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  • Open Access English
    Authors: 
    Clyne, Margot; Lamarque, Jean-Francois; Mills, Michael J.; Khodri, Myriam; Ball, William; Bekki, Slimane; Dhomse, Sandip S.; Lebas, Nicolas; Mann, Graham; Marshall, Lauren; +13 more
    Project: UKRI | The North Atlantic Climat... (NE/N018001/1), EC | STRATOCLIM (603557), UKRI | Reconciling Volcanic Forc... (NE/S000887/1), NSF | Decadal Prediction Follow... (1430051), SNSF | SPARC International Proje... (138017)

    As part of the Model Intercomparison Project on the climatic response to Volcanic forcing (VolMIP), several climate modeling centers performed a coordinated pre-study experiment with interactive stratospheric aerosol models simulating the volcanic aerosol cloud from an eruption resembling the 1815 Mt. Tambora eruption (VolMIP-Tambora ISA ensemble). The pre-study provided the ancillary ability to assess intermodel diversity in the radiative forcing for a large stratospheric-injecting equatorial eruption when the volcanic aerosol cloud is simulated interactively. An initial analysis of the VolMIP-Tambora ISA ensemble showed large disparities between models in the stratospheric global mean aerosol optical depth (AOD). In this study, we now show that stratospheric global mean AOD differences among the participating models are primarily due to differences in aerosol size, which we track here by effective radius. We identify specific physical and chemical processes that are missing in some models and/or parameterized differently between models, which are together causing the differences in effective radius. In particular, our analysis indicates that interactively tracking hydroxyl radical (OH) chemistry following a large volcanic injection of sulfur dioxide (SO2) is an important factor in allowing for the timescale for sulfate formation to be properly simulated. In addition, depending on the timescale of sulfate formation, there can be a large difference in effective radius and subsequently AOD that results from whether the SO2 is injected in a single model grid cell near the location of the volcanic eruption, or whether it is injected as a longitudinally averaged band around the Earth.

  • Open Access English
    Authors: 
    Zouzoua, Maurin; Lohou, Fabienne; Assamoi, Paul; Lothon, Marie; Yoboue, Véronique; Dione, Cheikh; Kalthoff, Norbert; Adler, Bianca; Babić, Karmen; Pedruzo-Bagazgoitia, Xabier; +1 more
    Project: EC | DACCIWA (603502)

    Within the framework of the DACCIWA (Dynamics–Aerosol–Chemistry–Cloud Interactions in West Africa) project and based on a field experiment conducted in June and July 2016, we analyze the daytime breakup of continental low-level stratiform clouds in southern West Africa. We use the observational data gathered during 22 precipitation-free occurrences at Savè, Benin. Our analysis, which starts from the stratiform cloud formation usually at night, focuses on the role played by the coupling between cloud and surface in the transition towards shallow convective clouds during daytime. It is based on several diagnostics, including the Richardson number and various cloud macrophysical properties. The distance between the cloud base height and lifting condensation level is used as a criterion of coupling. We also make an attempt to estimate the most predominant terms of the liquid water path budget in the early morning. When the nocturnal low-level stratiform cloud forms, it is decoupled from the surface except in one case. In the early morning, the cloud is found coupled with the surface in 9 cases and remains decoupled in the 13 other cases. The coupling, which occurs within the 4 h after cloud formation, is accompanied by cloud base lowering and near-neutral thermal stability in the subcloud layer. Further, at the initial stage of the transition, the stratiform cloud base is slightly cooler, wetter and more homogeneous in coupled cases. The moisture jump at the cloud top is usually found to be lower than 2 g kg−1 and the temperature jump within 1–5 K, which is significantly smaller than typical marine stratocumulus and explained by the monsoon flow environment in which the stratiform cloud develops over West Africa. No significant difference in liquid water path budget terms was found between coupled and decoupled cases. In agreement with previous numerical studies, we found that the stratiform cloud maintenance before sunrise results from the interplay between the predominant radiative cooling, entrainment and large-scale subsidence at its top. Three transition scenarios were observed depending on the state of coupling at the initial stage. In coupled cases, the low-level stratiform cloud remains coupled until its breakup. In five of the decoupled cases, the cloud couples with the surface as the lifting condensation level rises. In the eight remaining cases, the stratiform cloud remains hypothetically decoupled from the surface throughout its life cycle since the height of its base remains separated from the condensation level. In cases of coupling during the transition, the stratiform cloud base lifts with the growing convective boundary layer roughly between 06:30 and 08:00 UTC. The cloud deck breakup, occurring at 11:00 UTC or later, leads to the formation of shallow convective clouds. When the decoupling subsists, shallow cumulus clouds form below the stratiform cloud deck between 06:30 and 09:00 UTC. The breakup time in this scenario has a stronger variability and occurs before 11:00 UTC in most cases. Thus, we argue that the coupling with the surface during daytime hours has a crucial role in the low-level stratiform cloud maintenance and its transition towards shallow convective clouds.

