found to maximize in summer when atmospheric deposition impact on the marine ecosystem is the highest due to ocean stratification. Thus, according to this global study, a largely unknown but potentially important role of terrestrial bioaerosols as suppliers of bioavailable P to the global ocean is also revealed. Overall, this work provides new insights to the atmospheric P cycle by demonstrating that biological materials are important carriers of bioavailable P, with very important implications for past and future responses of marine ecosystems to global change.

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    Authors: Wagner, Robert; Yan, Chao; Lehtipalo, Katrianne; Duplissy, Jonathan; +69 Authors

    The formation of secondary particles in the atmosphere accounts for more than half of global cloud condensation nuclei. Experiments at the CERN CLOUD (Cosmics Leaving OUtdoor Droplets) chamber have underlined the importance of ions for new particle formation, but quantifying their effect in the atmosphere remains challenging. By using a novel instrument setup consisting of two nanoparticle counters, one of them equipped with an ion filter, we were able to further investigate the ion-related mechanisms of new particle formation. In autumn 2015, we carried out experiments at CLOUD on four systems of different chemical compositions involving monoterpenes, sulfuric acid, nitrogen oxides, and ammonia. We measured the influence of ions on the nucleation rates under precisely controlled and atmospherically relevant conditions. Our results indicate that ions enhance the nucleation process when the charge is necessary to stabilize newly formed clusters, i.e., in conditions in which neutral clusters are unstable. For charged clusters that were formed by ion-induced nucleation, we were able to measure, for the first time, their progressive neutralization due to recombination with oppositely charged ions. A large fraction of the clusters carried a charge at 1.5 nm diameter. However, depending on particle growth rates and ion concentrations, charged clusters were largely neutralized by ion–ion recombination before they grew to 2.5 nm. At this size, more than 90 % of particles were neutral. In other words, particles may originate from ion-induced nucleation, although they are neutral upon detection at diameters larger than 2.5 nm. Observations at Hyytiälä, Finland, showed lower ion concentrations and a lower contribution of ion-induced nucleation than measured at CLOUD under similar conditions. Although this can be partly explained by the observation that ion-induced fractions decrease towards lower ion concentrations, further investigations are needed to resolve the origin of the discrepancy.

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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: Romero-Alvarez, Johana; Lupaşcu, Aurelia; Lowe, Douglas; Badia, Alba; +4 Authors

    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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    Authors: Stolzenburg, Dominik; Simon, Mario; Ranjithkumar, Ananth; Kürten, Andreas; +74 Authors

    In the present-day atmosphere, sulfuric acid is the most important vapour for aerosol particle formation and initial growth. However, the growth rates of nanoparticles (<10 nm) from sulfuric acid remain poorly measured. Therefore, the effect of stabilizing bases, the contribution of ions and the impact of attractive forces on molecular collisions are under debate. Here, we present precise growth rate measurements of uncharged sulfuric acid particles from 1.8 to 10 nm, performed under atmospheric conditions in the CERN (European Organization for Nuclear Research) CLOUD chamber. Our results show that the evaporation of sulfuric acid particles above 2 nm is negligible, and growth proceeds kinetically even at low ammonia concentrations. The experimental growth rates exceed the hard-sphere kinetic limit for the condensation of sulfuric acid. We demonstrate that this results from van der Waals forces between the vapour molecules and particles and disentangle it from charge–dipole interactions. The magnitude of the enhancement depends on the assumed particle hydration and collision kinetics but is increasingly important at smaller sizes, resulting in a steep rise in the observed growth rates with decreasing size. Including the experimental results in a global model, we find that the enhanced growth rate of sulfuric acid particles increases the predicted particle number concentrations in the upper free troposphere by more than 50 %.

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    Authors: Sellitto, Pasquale; Guermazi, Henda; Carboni, Elisa; Siddans, Richard; +1 Authors

    We developed an optimal-estimation algorithm to simultaneously retrieve, for the first time, coexisting volcanic gaseous SO2 and sulfate aerosols (SA) from ground-based Fourier transform infrared (FTIR) observations. These effluents, both linked to magmatic degassing process and subsequent atmospheric evolution processes, have overlapping spectral signatures leading to mutual potential interferences when retrieving one species without considering the other. We show that significant overestimations may be introduced in SO2 retrievals if the radiative impact of coexistent SA is not accounted for, which may have impacted existing SO2 long-term series, e.g. from satellite platforms. The method was applied to proximal observations at Masaya volcano, where SO2 and SA concentrations, and SA acidity, were retrieved. A gas-to-particle sulfur partitioning of 400 and a strong SA acidity (sulfuric acid concentration: 65 %) were found, consistent with past in situ observations at this volcano. This method is easily exportable to other volcanoes to monitor magma extraction processes and the atmospheric sulfur cycle in the case of ash-free plumes.

