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Keskinen, Helmi ; Virtanen, Annele ; Joutsensaari, Jorma ; Tsagkogeorgas, Georgios ; Duplissy, Jonathan ; Schobesberger, Siegfried ; Gysel, Martin ; Riccobono, Francesco ; Slowik, Jay G. ; Bianchi, Federico ; Yli-Juuti, Taina ; Lehtipalo, Katrianne ; Rondo, Linda ; Breitenlechner, Martin ; Kupc, Agnieszka ; Almeida, Joao ; Amorin, António ; Dunne, Eimear M. ; Downward, Andrew J. ; Ehrhart, Sebastian ; Franchin, Alessandro ; Kajos, Maija K. ; Kirkby, Jasper ; Kürten, Christoph Andreas ; Nieminen, Tuomo ; Makhmutov, Vladimir ; Mathot, Serge ; Miettinen, Pasi ; Onnela, Antti ; Petäjä, Tuukka ; Praplan, Arnaud Patrick ; Santos, Filipe Duarte ; Schallhart, Simon ; Sipilä, Mikko ; Stozhkov, Yuri ; Tomé, Antonio ; Vaattovaara, Petri ; Wimmer, Daniela ; Prévôt, André Stephan Henry ; Dommen, Josef ; Donahue, Neil McPherson ; Flagan, Richard C. ; Weingartner, Ernest ; Viisanen, Yrjö ; Riipinen, Ilona ; Hansel, Armin ; Curtius, Joachim ; Kulmala, Markku ; Worsnop, Douglas R. ; Baltensperger, Urs ; Wex, Heike ; Stratmann, Frank ; Laaksonen, Ari
Sulphuric acid, ammonia, amines, and oxidised organics play a crucial role in nanoparticle formation in the atmosphere. In this study, we investigate the composition of nucleated nanoparticles formed from these compounds in the CLOUD (Cosmics Leaving Outdoor Droplets) chamber experiments at CERN (Centre européen pour la recherche nucléaire). The investigation was carried out via analysis of the particle hygroscopicity, ethanol affinity, oxidation state, and ion composition. Hygroscopicity was studied by a hygroscopic tandem differential mobility analyser and a cloud condensation nuclei counter, ethanol affinity by an organic differential mobility analyser and particle oxidation level by a high-resolution time-of-flight aerosol mass spectrometer. The ion composition was studied by an atmospheric pressure interface time-of-flight mass spectrometer. The volume fraction of the organics in the particles during their growth from sizes of a few nanometers to tens of nanometers was derived from measured hygroscopicity assuming the Zdanovskii–Stokes–Robinson relationship, and compared to values gained from the spectrometers. The ZSR-relationship was also applied to obtain the measured ethanol affinities during the particle growth, which were used to derive the volume fractions of sulphuric acid and the other inorganics (e.g. ammonium salts). In the presence of sulphuric acid and ammonia, particles with a mobility diameter of 150 nm were chemically neutralised to ammonium sulphate. In the presence of oxidation products of pinanediol, the organic volume fraction of freshly nucleated particles increased from 0.4 to ~0.9, with an increase in diameter from 2 to 63 nm. Conversely, the sulphuric acid volume fraction decreased from 0.6 to 0.1 when the particle diameter increased from 2 to 50 nm. The results provide information on the composition of nucleated aerosol particles during their growth in the presence of various combinations of sulphuric acid, ammonia, dimethylamine and organic oxidation products.