  • Open Access English
    Authors: 
    Debevec, Cécile; Sauvage, Stéphane; Gros, Valérie; Salameh, Thérèse; Sciare, Jean; Dulac, François; Locoge, Nadine;
    Project: ANR | Cappa (ANR-11-LABX-0005), EC | DEFI-VOC (293897)

    An original time series of about 300 atmospheric measurements of a wide range of volatile organic compounds (VOCs) was obtained at a remote Mediterranean station on the northern tip of Corsica (Ersa, France) over 25 months from June 2012 to June 2014. This study presents the seasonal variabilities of 35 selected VOCs and their various associated sources. The VOC abundance was largely dominated by oxygenated VOCs (OVOCs) along with primary anthropogenic VOCs with a long lifetime in the atmosphere. VOC temporal variations were then examined. Primarily of local origin, biogenic VOCs exhibited notable seasonal and interannual variations, related to temperature and solar radiation. Anthropogenic compounds showed increased concentrations in winter (JFM months) followed by a decrease in spring/summer (AMJ/JAS months) and higher winter concentration levels in 2013 than in 2014 by up to 0.3 µg m−3 in the cases of propane, acetylene and benzene. OVOC concentrations were generally high in summertime, mainly due to secondary anthropogenic/biogenic and primary biogenic sources, whereas their lower concentrations during autumn and winter were potentially more influenced by primary/secondary anthropogenic sources. Moreover, an apportionment factorial analysis was applied to a database comprising a selection of 14 individual or grouped VOCs by means of the positive matrix factorization (PMF) technique. A PMF five-factor solution was taken on. It includes an anthropogenic factor (which contributed 39 % to the total concentration of the VOCs selected in the PMF analysis) connected to the regional background pollution, three other anthropogenic factors (namely short-lived anthropogenic sources, evaporative sources, and long-lived combustion sources, which together accounted for 57 %) originating from either nearby or more distant emission areas (such as Italy and south of France), and a local biogenic source (4 %). Variations in these main sources impacting VOC concentrations observed at the Ersa station were also investigated at seasonal and interannual scales. In spring and summer, VOC concentrations observed at Ersa were the lowest in the 2-year period, despite higher biogenic source contributions. During these seasons, anthropogenic sources advected to Ersa were largely influenced by chemical transformations and vertical dispersion phenomena and were mainly of regional origins. During autumn and winter, anthropogenic sources showed higher contributions when European air masses were advected to Ersa and could be associated with potential emission areas located in Italy and possibly more distant ones in central Europe. Higher VOC winter concentrations in 2013 than in 2014 could be related to contribution variations in anthropogenic sources probably governed by their emission strength with external parameters, i.e. weaker dispersion phenomena and the pollutant depletion. High-frequency observations collected during several intensive field campaigns conducted at Ersa during the three summers 2012–2014 confirmed findings drawn from bi-weekly samples of the 2-year period in terms of summer concentration levels and source apportionment. However, they also suggested that higher sampling frequency and temporal resolution, in particular to observe VOC concentration variations during the daily cycle, would have been necessary to confirm the deconvolution of the different anthropogenic sources identified following the PMF approach. Finally, comparisons of the 25 months of Ersa observations with VOC measurements conducted at 17 other European monitoring stations highlighted the representativeness of the Ersa station for monitoring seasonal variations in VOC regional pollution impacting continental Europe. Nevertheless, VOC winter concentration levels can significantly vary between sites, pointing out spatial variations in anthropogenic source contributions. As a result, Ersa concentration variations in winter were more representative of VOC regional pollution impacting central Europe. Moreover, interannual and spatial variations in VOC winter concentration levels were significantly impacted by synoptic phenomena influencing meteorological conditions observed in continental Europe, suggesting that short observation periods may reflect the variability of the identified parameters under the specific meteorological conditions of the study period.

  • Open Access English
    Authors: 
    Schrod, Jann; Thomson, Erik S.; Weber, Daniel; Kossmann, Jens; Pöhlker, Christopher; Saturno, Jorge; Ditas, Florian; Artaxo, Paulo; Clouard, Valérie; Saurel, Jean-Marie; +3 more
    Project: EC | BACCHUS (603445)

    Ice particle activation and evolution have important atmospheric implications for cloud formation, initiation of precipitation and radiative interactions. The initial formation of atmospheric ice by heterogeneous ice nucleation requires the presence of a nucleating seed, an ice-nucleating particle (INP), to facilitate its first emergence. Unfortunately, only a few long-term measurements of INPs exist, and as a result, knowledge about geographic and seasonal variations of INP concentrations is sparse. Here we present data from nearly 2 years of INP measurements from four stations in different regions of the world: the Amazon (Brazil), the Caribbean (Martinique), central Europe (Germany) and the Arctic (Svalbard). The sites feature diverse geographical climates and ecosystems that are associated with dissimilar transport patterns, aerosol characteristics and levels of anthropogenic impact (ranging from near pristine to mostly rural). Interestingly, observed INP concentrations, which represent measurements in the deposition and condensation freezing modes, do not differ greatly from site to site but usually fall well within the same order of magnitude. Moreover, short-term variability overwhelms all long-term trends and/or seasonality in the INP concentration at all locations. An analysis of the frequency distributions of INP concentrations suggests that INPs tend to be well mixed and reflective of large-scale air mass movements. No universal physical or chemical parameter could be identified to be a causal link driving INP climatology, highlighting the complex nature of the ice nucleation process. Amazonian INP concentrations were mostly unaffected by the biomass burning season, even though aerosol concentrations increase by a factor of 10 from the wet to dry season. Caribbean INPs were positively correlated to parameters related to transported mineral dust, which is known to increase during the Northern Hemisphere summer. A wind sector analysis revealed the absence of an anthropogenic impact on average INP concentrations at the site in central Europe. Likewise, no Arctic haze influence was observed on INPs at the Arctic site, where low concentrations were generally measured. We consider the collected data to be a unique resource for the community that illustrates some of the challenges and knowledge gaps of the field in general, while specifically highlighting the need for more long-term observations of INPs worldwide.

