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  • 2013-2022
  • Research software
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  • European Commission
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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/ 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/
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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/
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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 %.

    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/ 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/
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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.

    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 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: 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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    Copernicus Publications
    Other ORP type . 2018
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      Copernicus Publications
      Other ORP type . 2018
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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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    Other ORP type . 2018
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    Authors: Sala, S.; Bönisch, H.; Keber, T.; Oram, D. E.; +2 Authors

    During the recent SHIVA (Stratospheric Ozone: Halogen Impacts in a Varying Atmosphere) project an extensive data set of all halogen species relevant for the atmospheric budget of total organic bromine was collected in the western Pacific region using the Falcon aircraft operated by the German Aerospace agency DLR (Deutsches Zentrum für Luft- und Raumfahrt) covering a vertical range from the planetary boundary layer up to the ceiling altitude of the aircraft of 13 km. In total, more than 700 measurements were performed with the newly developed fully automated in situ instrument GHOST-MS (Gas chromatograph for the Observation of Tracers – coupled with a Mass Spectrometer) by the Goethe University of Frankfurt (GUF) and with the onboard whole-air sampler WASP with subsequent ground-based state-of-the-art GC / MS analysis by the University of East Anglia (UEA). Both instruments yield good agreement for all major (CHBr3 and CH2Br2) and minor (CH2BrCl, CHBrCl2 and CHBr2Cl) VSLS (very short-lived substances), at least at the level of their 2σ measurement uncertainties. In contrast to the suggestion that the western Pacific could be a region of strongly increased atmospheric VSLS abundance (Pyle et al., 2011), we found only in the upper troposphere a slightly enhanced amount of total organic bromine from VSLS relative to the levels reported in Montzka and Reimann et al. (2011) for other tropical regions. From the SHIVA observations in the upper troposphere, a budget for total organic bromine, including four halons (H-1301, H-1211, H-1202, H-2402), CH3Br and the VSLS, is derived for the level of zero radiative heating (LZRH), the input region for the tropical tropopause layer (TTL) and thus also for the stratosphere. With the exception of the two minor VSLS CHBrCl2 and CHBr2Cl, excellent agreement with the values reported in Montzka and Reimann et al. (2011) is found, while being slightly higher than previous studies from our group based on balloon-borne measurements.

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    Other ORP type . 2018
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      Copernicus Publications
      Other ORP type . 2018
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    Authors: Heinze, C.; Meyer, S.; Goris, N.; Anderson, L.; +4 Authors

    Carbon dioxide (CO2) is, next to water vapour, considered to be the most important natural greenhouse gas on Earth. Rapidly rising atmospheric CO2 concentrations caused by human actions such as fossil fuel burning, land-use change or cement production over the past 250 years have given cause for concern that changes in Earth's climate system may progress at a much faster pace and larger extent than during the past 20 000 years. Investigating global carbon cycle pathways and finding suitable adaptation and mitigation strategies has, therefore, become of major concern in many research fields. The oceans have a key role in regulating atmospheric CO2 concentrations and currently take up about 25% of annual anthropogenic carbon emissions to the atmosphere. Questions that yet need to be answered are what the carbon uptake kinetics of the oceans will be in the future and how the increase in oceanic carbon inventory will affect its ecosystems and their services. This requires comprehensive investigations, including high-quality ocean carbon measurements on different spatial and temporal scales, the management of data in sophisticated databases, the application of Earth system models to provide future projections for given emission scenarios as well as a global synthesis and outreach to policy makers. In this paper, the current understanding of the ocean as an important carbon sink is reviewed with respect to these topics. Emphasis is placed on the complex interplay of different physical, chemical and biological processes that yield both positive and negative air–sea flux values for natural and anthropogenic CO2 as well as on increased CO2 (uptake) as the regulating force of the radiative warming of the atmosphere and the gradual acidification of the oceans. Major future ocean carbon challenges in the fields of ocean observations, modelling and process research as well as the relevance of other biogeochemical cycles and greenhouse gases are discussed.