Hobe, Marc von ; Bekki, Slimane ; Borrmann, Stephan ; Cairo, Francesco ; D'Amato, Francesco ; Di Donfrancesco, Guido ; Dörnbrack, Andreas ; Ebersoldt, Andreas ; Ebert, Martin ; Emde, Claudia ; Engel, Ines ; Ern, Manfred ; Frey, Wiebke ; Genco, Silvia ; Griessbach, Sabine ; Grooß, Jens-Uwe ; Gulde, Thomas ; Günther, Gebhard ; Hösen, Elisabeth ; Hoffmann, Lars ; Homonnai, Viktoria ; Hoyle, Christopher Robert ; Isaksen, Ivar S.A. ; Jackson, David R. ; Jánosi, Imre M. ; Jones, Rod L. ; Kandler, Konrad ; Kalicinsky, Christoph ; Keil, Andrea ; Khaykin, Sergey M. ; Khosrawi, Farahnaz ; Kivi, Rigel ; Kuttippurath, Jayan ; Laube, Johannes Christian ; Lefèvre, Franck ; Lehmann, Ralph ; Ludmann, Sabrina ; Luo, Beiping P. ; Marchand, Marion ; Meyer, Jessica ; Mitev, Valentin ; Molleker, Sergej ; Müller, Rolf ; Oelhaf, Hermann ; Olschewski, Friedhelm ; Orsolini, Yvan ; Peter, Thomas ; Pfeilsticker, Klaus ; Piesch, Christof ; Pitts, Michael C. ; Poole, Lamont R. ; Pope, Francis D. ; Ravegnani, Fabrizio ; Rex, Markus ; Riese, Martin ; Röckmann, Thomas ; Rognerud, Bjørg ; Roiger, Anke ; Rolf, Christian ; Santee, Michelle L. ; Scheibe, Monika ; Schiller, Cornelius ; Schlager, Hans ; Siciliani de Cumis, Matteo ; Sitnikov, Nikolay ; Søvde, Ole Amund ; Spang, Reinhold ; Spelten, Nicole ; Stordal, Frode ; Sumińska-Ebersoldt, Olga ; Viciani, Silvia ; Volk, C.-Michael ; vom Scheidt, Marcel ; Ulanovski, Alexey ; Gathen, Peter von der ; Walker, Kaley A. ; Wegner, Tobias ; Weigel, Ralf ; Weinbruch, Stephan ; Wetzel, Gerald ; Wienhold, Franck G. ; Wohltmann, Ingo ; Woiwode, Wolfgang ; Young, Isla A. K. ; Yushkov, Vladimir ; Zobrist, Bernhard ; Stroh, Fred
The international research project RECONCILE has addressed central questions regarding polar ozone depletion, with the objective to quantify some of the most relevant yet still uncertain physical and chemical processes and thereby improve prognostic modelling capabilities to realistically predict the response of the ozone layer to climate change. This overview paper outlines the scope and the general approach of RECONCILE, and it provides a summary of observations and modelling in 2010 and 2011 that have generated an in many respects unprecedented dataset to study processes in the Arctic winter stratosphere. Principally, it summarises important outcomes of RECONCILE including (i) better constraints and enhanced consistency on the set of parameters governing catalytic ozone destruction cycles, (ii) a better understanding of the role of cold binary aerosols in heterogeneous chlorine activation, (iii) an improved scheme of polar stratospheric cloud (PSC) processes that includes heterogeneous nucleation of nitric acid trihydrate (NAT) and ice on non-volatile background aerosol leading to better model parameterisations with respect to denitrification, and (iv) long transient simulations with a chemistry-climate model (CCM) updated based on the results of RECONCILE that better reproduce past ozone trends in Antarctica and are deemed to produce more reliable predictions of future ozone trends. The process studies and the global simulations conducted in RECONCILE show that in the Arctic, ozone depletion uncertainties in the chemical and microphysical processes are now clearly smaller than the sensitivity to dynamic variability.