  • Open Access English
    Authors: 
    Rowlinson, Matthew J.; Rap, Alexandru; Hamilton, Douglas S.; Pope, Richard J.; Hantson, Stijn; Arnold, Steve R.; Kaplan, Jed O.; Arneth, Almut; Chipperfield, Martyn P.; Forster, Piers M.; +1 more
    Project: UKRI | NERC Science @ Leeds and ... (NE/L002574/1), EC | CONSTRAIN (820829), EC | BACCHUS (603445), EC | LUC4C (603542)

    Tropospheric ozone concentrations are sensitive to natural emissions of precursor compounds. In contrast to existing assumptions, recent evidence indicates that terrestrial vegetation emissions in the pre-industrial era were larger than in the present day. We use a chemical transport model and a radiative transfer model to show that revised inventories of pre-industrial fire and biogenic emissions lead to an increase in simulated pre-industrial ozone concentrations, decreasing the estimated pre-industrial to present-day tropospheric ozone radiative forcing by up to 34 % (0.38 to 0.25 W m−2). We find that this change is sensitive to employing biomass burning and biogenic emissions inventories based on matching vegetation patterns, as the co-location of emission sources enhances the effect on ozone formation. Our forcing estimates are at the lower end of existing uncertainty range estimates (0.2–0.6 W m−2), without accounting for other sources of uncertainty. Thus, future work should focus on reassessing the uncertainty range of tropospheric ozone radiative forcing.

  • Open Access English
    Authors: 
    Stolzenburg, Dominik; Simon, Mario; Ranjithkumar, Ananth; Kürten, Andreas; Lehtipalo, Katrianne; Gordon, Hamish; Ehrhart, Sebastian; Finkenzeller, Henning; Pichelstorfer, Lukas; Nieminen, Tuomo; +68 more
    Project: EC | COFUND-FP-CERN-2014 (665779), EC | CLOUD-MOTION (764991), FCT | CERN/FIS-COM/0014/2017 (CERN/FIS-COM/0014/2017), NSF | Collaborative Research: C... (1801280), AKA | Molecular steps of gas-to... (296628), SNSF | CLOUD Infrastructure proj... (172622), AKA | From Autoxidation to Auto... (299574), EC | NANODYNAMITE (616075), FWF | Chemical composition of a... (P 27295), AKA | Centre of Excellence in A... (307331),...

    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 %.

  • Open Access English
    Authors: 
    Johansson, Sören; Höpfner, Michael; Kirner, Oliver; Wohltmann, Ingo; Bucci, Silvia; Legras, Bernard; Friedl-Vallon, Felix; Glatthor, Norbert; Kretschmer, Erik; Ungermann, Jörn; +1 more
    Project: EC | STRATOCLIM (603557)

    We present the first high-resolution measurements of pollutant trace gases in the Asian summer monsoon upper troposphere and lowermost stratosphere (UTLS) from the Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) during the StratoClim (Stratospheric and upper tropospheric processes for better climate predictions) campaign based in Kathmandu, Nepal, 2017. Measurements of peroxyacetyl nitrate (PAN), acetylene (C2H2), and formic acid (HCOOH) show strong local enhancements up to altitudes of 16 km. More than 500 pptv of PAN, more than 200 pptv of C2H2, and more than 200 pptv of HCOOH are observed. Air masses with increased volume mixing ratios of PAN and C2H2 at altitudes up to 18 km, reaching to the lowermost stratosphere, were present at these altitudes for more than 10 d, as indicated by trajectory analysis. A local minimum of HCOOH is correlated with a previously reported maximum of ammonia (NH3), which suggests different washout efficiencies of these species in the same air masses. A backward trajectory analysis based on the models Alfred Wegener InsTitute LAgrangian Chemistry/Transport System (ATLAS) and TRACZILLA, using advanced techniques for detection of convective events, and starting at geolocations of GLORIA measurements with enhanced pollution trace gas concentrations, has been performed. The analysis shows that convective events along trajectories leading to GLORIA measurements with enhanced pollutants are located close to regions where satellite measurements by the Ozone Monitoring Instrument (OMI) indicate enhanced tropospheric columns of nitrogen dioxide (NO2) in the days prior to the observation. A comparison to the global atmospheric models Copernicus Atmosphere Monitoring Service (CAMS) and ECHAM/MESSy Atmospheric Chemistry (EMAC) has been performed. It is shown that these models are able to reproduce large-scale structures of the pollution trace gas distributions for one part of the flight, while the other part of the flight reveals large discrepancies between models and measurement. These discrepancies possibly result from convective events that are not resolved or parameterized in the models, uncertainties in the emissions of source gases, and uncertainties in the rate constants of chemical reactions.