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      Copernicus Publications
      Other ORP type . 2019
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    Authors: Frege, Carla; Ortega, Ismael K.; Rissanen, Matti P.; Praplan, Arnaud P.; +49 Authors

    It was recently shown by the CERN CLOUD experiment that biogenic highly oxygenated molecules (HOMs) form particles under atmospheric conditions in the absence of sulfuric acid, where ions enhance the nucleation rate by 1–2 orders of magnitude. The biogenic HOMs were produced from ozonolysis of α-pinene at 5 ∘C. Here we extend this study to compare the molecular composition of positive and negative HOM clusters measured with atmospheric pressure interface time-of-flight mass spectrometers (APi-TOFs), at three different temperatures (25, 5 and −25 ∘C). Most negative HOM clusters include a nitrate (NO3-) ion, and the spectra are similar to those seen in the nighttime boreal forest. On the other hand, most positive HOM clusters include an ammonium (NH4+) ion, and the spectra are characterized by mass bands that differ in their molecular weight by ∼ 20 C atoms, corresponding to HOM dimers. At lower temperatures the average oxygen to carbon (O : C) ratio of the HOM clusters decreases for both polarities, reflecting an overall reduction of HOM formation with decreasing temperature. This indicates a decrease in the rate of autoxidation with temperature due to a rather high activation energy as has previously been determined by quantum chemical calculations. Furthermore, at the lowest temperature (−25 ∘C), the presence of C30 clusters shows that HOM monomers start to contribute to the nucleation of positive clusters. These experimental findings are supported by quantum chemical calculations of the binding energies of representative neutral and charged clusters.

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    Copernicus Publications
    Other ORP type . 2019
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      Copernicus Publications
      Other ORP type . 2019
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    Authors: Watson-Parris, Duncan; Schutgens, Nick; Reddington, Carly; Pringle, Kirsty J.; +5 Authors

    Despite ongoing efforts, the vertical distribution of aerosols globally is poorly understood. This in turn leads to large uncertainties in the contributions of the direct and indirect aerosol forcing on climate. Using the Global Aerosol Synthesis and Science Project (GASSP) database – the largest synthesised collection of in-situ aircraft measurements currently available, with more than 1000 flights from 37 campaigns from around the world – we investigate the vertical structure of sub-micron aerosols across a wide range of regions and environments. The application of this unique dataset to assess the vertical distributions of number size distribution and Cloud Condensation Nuclei (CCN) in the global aerosol-climate model ECHAM-HAM reveals that the model underestimates accumulation mode particles in the upper troposphere, especially in remote regions. The processes underlying this discrepancy are explored using different aerosol microphysical schemes and a process sensitivity analysis. These show that the biases are predominantly related to aerosol ageing and removal rather than emissions.

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    Authors: Dumousseaud, C.; Achterberg, E. P.; Tyrrell, T.; Charalampopoulou, A.; +3 Authors

    Future climate change as a result of increasing atmospheric CO2 concentrations is expected to strongly affect the oceans, with shallower winter mixing and consequent reduction in primary production and oceanic carbon drawdown in low and mid-latitudinal oceanic regions. Here we test this hypothesis by examining the effects of cold and warm winters on the carbonate system in the surface waters of the Northeast Atlantic Ocean for the period between 2005 and 2007. Monthly observations were made between the English Channel and the Bay of Biscay using a ship of opportunity program. During the colder winter of 2005/2006, the maximum depth of the mixed layer reached up to 650 m in the Bay of Biscay, whilst during the warmer (by 2.6 ± 0.5 °C) winter of 2006/2007 the mixed layer depth reached only 300 m. The inter-annual differences in late winter concentrations of nitrate (2.8 ± 1.1 μmol l−1) and dissolved inorganic carbon (22 ± 6 μmol kg−1, with higher concentrations at the end of the colder winter (2005/2006), led to differences in the dissolved oxygen anomaly and the chlorophyll α-fluorescence data for the subsequent growing season. In contrast to model predictions, the calculated air-sea CO2 fluxes (ranging from +3.7 to −4.8 mmol m−2 d−1) showed an increased oceanic CO2 uptake in the Bay of Biscay following the warmer winter of 2006/2007 associated with wind speed and sea surface temperature differences.

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      Other ORP type . 2018
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    Authors: Prestele, Reinhard; Arneth, Almut; Bondeau, Alberte; Noblet-Ducoudré, Nathalie; +4 Authors

    Land-use and land-cover change (LULCC) represents one of the key drivers of global environmental change. However, the processes and drivers of anthropogenic land-use activity are still overly simplistically implemented in terrestrial biosphere models (TBMs). The published results of these models are used in major assessments of processes and impacts of global environmental change, such as the reports of the Intergovernmental Panel on Climate Change (IPCC). Fully coupled models of climate, land use and biogeochemical cycles to explore land use–climate interactions across spatial scales are currently not available. Instead, information on land use is provided as exogenous data from the land-use change modules of integrated assessment models (IAMs) to TBMs. In this article, we discuss, based on literature review and illustrative analysis of empirical and modeled LULCC data, three major challenges of this current LULCC representation and their implications for land use–climate interaction studies: (I) provision of consistent, harmonized, land-use time series spanning from historical reconstructions to future projections while accounting for uncertainties associated with different land-use modeling approaches, (II) accounting for sub-grid processes and bidirectional changes (gross changes) across spatial scales, and (III) the allocation strategy of independent land-use data at the grid cell level in TBMs. We discuss the factors that hamper the development of improved land-use representation, which sufficiently accounts for uncertainties in the land-use modeling process. We propose that LULCC data-provider and user communities should engage in the joint development and evaluation of enhanced LULCC time series, which account for the diversity of LULCC modeling and increasingly include empirically based information about sub-grid processes and land-use transition trajectories, to improve the representation of land use in TBMs. Moreover, we suggest concentrating on the development of integrated modeling frameworks that may provide further understanding of possible land–climate–society feedbacks.

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    Authors: Leedham, E. C.; Hughes, C.; Keng, F. S. L.; Phang, S.-M.; +2 Authors