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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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    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: 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: 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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    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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      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/
  • 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: 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/
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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: 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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    Authors: Sala, S.; Bönisch, H.; Keber, T.; Oram, D. E.; +2 Authors

    During the recent SHIVA (Stratospheric Ozone: Halogen Impacts in a Varying Atmosphere) project an extensive data set of all halogen species relevant for the atmospheric budget of total organic bromine was collected in the western Pacific region using the Falcon aircraft operated by the German Aerospace agency DLR (Deutsches Zentrum für Luft- und Raumfahrt) covering a vertical range from the planetary boundary layer up to the ceiling altitude of the aircraft of 13 km. In total, more than 700 measurements were performed with the newly developed fully automated in situ instrument GHOST-MS (Gas chromatograph for the Observation of Tracers – coupled with a Mass Spectrometer) by the Goethe University of Frankfurt (GUF) and with the onboard whole-air sampler WASP with subsequent ground-based state-of-the-art GC / MS analysis by the University of East Anglia (UEA). Both instruments yield good agreement for all major (CHBr3 and CH2Br2) and minor (CH2BrCl, CHBrCl2 and CHBr2Cl) VSLS (very short-lived substances), at least at the level of their 2σ measurement uncertainties. In contrast to the suggestion that the western Pacific could be a region of strongly increased atmospheric VSLS abundance (Pyle et al., 2011), we found only in the upper troposphere a slightly enhanced amount of total organic bromine from VSLS relative to the levels reported in Montzka and Reimann et al. (2011) for other tropical regions. From the SHIVA observations in the upper troposphere, a budget for total organic bromine, including four halons (H-1301, H-1211, H-1202, H-2402), CH3Br and the VSLS, is derived for the level of zero radiative heating (LZRH), the input region for the tropical tropopause layer (TTL) and thus also for the stratosphere. With the exception of the two minor VSLS CHBrCl2 and CHBr2Cl, excellent agreement with the values reported in Montzka and Reimann et al. (2011) is found, while being slightly higher than previous studies from our group based on balloon-borne measurements.

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    Copernicus Publications
    Other ORP type . 2018
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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 . 2018
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    Authors: Heinze, C.; Meyer, S.; Goris, N.; Anderson, L.; +4 Authors

    Carbon dioxide (CO2) is, next to water vapour, considered to be the most important natural greenhouse gas on Earth. Rapidly rising atmospheric CO2 concentrations caused by human actions such as fossil fuel burning, land-use change or cement production over the past 250 years have given cause for concern that changes in Earth's climate system may progress at a much faster pace and larger extent than during the past 20 000 years. Investigating global carbon cycle pathways and finding suitable adaptation and mitigation strategies has, therefore, become of major concern in many research fields. The oceans have a key role in regulating atmospheric CO2 concentrations and currently take up about 25% of annual anthropogenic carbon emissions to the atmosphere. Questions that yet need to be answered are what the carbon uptake kinetics of the oceans will be in the future and how the increase in oceanic carbon inventory will affect its ecosystems and their services. This requires comprehensive investigations, including high-quality ocean carbon measurements on different spatial and temporal scales, the management of data in sophisticated databases, the application of Earth system models to provide future projections for given emission scenarios as well as a global synthesis and outreach to policy makers. In this paper, the current understanding of the ocean as an important carbon sink is reviewed with respect to these topics. Emphasis is placed on the complex interplay of different physical, chemical and biological processes that yield both positive and negative air–sea flux values for natural and anthropogenic CO2 as well as on increased CO2 (uptake) as the regulating force of the radiative warming of the atmosphere and the gradual acidification of the oceans. Major future ocean carbon challenges in the fields of ocean observations, modelling and process research as well as the relevance of other biogeochemical cycles and greenhouse gases are discussed.

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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
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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/ Norwegian Open Resea...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 . 2018
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