  • Open Access English
    Authors: 
    Brilke, Sophia; Fölker, Nikolaus; Müller, Thomas; Kandler, Konrad; Gong, Xianda; Peischl, Jeff; Weinzierl, Bernadett; Winkler, Paul M.;
    Project: EC | A-LIFE (640458), EC | NANODYNAMITE (616075)

    Atmospheric particle size distributions were measured in Paphos, Cyprus, during the A-LIFE (absorbing aerosol layers in a changing climate: ageing, lifetime and dynamics) field experiment from 3 to 30 April 2017. The newly developed differential mobility analyser train (DMA-train) was deployed for the first time in an atmospheric environment for the direct measurement of the nucleation mode size range between 1.8 and 10 nm diameter. The DMA-train set-up consists of seven size channels, of which five are set to fixed particle mobility diameters and two additional diameters are obtained by alternating voltage settings in one DMA every 10 s. In combination with a conventional mobility particle size spectrometer (MPSS) and an aerodynamic particle sizer (APS) the complete atmospheric aerosol size distribution from 1.8 nm to 10 µm was covered. The focus of the A-LIFE study was to characterize new particle formation (NPF) in the eastern Mediterranean region at a measurement site with strong local pollution sources. The nearby Paphos airport was found to be a large emission source for nucleation mode particles, and we analysed the size distribution of the airport emission plumes at approximately 500 m from the main runway. The analysis yielded nine NPF events in 27 measurement days from the combined analysis of the DMA-train, MPSS and trace gas monitors. Growth rate calculations were performed, and a size dependency of the initial growth rate (<10 nm) was observed for one event case. Fast changes of the sub-10 nm size distribution on a timescale of a few minutes were captured by the DMA-train measurement during early particle growth and are discussed in a second event case. In two cases, particle formation and growth were detected in the nucleation mode size range which did not exceed the 10 nm threshold. This finding implies that NPF likely occurs more frequently than estimated from studies where the lower nanometre size regime is not covered by the size distribution measurements.

  • Open Access English
    Authors: 
    Andersson, August; Kirillova, Elena N.; Decesari, Stefano; DeWitt, Langley; Gasore, Jimmy; Potter, Katherine E.; Prinn, Ronald G.; Rupakheti, Maheswar; Dieu Ndikubwimana, Jean; Nkusi, Julius; +1 more
    Project: EC | HIMALAYABROWNCARBON (623386)

    Sub-Saharan Africa (SSA) is a global hot spot for aerosol emissions, which affect the regional climate and air quality. In this paper, we use ground-based observations to address the large uncertainties in the source-resolved emission estimation of carbonaceous aerosols. Ambient fine fraction aerosol was collected on filters at the high-altitude (2590 m a.s.l.) Rwanda Climate Observatory (RCO), a SSA background site, during the dry and wet seasons in 2014 and 2015. The concentrations of both the carbonaceous and inorganic ion components show a strong seasonal cycle, with highly elevated concentrations during the dry season. Source marker ratios, including carbon isotopes, show that the wet and dry seasons have distinct aerosol compositions. The dry season is characterized by elevated amounts of biomass burning products, which approach ∼95 % for carbonaceous aerosols. An isotopic mass-balance estimate shows that the amount of the carbonaceous aerosol stemming from savanna fires may increase from 0.2 µg m−3 in the wet season up to 10 µg m−3 during the dry season. Based on these results, we quantitatively show that savanna fire is the key modulator of the seasonal aerosol composition variability at the RCO.

  • Open Access English
    Authors: 
    Kipling, Zak; Labbouz, Laurent; Stier, Philip;
    Project: EC | BACCHUS (603445), EC | RECAP (724602), EC | ACCLAIM (280025)

    The interactions between aerosols and convective clouds represent some of the greatest uncertainties in the climate impact of aerosols in the atmosphere. A wide variety of mechanisms have been proposed by which aerosols may invigorate, suppress or change the properties of individual convective clouds, some of which can be reproduced in high-resolution limited-area models. However, there may also be mesoscale, regional or global adjustments which modulate or dampen such impacts which cannot be captured in the limited domain of such models. The Convective Cloud Field Model (CCFM) provides a mechanism to simulate a population of convective clouds, complete with microphysics and interactions between clouds, within each grid column at resolutions used for global climate modelling, so that a representation of the microphysical aerosol response within each parameterised cloud type is possible. Using CCFM within the global aerosol–climate model ECHAM–HAM, we demonstrate how the parameterised cloud field responds to the present-day anthropogenic aerosol perturbation in different regions. In particular, we show that in regions with strongly forced deep convection and/or significant aerosol effects via large-scale processes, the changes in the convective cloud field due to microphysical effects are rather small; however in a more weakly forced regime such as the Caribbean, where large-scale aerosol effects are small, a signature of convective invigoration does become apparent.