Hall, Brad D. ; Engel, Andreas ; Mühle, Jens ; Elkins, James William ; Artuso, Florinda ; Atlas, Elliot L. ; Aydin, Murat ; Blake, Donald R. ; Brunke, Ernst-Günther ; Chiavarini, Salvatore ; Fraser, Paul J. ; Happell, James D. ; Krummel, Paul B. ; Levin, Ingeborg ; Loewenstein, Max ; Maione, Michela ; Montzka, Stephen A. ; O'Doherty, Simon ; Reimann, Stefan ; Rhoderick, George J. ; Saltzman, Eric S. ; Scheel, Hans-Eckhart ; Steele, L. Paul ; Vollmer, Martin K. ; Weiss, Ray F. ; Worthy, Douglas E. ; Yokouchi, Yoko
The International Halocarbons in Air Comparison Experiment (IHALACE) was conducted to document relationships between calibration scales among various laboratories that measure atmospheric greenhouse and ozone depleting gases. Six stainless steel cylinders containing natural and modified natural air samples were circulated among 19 laboratories. Results from this experiment reveal relatively good agreement among commonly used calibration scales for a number of trace gases present in the unpolluted atmosphere at pmol mol−1 (parts per trillion) levels, such as chlorofluorocarbons (CFCs), hydrochlorofluorocarbons (HCFCs), and hydrofluorocarbons (HFCs). Some scale relationships were found to be consistent with those derived from bi-lateral experiments or from analysis of atmospheric data, while others revealed discrepancies. The transfer of calibration scales among laboratories was found to be problematic in many cases, meaning that measurements tied to a common scale may not, in fact, be compatible. These results reveal substantial improvements in calibration over previous comparisons. However there is room for improvement in communication and coordination of calibration activities with respect to the measurement of halogenated and related trace gases.
Nölscher, Anke Christine ; Bourtsoukidis, Efstratios ; Bonn, Boris ; Kesselmeier, Jürgen ; Lelieveld, Johannes ; Williams, Jonathan
Numerous reactive volatile organic compounds (VOCs) are emitted into the atmosphere by vegetation. Most biogenic VOCs are highly reactive towards the atmosphere's most important oxidant, the hydroxyl (OH) radical. One way to investigate the chemical interplay between biosphere and atmosphere is through the measurement of total OH reactivity, the total loss rate of OH radicals. This study presents the first determination of total OH reactivity emission rates (measurements via the comparative reactivity method) based on a branch cuvette enclosure system mounted on a Norway spruce (Picea abies) throughout spring, summer and autumn 2011. In parallel VOC emission rates were monitored by a second proton-transfer-reaction mass spectrometer (PTR-MS), and total ozone (O3) loss rates were obtained inside the cuvette. Total OH reactivity emission rates were in general temperature and light dependent, showing strong diel cycles with highest values during daytime. Monoterpene emissions contributed most, accounting for 56–69% of the measured total OH reactivity flux in spring and early summer. However, during late summer and autumn the monoterpene contribution decreased to 11–16%. At this time, a large missing fraction of the total OH reactivity emission rate (70–84%) was found when compared to the VOC budget measured by PTR-MS. Total OH reactivity and missing total OH reactivity emission rates reached maximum values in late summer corresponding to the period of highest temperature. Total O3 loss rates within the closed cuvette showed similar diel profiles and comparable seasonality to the total OH reactivity fluxes.
Total OH reactivity fluxes were also compared to emissions from needle storage pools predicted by a temperature-only-dependent algorithm. Deviations of total OH reactivity fluxes from the temperature-only-dependent emission algorithm were observed for occasions of mechanical and heat stress. While for mechanical stress, induced by strong wind, measured VOCs could explain total OH reactivity emissions, during heat stress they could not. The temperature-driven algorithm matched the diel variation of total OH reactivity emission rates much better in spring than in summer, indicating a different production and emission scheme for summer and early autumn. During these times, unmeasured and possibly unknown primary biogenic emissions contributed significantly to the observed total OH reactivity flux.