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35 Research products, page 1 of 4
  • Open Access English
    Authors: 
    Clyne, Margot; Lamarque, Jean-Francois; Mills, Michael J.; Khodri, Myriam; Ball, William; Bekki, Slimane; Dhomse, Sandip S.; Lebas, Nicolas; Mann, Graham; Marshall, Lauren; +13 more
    Project: UKRI | The North Atlantic Climat... (NE/N018001/1), EC | STRATOCLIM (603557), UKRI | Reconciling Volcanic Forc... (NE/S000887/1), NSF | Decadal Prediction Follow... (1430051), SNSF | SPARC International Proje... (138017)

    As part of the Model Intercomparison Project on the climatic response to Volcanic forcing (VolMIP), several climate modeling centers performed a coordinated pre-study experiment with interactive stratospheric aerosol models simulating the volcanic aerosol cloud from an eruption resembling the 1815 Mt. Tambora eruption (VolMIP-Tambora ISA ensemble). The pre-study provided the ancillary ability to assess intermodel diversity in the radiative forcing for a large stratospheric-injecting equatorial eruption when the volcanic aerosol cloud is simulated interactively. An initial analysis of the VolMIP-Tambora ISA ensemble showed large disparities between models in the stratospheric global mean aerosol optical depth (AOD). In this study, we now show that stratospheric global mean AOD differences among the participating models are primarily due to differences in aerosol size, which we track here by effective radius. We identify specific physical and chemical processes that are missing in some models and/or parameterized differently between models, which are together causing the differences in effective radius. In particular, our analysis indicates that interactively tracking hydroxyl radical (OH) chemistry following a large volcanic injection of sulfur dioxide (SO2) is an important factor in allowing for the timescale for sulfate formation to be properly simulated. In addition, depending on the timescale of sulfate formation, there can be a large difference in effective radius and subsequently AOD that results from whether the SO2 is injected in a single model grid cell near the location of the volcanic eruption, or whether it is injected as a longitudinally averaged band around the Earth.

  • Open Access English
    Authors: 
    Zouzoua, Maurin; Lohou, Fabienne; Assamoi, Paul; Lothon, Marie; Yoboue, Véronique; Dione, Cheikh; Kalthoff, Norbert; Adler, Bianca; Babić, Karmen; Pedruzo-Bagazgoitia, Xabier; +1 more
    Project: EC | DACCIWA (603502)

    Within the framework of the DACCIWA (Dynamics–Aerosol–Chemistry–Cloud Interactions in West Africa) project and based on a field experiment conducted in June and July 2016, we analyze the daytime breakup of continental low-level stratiform clouds in southern West Africa. We use the observational data gathered during 22 precipitation-free occurrences at Savè, Benin. Our analysis, which starts from the stratiform cloud formation usually at night, focuses on the role played by the coupling between cloud and surface in the transition towards shallow convective clouds during daytime. It is based on several diagnostics, including the Richardson number and various cloud macrophysical properties. The distance between the cloud base height and lifting condensation level is used as a criterion of coupling. We also make an attempt to estimate the most predominant terms of the liquid water path budget in the early morning. When the nocturnal low-level stratiform cloud forms, it is decoupled from the surface except in one case. In the early morning, the cloud is found coupled with the surface in 9 cases and remains decoupled in the 13 other cases. The coupling, which occurs within the 4 h after cloud formation, is accompanied by cloud base lowering and near-neutral thermal stability in the subcloud layer. Further, at the initial stage of the transition, the stratiform cloud base is slightly cooler, wetter and more homogeneous in coupled cases. The moisture jump at the cloud top is usually found to be lower than 2 g kg−1 and the temperature jump within 1–5 K, which is significantly smaller than typical marine stratocumulus and explained by the monsoon flow environment in which the stratiform cloud develops over West Africa. No significant difference in liquid water path budget terms was found between coupled and decoupled cases. In agreement with previous numerical studies, we found that the stratiform cloud maintenance before sunrise results from the interplay between the predominant radiative cooling, entrainment and large-scale subsidence at its top. Three transition scenarios were observed depending on the state of coupling at the initial stage. In coupled cases, the low-level stratiform cloud remains coupled until its breakup. In five of the decoupled cases, the cloud couples with the surface as the lifting condensation level rises. In the eight remaining cases, the stratiform cloud remains hypothetically decoupled from the surface throughout its life cycle since the height of its base remains separated from the condensation level. In cases of coupling during the transition, the stratiform cloud base lifts with the growing convective boundary layer roughly between 06:30 and 08:00 UTC. The cloud deck breakup, occurring at 11:00 UTC or later, leads to the formation of shallow convective clouds. When the decoupling subsists, shallow cumulus clouds form below the stratiform cloud deck between 06:30 and 09:00 UTC. The breakup time in this scenario has a stronger variability and occurs before 11:00 UTC in most cases. Thus, we argue that the coupling with the surface during daytime hours has a crucial role in the low-level stratiform cloud maintenance and its transition towards shallow convective clouds.

  • Open Access English
    Authors: 
    Debevec, Cécile; Sauvage, Stéphane; Gros, Valérie; Salameh, Thérèse; Sciare, Jean; Dulac, François; Locoge, Nadine;
    Project: ANR | Cappa (ANR-11-LABX-0005), EC | DEFI-VOC (293897)

    An original time series of about 300 atmospheric measurements of a wide range of volatile organic compounds (VOCs) was obtained at a remote Mediterranean station on the northern tip of Corsica (Ersa, France) over 25 months from June 2012 to June 2014. This study presents the seasonal variabilities of 35 selected VOCs and their various associated sources. The VOC abundance was largely dominated by oxygenated VOCs (OVOCs) along with primary anthropogenic VOCs with a long lifetime in the atmosphere. VOC temporal variations were then examined. Primarily of local origin, biogenic VOCs exhibited notable seasonal and interannual variations, related to temperature and solar radiation. Anthropogenic compounds showed increased concentrations in winter (JFM months) followed by a decrease in spring/summer (AMJ/JAS months) and higher winter concentration levels in 2013 than in 2014 by up to 0.3 µg m−3 in the cases of propane, acetylene and benzene. OVOC concentrations were generally high in summertime, mainly due to secondary anthropogenic/biogenic and primary biogenic sources, whereas their lower concentrations during autumn and winter were potentially more influenced by primary/secondary anthropogenic sources. Moreover, an apportionment factorial analysis was applied to a database comprising a selection of 14 individual or grouped VOCs by means of the positive matrix factorization (PMF) technique. A PMF five-factor solution was taken on. It includes an anthropogenic factor (which contributed 39 % to the total concentration of the VOCs selected in the PMF analysis) connected to the regional background pollution, three other anthropogenic factors (namely short-lived anthropogenic sources, evaporative sources, and long-lived combustion sources, which together accounted for 57 %) originating from either nearby or more distant emission areas (such as Italy and south of France), and a local biogenic source (4 %). Variations in these main sources impacting VOC concentrations observed at the Ersa station were also investigated at seasonal and interannual scales. In spring and summer, VOC concentrations observed at Ersa were the lowest in the 2-year period, despite higher biogenic source contributions. During these seasons, anthropogenic sources advected to Ersa were largely influenced by chemical transformations and vertical dispersion phenomena and were mainly of regional origins. During autumn and winter, anthropogenic sources showed higher contributions when European air masses were advected to Ersa and could be associated with potential emission areas located in Italy and possibly more distant ones in central Europe. Higher VOC winter concentrations in 2013 than in 2014 could be related to contribution variations in anthropogenic sources probably governed by their emission strength with external parameters, i.e. weaker dispersion phenomena and the pollutant depletion. High-frequency observations collected during several intensive field campaigns conducted at Ersa during the three summers 2012–2014 confirmed findings drawn from bi-weekly samples of the 2-year period in terms of summer concentration levels and source apportionment. However, they also suggested that higher sampling frequency and temporal resolution, in particular to observe VOC concentration variations during the daily cycle, would have been necessary to confirm the deconvolution of the different anthropogenic sources identified following the PMF approach. Finally, comparisons of the 25 months of Ersa observations with VOC measurements conducted at 17 other European monitoring stations highlighted the representativeness of the Ersa station for monitoring seasonal variations in VOC regional pollution impacting continental Europe. Nevertheless, VOC winter concentration levels can significantly vary between sites, pointing out spatial variations in anthropogenic source contributions. As a result, Ersa concentration variations in winter were more representative of VOC regional pollution impacting central Europe. Moreover, interannual and spatial variations in VOC winter concentration levels were significantly impacted by synoptic phenomena influencing meteorological conditions observed in continental Europe, suggesting that short observation periods may reflect the variability of the identified parameters under the specific meteorological conditions of the study period.

  • Open Access English
    Authors: 
    Schrod, Jann; Thomson, Erik S.; Weber, Daniel; Kossmann, Jens; Pöhlker, Christopher; Saturno, Jorge; Ditas, Florian; Artaxo, Paulo; Clouard, Valérie; Saurel, Jean-Marie; +3 more
    Project: EC | BACCHUS (603445)

    Ice particle activation and evolution have important atmospheric implications for cloud formation, initiation of precipitation and radiative interactions. The initial formation of atmospheric ice by heterogeneous ice nucleation requires the presence of a nucleating seed, an ice-nucleating particle (INP), to facilitate its first emergence. Unfortunately, only a few long-term measurements of INPs exist, and as a result, knowledge about geographic and seasonal variations of INP concentrations is sparse. Here we present data from nearly 2 years of INP measurements from four stations in different regions of the world: the Amazon (Brazil), the Caribbean (Martinique), central Europe (Germany) and the Arctic (Svalbard). The sites feature diverse geographical climates and ecosystems that are associated with dissimilar transport patterns, aerosol characteristics and levels of anthropogenic impact (ranging from near pristine to mostly rural). Interestingly, observed INP concentrations, which represent measurements in the deposition and condensation freezing modes, do not differ greatly from site to site but usually fall well within the same order of magnitude. Moreover, short-term variability overwhelms all long-term trends and/or seasonality in the INP concentration at all locations. An analysis of the frequency distributions of INP concentrations suggests that INPs tend to be well mixed and reflective of large-scale air mass movements. No universal physical or chemical parameter could be identified to be a causal link driving INP climatology, highlighting the complex nature of the ice nucleation process. Amazonian INP concentrations were mostly unaffected by the biomass burning season, even though aerosol concentrations increase by a factor of 10 from the wet to dry season. Caribbean INPs were positively correlated to parameters related to transported mineral dust, which is known to increase during the Northern Hemisphere summer. A wind sector analysis revealed the absence of an anthropogenic impact on average INP concentrations at the site in central Europe. Likewise, no Arctic haze influence was observed on INPs at the Arctic site, where low concentrations were generally measured. We consider the collected data to be a unique resource for the community that illustrates some of the challenges and knowledge gaps of the field in general, while specifically highlighting the need for more long-term observations of INPs worldwide.