has been demonstrated in climate models that both the Indian and East Asian summer monsoons (ISM and EASM) are strengthened by the uplift of the entire Asian orography or Tibetan Plateau (TP) (i.e. bulk mountain uplift). Such an effect is widely perceived as the major mechanism contributing to the evolution of Asian summer monsoons in the Neogene. However, geological evidence suggests more diachronous growth of the Asian orography (i.e. regional mountain uplift) than bulk mountain uplift. This demands a re-evaluation of the relation between mountain uplift and the Asian monsoon in the geological periods. In this study, sensitivity experiments considering the diachronous growth of different parts of the Asian orography are performed using the regional climate model COSMO-CLM to investigate their effects on the Asian summer monsoons. The results show that, different from the bulk mountain uplift, the regional mountain uplift can lead to an asynchronous development of the ISM and EASM. While the ISM is primarily intensified by the thermal insulation (mechanical blocking) effect of the southern TP (Zagros Mountains), the EASM is mainly enhanced by the surface sensible heating of the central, northern and eastern TP. Such elevated surface heating can induce a low-level cyclonic anomaly around the TP that reduces the ISM by suppressing the lower tropospheric monsoon vorticity, but promotes the EASM by strengthening the warm advection from the south of the TP that sustains the monsoon convection. Our findings provide new insights to the evolution of the Asian summer monsoons and their interaction with the tectonic changes in the Neogene.
Spatial interpolation of rain gauge data is important in forcing of hydrological simulations or evaluation of weather predictions, for example. This paper investigates the application of statistical distance, like one minus common variance of observation time series, between data sites instead of geographical distance in interpolation. Here, as a typical representative of interpolation methods the inverse distance weighting interpolation is applied and the test data is daily precipitation observed in Austria. Choosing statistical distance instead of geographical distance in interpolation of available coarse network observations to sites of a denser network, which is not reporting for the interpolation date, yields more robust interpolation results. The most distinct performance enhancement is in or close to mountainous terrain. Therefore, application of statistical distance in the inverse distance weighting interpolation or in similar methods can parsimoniously densify the currently available observation network. Additionally, the success further motivates search for conceptual rain-orography interaction models as components of spatial rain interpolation algorithms in mountainous terrain.
Spatial interpolation of rain gauge data is important in forcing of hydrological simulations or evaluation of weather predictions, for example. The spatial density of available data sites is often changing with time. This paper investigates the application of statistical distance, like one minus common variance of time series, between data sites instead of geographical distance in interpolation. Here, as a typical representative of interpolation methods the inverse distance weighting interpolation is applied and the test data is daily precipitation observed in Austria. Choosing statistical distance instead of geographical distance in interpolation of an actually available coarse observation network yields more robust interpolation results at sites of a denser network with actually lacking observations. The performance enhancement is in or close to mountainous terrain. This has the potential to parsimoniously densify the currently available observation network. Additionally, the success further motivates search for conceptual rain-orography interaction models as components of spatial rain interpolation algorithms in mountainous terrain.
In this study, two different methods were applied to derive daily and monthly sunshine duration based on high-resolution satellite products provided by the European Organisation for the Exploitation of Meteorological Satellites (EUMETSAT) Satellite Application Facility on Climate Monitoring using data from Meteosat Second Generation (MSG) SEVIRI (Spinning Enhanced Visible and Infrared Imager). The satellite products were either hourly cloud type or hourly surface incoming direct radiation. The satellite sunshine duration estimates were not found to be significantly different using the native 15-minute temporal resolution of SEVIRI. The satellite-based sunshine duration products give additional spatial information over the European continent compared with equivalent in situ-based products. An evaluation of the satellite sunshine duration by product intercomparison and against station measurements was carried out to determine their accuracy. The satellite data were found to be within ±1 h/day compared to high-quality Baseline Surface Radiation Network or surface synoptic observations (SYNOP) station measurements. The satellite-based products differ more over the oceans than over land, mainly because of the treatment of fractional clouds in the cloud type-based sunshine duration product. This paper presents the methods used to derive the satellite sunshine duration products and the performance of the different retrievals. The main benefits and disadvantages compared to station-based products are also discussed.
Bernhardt-Römermann, Markus ; Römermann, Christine ; Patta Pillar, Valério de ; Kudernatsch, Thomas ; Fischer, Anton
The current study tested the assumption that floristic and functional diversity patterns are negatively related to soil nitrogen content. We analyzed 20 plots with soil N-contents ranging from 0.63% to 1.06% in a deciduous forest near Munich (Germany). To describe species adaptation strategies to different nitrogen availabilities, we used a plant functional type (PFT) approach. Each identified PFT represents one realized adaptation strategy to the current environment. These were correlated, next to plant species richness and evenness, to soil nitrogen contents. We found that N-efficient species were typical for low soil nitrogen contents, while N-requiring species occur at high N-contents. In contrast to our initial hypotheses, floristic and functional diversity measures (number of PFTs) were positively related to nitrogen content in the soil. Every functional group has its own adaptation to the prevailing environmental conditions; in consequence, these functional groups can co-exist but do not out-compete one another. The increased number of functional groups at high N-contents leads to increased species richness. Hence, for explaining diversity patterns we need to consider species groups representing different adaptations to the current environmental conditions. Such co-existing ecological strategies may even overcome the importance of competition in their effect on biodiversity.
This article presents an environmental remote sensing application using a UAV that is specifically aimed at reducing the data gap between field scale and satellite scale in soil erosion monitoring in Morocco. A fixed-wing aircraft type Sirius I (MAVinci, Germany) equipped with a digital system camera (Panasonic) is employed. UAV surveys are conducted over different study sites with varying extents and flying heights in order to provide both very high resolution site-specific data and lower-resolution overviews, thus fully exploiting the large potential of the chosen UAV for multi-scale mapping purposes. Depending on the scale and area coverage, two different approaches for georeferencing are used, based on high-precision GCPs or the UAV’s log file with exterior orientation values respectively. The photogrammetric image processing enables the creation of Digital Terrain Models (DTMs) and ortho-image mosaics with very high resolution on a sub-decimetre level. The created data products were used for quantifying gully and badland erosion in 2D and 3D as well as for the analysis of the surrounding areas and landscape development for larger extents.
Reduction of greenhouse gas (GHG) emissions to minimize climate change requires very significant societal effort. To motivate this effort, it is important to clarify the benefits of avoided emissions. To this end, we analysed the impact of four emissions scenarios on future renewable groundwater resources, which range from 1600 GtCO2 during the 21st century (RCP2.6) to 7300 GtCO2 (RCP8.5). Climate modelling uncertainty was taken into account by applying the bias-corrected output of a small ensemble of five CMIP5 global climate models (GCM) as provided by the ISI-MIP effort to the global hydrological model WaterGAP. Despite significant climate model uncertainty, the benefits of avoided emissions with respect to renewable groundwater resources (i.e. groundwater recharge (GWR)) are obvious. The percentage of projected global population (SSP2 population scenario) suffering from a significant decrease of GWR of more than 10% by the 2080s as compared to 1971–2000 decreases from 38% (GCM range 27–50%) for RCP8.5 to 24% (11–39%) for RCP2.6. The population fraction that is spared from any significant GWR change would increase from 29% to 47% if emissions were restricted to RCP2.6. Increases of GWR are more likely to occur in areas with below average population density, while GWR decreases of more than 30% affect especially (semi)arid regions, across all GCMs. Considering change of renewable groundwater resources as a function of mean global temperature (GMT) rise, the land area that is affected by GWR decreases of more than 30% and 70% increases linearly with global warming from 0 to 3 ° C. For each degree of GMT rise, an additional 4% of the global land area (except Greenland and Antarctica) is affected by a GWR decrease of more than 30%, and an additional 1% is affected by a decrease of more than 70%.
The 99th Annual Meeting of the Geologische Vereinigung (GV) and International Conference on Earth Control on Planetary Life and Environment, held in October 2009 at the Geosciences Centre of the Georg-August-Universität Göttingen, brings together researchers from all fields of Earth Sciences and beyond to shape an attractive interdisciplinary program on the geological history of Planet Earth and its control over and interaction with biological evolution, development of habitats, environmental and climate change as well as history and culture of Homo sapiens. This volume contains the abstracts of invited keynote lectures as well as all oral and poster presentations.