  • Open Access English
    Authors: 
    Rowlinson, Matthew J.; Rap, Alexandru; Hamilton, Douglas S.; Pope, Richard J.; Hantson, Stijn; Arnold, Steve R.; Kaplan, Jed O.; Arneth, Almut; Chipperfield, Martyn P.; Forster, Piers M.; +1 more
    Project: UKRI | NERC Science @ Leeds and ... (NE/L002574/1), EC | CONSTRAIN (820829), EC | BACCHUS (603445), EC | LUC4C (603542)

    Tropospheric ozone concentrations are sensitive to natural emissions of precursor compounds. In contrast to existing assumptions, recent evidence indicates that terrestrial vegetation emissions in the pre-industrial era were larger than in the present day. We use a chemical transport model and a radiative transfer model to show that revised inventories of pre-industrial fire and biogenic emissions lead to an increase in simulated pre-industrial ozone concentrations, decreasing the estimated pre-industrial to present-day tropospheric ozone radiative forcing by up to 34 % (0.38 to 0.25 W m−2). We find that this change is sensitive to employing biomass burning and biogenic emissions inventories based on matching vegetation patterns, as the co-location of emission sources enhances the effect on ozone formation. Our forcing estimates are at the lower end of existing uncertainty range estimates (0.2–0.6 W m−2), without accounting for other sources of uncertainty. Thus, future work should focus on reassessing the uncertainty range of tropospheric ozone radiative forcing.

  • Open Access English
    Authors: 
    Stolzenburg, Dominik; Simon, Mario; Ranjithkumar, Ananth; Kürten, Andreas; Lehtipalo, Katrianne; Gordon, Hamish; Ehrhart, Sebastian; Finkenzeller, Henning; Pichelstorfer, Lukas; Nieminen, Tuomo; +68 more
    Project: EC | COFUND-FP-CERN-2014 (665779), EC | CLOUD-MOTION (764991), FCT | CERN/FIS-COM/0014/2017 (CERN/FIS-COM/0014/2017), NSF | Collaborative Research: C... (1801280), AKA | Molecular steps of gas-to... (296628), SNSF | CLOUD Infrastructure proj... (172622), AKA | From Autoxidation to Auto... (299574), EC | NANODYNAMITE (616075), FWF | Chemical composition of a... (P 27295), AKA | Centre of Excellence in A... (307331),...

    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 %.

  • Open Access English
    Authors: 
    Johansson, Sören; Höpfner, Michael; Kirner, Oliver; Wohltmann, Ingo; Bucci, Silvia; Legras, Bernard; Friedl-Vallon, Felix; Glatthor, Norbert; Kretschmer, Erik; Ungermann, Jörn; +1 more
    Project: EC | STRATOCLIM (603557)

    We present the first high-resolution measurements of pollutant trace gases in the Asian summer monsoon upper troposphere and lowermost stratosphere (UTLS) from the Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) during the StratoClim (Stratospheric and upper tropospheric processes for better climate predictions) campaign based in Kathmandu, Nepal, 2017. Measurements of peroxyacetyl nitrate (PAN), acetylene (C2H2), and formic acid (HCOOH) show strong local enhancements up to altitudes of 16 km. More than 500 pptv of PAN, more than 200 pptv of C2H2, and more than 200 pptv of HCOOH are observed. Air masses with increased volume mixing ratios of PAN and C2H2 at altitudes up to 18 km, reaching to the lowermost stratosphere, were present at these altitudes for more than 10 d, as indicated by trajectory analysis. A local minimum of HCOOH is correlated with a previously reported maximum of ammonia (NH3), which suggests different washout efficiencies of these species in the same air masses. A backward trajectory analysis based on the models Alfred Wegener InsTitute LAgrangian Chemistry/Transport System (ATLAS) and TRACZILLA, using advanced techniques for detection of convective events, and starting at geolocations of GLORIA measurements with enhanced pollution trace gas concentrations, has been performed. The analysis shows that convective events along trajectories leading to GLORIA measurements with enhanced pollutants are located close to regions where satellite measurements by the Ozone Monitoring Instrument (OMI) indicate enhanced tropospheric columns of nitrogen dioxide (NO2) in the days prior to the observation. A comparison to the global atmospheric models Copernicus Atmosphere Monitoring Service (CAMS) and ECHAM/MESSy Atmospheric Chemistry (EMAC) has been performed. It is shown that these models are able to reproduce large-scale structures of the pollution trace gas distributions for one part of the flight, while the other part of the flight reveals large discrepancies between models and measurement. These discrepancies possibly result from convective events that are not resolved or parameterized in the models, uncertainties in the emissions of source gases, and uncertainties in the rate constants of chemical reactions.