Environmental change impacts on the C- and N-cycle of European forests: a model comparison study
(2013)
Cameron, David R. ; Oijen, Marcel van ; Werner, Christian ; Butterbach-Bahl, Klaus ; Haas, Edwin ; Heuvelink, Gerardus Bernardus Maria ; Grote, Rüdiger ; Kiese, Ralf ; Kros, Johannes ; Kuhnert, Matthias ; Leip, Adrian ; Reinds, Gert Jan ; Reuter, Hannes Isaak ; Schelhaas, Mart Jan ; De Vries, Wim ; Yeluripati, Jagadeesh
Forests are important components of the greenhouse gas balance of Europe. There is considerable uncertainty about how predicted changes to climate and nitrogen deposition will perturb the carbon and nitrogen cycles of European forests and thereby alter forest growth, carbon sequestration and N2O emission. The present study aimed to quantify the carbon and nitrogen balance, including the exchange of greenhouse gases, of European forests over the period 2010–2030, with a particular emphasis on the spatial variability of change. The analysis was carried out for two tree species: European beech and Scots pine. For this purpose, four different dynamic models were used: BASFOR, DailyDayCent, INTEGRATOR and Landscape-DNDC. These models span a range from semi-empirical to complex mechanistic. Comparison of these models allowed assessment of the extent to which model predictions depended on differences in model inputs and structure. We found a European average carbon sink of 0.160 ± 0.020 kgC m−2 yr−1 (pine) and 0.138 ± 0.062 kgC m−2 yr−1 (beech) and N2O source of 0.285 ± 0.125 kgN ha−1 yr−1 (pine) and 0.575 ± 0.105 kgN ha−1 yr−1 (beech). The European average greenhouse gas potential of the carbon sink was 18 (pine) and 8 (beech) times that of the N2O source. Carbon sequestration was larger in the trees than in the soil. Carbon sequestration and forest growth were largest in central Europe and lowest in northern Sweden and Finland, N. Poland and S. Spain. No single driver was found to dominate change across Europe. Forests were found to be most sensitive to change in environmental drivers where the drivers were limiting growth, where changes were particularly large or where changes acted in concert. The models disagreed as to which environmental changes were most significant for the geographical variation in forest growth and as to which tree species showed the largest rate of carbon sequestration. Pine and beech forests were found to have differing sensitivities to environmental change, in particular the response to changes in nitrogen and precipitation, with beech forest more vulnerable to drought. There was considerable uncertainty about the geographical location of N2O emissions. Two of the models BASFOR and LandscapeDNDC had largest emissions in central Europe where nitrogen deposition and soil nitrogen were largest, whereas the two other models identified different regions with large N2O emission. N2O emissions were found to be larger from beech than pine forests and were found to be particularly sensitive to forest growth.
Cameron, David R. ; Oijen, Marcel van ; Werner, Christian ; Butterbach-Bahl, Klaus ; Haas, Edwin ; Heuvelink, Gerardus Bernardus Maria ; Grote, Rüdiger ; Kiese, Ralf ; Kuhnert, Matthias ; Kros, Johannes ; Leip, Adrian ; Reinds, Gert Jan ; Reuter, Hannes Isaak ; Schelhaas, Mart Jan ; De Vries, Wim ; Yeluripati, Jagadeesh
Forests are important components of the greenhouse gas balance of Europe. There is considerable uncertainty about how predicted changes to climate and nitrogen deposition will perturb the carbon and nitrogen cycles of European forests and thereby alter forest growth, carbon sequestration and N2O emission. The present study aimed to quantify the carbon and nitrogen balance, including the exchange of greenhouse gases, of European forests over the period 2010–2030, with a particular emphasis on the spatial variability of change. The analysis was carried out for two tree species: European beech and Scots pine. For this purpose, four different dynamic models were used: BASFOR, DailyDayCent, INTEGRATOR and Landscape-DNDC. These models span a range from semi-empirical to complex mechanistic. Comparison of these models allowed assessment of the extent to which model predictions depended on differences in model inputs and structure. We found a European average carbon sink of 0.160 ± 0.020 kgC m−2 yr−1 (pine) and 0.138 ± 0.062 kgC m−2 yr−1 (beech) and N2O source of 0.285 ± 0.125 kgN ha−1 yr−1 (pine) and 0.575 ± 0.105 kgN ha−1 yr−1 (beech). The European average greenhouse gas potential of the carbon source was 18 (pine) and 8 (beech) times that of the N2O source. Carbon sequestration was larger in the trees than in the soil. Carbon sequestration and forest growth were largest in central Europe and lowest in northern Sweden and Finland, N. Poland and S. Spain. No single driver was found to dominate change across Europe. Forests were found to be most sensitive to change in environmental drivers where the drivers were limiting growth, where changes were particularly large or where changes acted in concert. The models disagreed as to which environmental changes were most significant for the geographical variation in forest growth and as to which tree species showed the largest rate of carbon sequestration. Pine and beech forests were found to have differing sensitivities to environmental change, in particular the response to changes in nitrogen and precipitation, with beech forest more vulnerable to drought. There was considerable uncertainty about the geographical location of N2O emissions. Two of the models BASFOR and LandscapeDNDC had largest emissions in central Europe where nitrogen deposition and soil nitrogen were largest whereas the two other models identified different regions with large N2O emission. N2O emissions were found to be larger from beech than pine forests and were found to be particularly sensitive to forest growth.
Wimmer, Daniela ; Lehtipalo, Katrianne ; Franchin, Alessandro ; Kangasluoma, Juha ; Kreissl, Fabian ; Kürten, Christoph Andreas ; Kupc, Agnieszka ; Metzger, Axel ; Mikkilä, Jyri ; Petäjä, Tuukka ; Riccobono, Francesco ; Vanhanen, Joonas ; Kulmala, Markku ; Curtius, Joachim
When studying new particle formation, the uncertainty in determining the "true" nucleation rate is considerably reduced when using Condensation Particle Counters (CPCs) capable of measuring concentrations of aerosol particles at sizes close to or even at the critical cluster size (1–2 nm). Recently CPCs, able to reliably detect particles below 2 nm in size and even close to 1 nm became available. The corrections needed to calculate nucleation rates are substantially reduced compared to scaling the observed formation rate to the nucleation rate at the critical cluster size. However, this improved instrumentation requires a careful characterization of their cut-off size and the shape of the detection efficiency curve because relatively small shifts in the cut-off size can translate into larger relative errors when measuring particles close to the cut-off size.
Here we describe the development of two continuous flow CPCs using diethylene glycol (DEG) as the working fluid. The design is based on two TSI 3776 counters. Several sets of measurements to characterize their performance at different temperature settings were carried out. Furthermore two mixing-type Particle Size Magnifiers (PSM) A09 from Airmodus were characterized in parallel. One PSM was operated at the highest mixing ratio (1 L min−1 saturator flow), and the other was operated in a scanning mode, where the mixing ratios are changed periodically, resulting in a range of cut-off sizes. Different test aerosols were generated using a nano-Differential Mobility Analyzer (nano-DMA) or a high resolution DMA, to obtain detection efficiency curves for all four CPCs. One calibration setup included a high resolution mass spectrometer (APi-TOF) for the determination of the chemical composition of the generated clusters. The lowest cut-off sizes were achieved with negatively charged ammonium sulphate clusters, resulting in cut-offs of 1.4 nm for the laminar flow CPCs and 1.2 and 1.1 nm for the PSMs. A comparison of one of the laminar-flow CPCs and one of the PSMs measuring ambient and laboratory air showed good agreement between the instruments.
The SAWNUC microphysical aerosol nucleation model is used to study the effect of reactor walls on the interpretation of nucleation experiments with respect to nucleation theory. This work shows that loss processes, such as wall losses, influence the interpretation of nucleation experiments, especially at low growth rates and short lifetime of freshly nucleated particles. In these cases the power dependency of the formation rates, determined at a certain particle size, with respect to H2SO4 does not correspond to the approximate number of H2SO4 molecules in the critical cluster as expected by the first nucleation theorem. Observed ∂log(J)/∂log([H2SO4]) therefore can vary widely for identical nucleation conditions but different sink terms.