  • Open Access English
    Authors: 
    Brilke, Sophia; Fölker, Nikolaus; Müller, Thomas; Kandler, Konrad; Gong, Xianda; Peischl, Jeff; Weinzierl, Bernadett; Winkler, Paul M.;
    Project: EC | A-LIFE (640458), EC | NANODYNAMITE (616075)

    Atmospheric particle size distributions were measured in Paphos, Cyprus, during the A-LIFE (absorbing aerosol layers in a changing climate: ageing, lifetime and dynamics) field experiment from 3 to 30 April 2017. The newly developed differential mobility analyser train (DMA-train) was deployed for the first time in an atmospheric environment for the direct measurement of the nucleation mode size range between 1.8 and 10 nm diameter. The DMA-train set-up consists of seven size channels, of which five are set to fixed particle mobility diameters and two additional diameters are obtained by alternating voltage settings in one DMA every 10 s. In combination with a conventional mobility particle size spectrometer (MPSS) and an aerodynamic particle sizer (APS) the complete atmospheric aerosol size distribution from 1.8 nm to 10 µm was covered. The focus of the A-LIFE study was to characterize new particle formation (NPF) in the eastern Mediterranean region at a measurement site with strong local pollution sources. The nearby Paphos airport was found to be a large emission source for nucleation mode particles, and we analysed the size distribution of the airport emission plumes at approximately 500 m from the main runway. The analysis yielded nine NPF events in 27 measurement days from the combined analysis of the DMA-train, MPSS and trace gas monitors. Growth rate calculations were performed, and a size dependency of the initial growth rate (<10 nm) was observed for one event case. Fast changes of the sub-10 nm size distribution on a timescale of a few minutes were captured by the DMA-train measurement during early particle growth and are discussed in a second event case. In two cases, particle formation and growth were detected in the nucleation mode size range which did not exceed the 10 nm threshold. This finding implies that NPF likely occurs more frequently than estimated from studies where the lower nanometre size regime is not covered by the size distribution measurements.

  • Open Access English
    Authors: 
    Andersson, August; Kirillova, Elena N.; Decesari, Stefano; DeWitt, Langley; Gasore, Jimmy; Potter, Katherine E.; Prinn, Ronald G.; Rupakheti, Maheswar; Dieu Ndikubwimana, Jean; Nkusi, Julius; +1 more
    Project: EC | HIMALAYABROWNCARBON (623386)

    Sub-Saharan Africa (SSA) is a global hot spot for aerosol emissions, which affect the regional climate and air quality. In this paper, we use ground-based observations to address the large uncertainties in the source-resolved emission estimation of carbonaceous aerosols. Ambient fine fraction aerosol was collected on filters at the high-altitude (2590 m a.s.l.) Rwanda Climate Observatory (RCO), a SSA background site, during the dry and wet seasons in 2014 and 2015. The concentrations of both the carbonaceous and inorganic ion components show a strong seasonal cycle, with highly elevated concentrations during the dry season. Source marker ratios, including carbon isotopes, show that the wet and dry seasons have distinct aerosol compositions. The dry season is characterized by elevated amounts of biomass burning products, which approach ∼95 % for carbonaceous aerosols. An isotopic mass-balance estimate shows that the amount of the carbonaceous aerosol stemming from savanna fires may increase from 0.2 µg m−3 in the wet season up to 10 µg m−3 during the dry season. Based on these results, we quantitatively show that savanna fire is the key modulator of the seasonal aerosol composition variability at the RCO.

  • Open Access English
    Authors: 
    Kipling, Zak; Labbouz, Laurent; Stier, Philip;
    Project: EC | BACCHUS (603445), EC | RECAP (724602), EC | ACCLAIM (280025)

    The interactions between aerosols and convective clouds represent some of the greatest uncertainties in the climate impact of aerosols in the atmosphere. A wide variety of mechanisms have been proposed by which aerosols may invigorate, suppress or change the properties of individual convective clouds, some of which can be reproduced in high-resolution limited-area models. However, there may also be mesoscale, regional or global adjustments which modulate or dampen such impacts which cannot be captured in the limited domain of such models. The Convective Cloud Field Model (CCFM) provides a mechanism to simulate a population of convective clouds, complete with microphysics and interactions between clouds, within each grid column at resolutions used for global climate modelling, so that a representation of the microphysical aerosol response within each parameterised cloud type is possible. Using CCFM within the global aerosol–climate model ECHAM–HAM, we demonstrate how the parameterised cloud field responds to the present-day anthropogenic aerosol perturbation in different regions. In particular, we show that in regions with strongly forced deep convection and/or significant aerosol effects via large-scale processes, the changes in the convective cloud field due to microphysical effects are rather small; however in a more weakly forced regime such as the Caribbean, where large-scale aerosol effects are small, a signature of convective invigoration does become apparent.

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