Tegtmeier, Susann ; Krüger, Kirstin ; Quack, Birgit ; Atlas, Elliot L. ; Blake, Donald R. ; Bönisch, Harald ; Engel, Andreas ; Hepach, Helmke ; Hossaini, Ryan ; Navarro, Maria A. ; Raimund, Stefan ; Sala, Stephan ; Shi, Qiang ; Ziska, Franziska
We investigate the contribution of oceanic methyl iodide (CH3I) to the stratospheric iodine budget. Based on CH3I measurements during three tropical ship campaigns and the Lagrangian transport model FLEXPART we provide a detailed analysis of CH3I transport from the ocean surface to the cold point in the upper tropical tropopause layer (TTL). While average oceanic emissions differ by less than 50% from campaign to campaign, the measurements show much stronger variations within each campaign. A positive correlation between the oceanic CH3I emissions and the efficiency of CH3I troposphere–stratosphere transport has been identified for some cruise sections. The mechanism of strong horizontal surface winds triggering large emissions on the one hand and being associated with tropical convective systems, such as developing typhoons, on the other hand, could explain the identified correlations. As a result of the simultaneous occurrence of large CH3I emissions and strong vertical uplift, localized maximum mixing ratios of 0.6 ppt CH3I at the cold point have been determined for observed peak emissions during the SHIVA-Sonne campaign in the coastal West Pacific. The other two campaigns give considerable smaller maxima of 0.1 ppt CH3I for the TransBrom campaign in the open West Pacific and 0.03 ppt for emissions from the coastal East Atlantic during the DRIVE campaign. In order to assess the representativeness of the large local mixing ratios we use climatological emission scenarios to derive global upper air estimates of CH3I abundances. The model results are compared to available upper air measurements including data from the recent ATTREX and HIPPO2 aircraft campaigns. In the East Pacific region, the location of the available measurement campaigns in the upper TTL, the comparisons give a good agreement indicating that around 0.01 to 0.02 ppt of CH3I enter the stratosphere. However, other tropical regions, which are subject to stronger convective activity show larger CH3I entrainment, e.g., 0.08 ppt in the West Pacific. The strong variations in the geographical distribution of CH3I entrainment suggest that currently available upper air measurements are not representative of global estimates and further campaigns will be necessary in order to better understand the CH3I contribution to stratospheric iodine.
Bradshaw, Catherine D. ; Lunt, Daniel J. ; Flecker, Rachel ; Salzmann, Ulrich ; Pound, Matthew J. ; Haywood, Alan M. ; Eronen, Jussi
In the original manuscript, Figs. 7–16 included fonts which were not correctly embedded in the file. As such, unless certain propriety software (ArcGIS) is installed on the viewing platform, the figures will appear corrupted. In this Corrigendum, Figs. 7–16 and their captions are reproduced with the fonts correctly embedded. Please find the correct figures below.
Bradshaw, Catherine D. ; Lunt, Daniel J. ; Flecker, Rachel ; Salzmann, Ulrich ; Pound, Matthew J. ; Haywood, Alan M. ; Eronen, Jussi
The late Miocene palaeorecord provides evidence for a warmer and wetter climate than that of today, and there is uncertainty in the palaeo-CO2 record of at least 200 ppm. We present results from fully coupled atmosphere-ocean-vegetation simulations for the late Miocene that examine the relative roles of palaeogeography (topography and ice sheet geometry) and CO2 concentration in the determination of late Miocene climate through comprehensive terrestrial model-data comparisons. Assuming that these data accurately reflect the late Miocene climate, and that the late Miocene palaeogeographic reconstruction used in the model is robust, then results indicate that:
1. Both palaeogeography and atmospheric CO2 contribute to the proxy-derived precipitation differences between the late Miocene and modern reference climates. However these contributions exibit synergy and so do not add linearly.
2. The vast majority of the proxy-derived temperature differences between the late Miocene and modern reference climates can only be accounted for if we assume a palaeo-CO2 concentration towards the higher end of the range of estimates.