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    Characterization of organic aerosol across the global remote troposphere: A comparison of ATom measurements and global chemistry models
    (Katlenburg-Lindau : EGU, 2020) Hodzic, Alma; Campuzano-Jost, Pedro; Bian, Huisheng; Chin, Mian; Colarco, Peter R.; Day, Douglas A.; Froyd, Karl D.; Heinold, Bernd; Katich, Joseph M.; Jo, Duseong S.; Kodros, John K.; Nault, Benjamin A.; Pierce, Jeffrey R.; Ray, Eric; Schacht, Jacob; Schill, Gregory P.; Schroder, Jason C.; Schwarz, Joshua P.; Sueper, Donna T.; Tegen, Ina; Tilmes, Simone; Tsigaridis, Kostas; Yu, Pengfei; Jimenez, Jose L.
    The spatial distribution and properties of submicron organic aerosol (OA) are among the key sources of uncertainty in our understanding of aerosol effects on climate. Uncertainties are particularly large over remote regions of the free troposphere and Southern Ocean, where very few data have been available and where OA predictions from AeroCom Phase II global models span 2 to 3 orders of magnitude, greatly exceeding the model spread over source regions. The (nearly) pole-to-pole vertical distribution of nonrefractory aerosols was measured with an aerosol mass spectrometer onboard the NASA DC-8 aircraft as part of the Atmospheric Tomography (ATom) mission during the Northern Hemisphere summer (August 2016) and winter (February 2017). This study presents the first extensive characterization of OA mass concentrations and their level of oxidation in the remote atmosphere. OA and sulfate are the major contributors by mass to submicron aerosols in the remote troposphere, together with sea salt in the marine boundary layer. Sulfate was dominant in the lower stratosphere. OA concentrations have a strong seasonal and zonal variability, with the highest levels measured in the lower troposphere in the summer and over the regions influenced by biomass burning from Africa (up to 10 μgsm-3). Lower concentrations (~ 0:1 0.3 μgsm-3) are observed in the northern middle and high latitudes and very low concentrations (< 0:1 μgsm-3) in the southern middle and high latitudes. The ATom dataset is used to evaluate predictions of eight current global chemistry models that implement a variety of commonly used representations of OA sources and chemistry, as well as of the AeroCom-II ensemble. The current model ensemble captures the average vertical and spatial distribution of measured OA concentrations, and the spread of the individual models remains within a factor of 5. These results are significantly improved over the AeroCom-II model ensemble, which shows large overestimations over these regions. However, some of the improved agreement with observations occurs for the wrong reasons, as models have the tendency to greatly overestimate the primary OA fraction and underestimate the sec-ondary fraction. Measured OA in the remote free troposphere is highly oxygenated, with organic aerosol to organic carbon (OA= OC) ratios of ~ 2.2 2.8, and is 30 % 60% more oxygenated than in current models, which can lead to significant errors in OA concentrations. The model measurement comparisons presented here support the concept of a more dynamic OA system as proposed by Hodzic et al. (2016), with enhanced removal of primary OA and a stronger production of secondary OA in global models needed to provide better agreement with observations. © 2020 IEEE Computer Society. All rights reserved.
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    Evaluation of wake influence on high-resolution balloon-sonde measurements
    (Göttingen : Copernicus GmbH, 2019) Söder, J.; Gerding, M.; Schneider, A.; Dörnbrack, A.; Wilms, H.; Wagner, J.; Lübken, F.-J.
    Balloons are used for various in situ measurements in the atmosphere. On turbulence measurements from rising balloons there is a potential for misinterpreting wake-created fluctuations in the trail of the balloon for atmospheric turbulence. These wake effects have an influence on temperature and humidity measurements from radiosondes as well. The primary aim of this study is to assess the likelihood for wake encounter on the payload below a rising balloon. Therefore, we present a tool for calculating this probability based on radiosonde wind data. This includes a retrieval of vertical winds from the radiosonde and an uncertainty analysis of the wake assessment. Our wake evaluation tool may be used for any balloon-gondola distance and provides a significant refinement compared to existing assessments. We have analysed wake effects for various balloon-gondola distances applying atmospheric background conditions from a set of 30 radiosondes. For a standard radiosonde we find an average probability for wake encounter of 28 %, pointing out the importance of estimating wake effects on sounding balloons. Furthermore, we find that even millimetre-sized objects in the payload can have significant effects on high-resolution turbulence measurements, if they are located upstream of the turbulence sensor. © Author(s) 2019. This work is distributed under.
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    Sensitivity of polar stratospheric ozone loss to uncertainties in chemical reaction kinetics
    (Göttingen : Copernicus GmbH, 2009) Kawa, S.R.; Stolarski, R.S.; Newman, P.A.; Douglass, A.R.; Rex, M.; Hofmann, D.J.; Santee, M.L.; Frieler, K.
    The impact and significance of uncertainties in model calculations of stratospheric ozone loss resulting from known uncertainty in chemical kinetics parameters is evaluated in trajectory chemistry simulations for the Antarctic and Arctic polar vortices. The uncertainty in modeled ozone loss is derived from Monte Carlo scenario simulations varying the kinetic (reaction and photolysis rate) parameters within their estimated uncertainty bounds. Simulations of a typical winter/spring Antarctic vortex scenario and Match scenarios in the Arctic produce large uncertainty in ozone loss rates and integrated seasonal loss. The simulations clearly indicate that the dominant source of model uncertainty in polar ozone loss is uncertainty in the Cl2O 2 photolysis reaction, which arises from uncertainty in laboratory-measured molecular cross sections at atmospherically important wavelengths. This estimated uncertainty in JCl 2O2 from laboratory measurements seriously hinders our ability to model polar ozone loss within useful quantitative error limits. Atmospheric observations, however, suggest that the Cl2O2 photolysis uncertainty may be less than that derived from the lab data. Comparisons to Match, South Pole ozonesonde, and Aura Microwave Limb Sounder (MLS) data all show that the nominal recommended rate simulations agree with data within uncertainties when the Cl2O2 photolysis error is reduced by a factor of two, in line with previous in situ ClOx measurements. Comparisons to simulations using recent cross sections from Pope et al. (2007) are outside the constrained error bounds in each case. Other reactions producing significant sensitivity in polar ozone loss include BrO + ClO and its branching ratios. These uncertainties challenge our confidence in modeling polar ozone depletion and projecting future changes in response to changing halogen emissions and climate. Further laboratory, theoretical, and possibly atmospheric studies are needed.
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    Development of a protocol for the auto-generation of explicit aqueous-phase oxidation schemes of organic compounds
    (Katlenburg-Lindau : EGU, 2019) Bräuer, Peter; Mouchel-Vallon, Camille; Tilgner, Andreas; Mutzel, Anke; Böge, Olaf; Rodigast, Maria; Poulain, Laurent; van Pinxteren, Dominik; Wolke, Ralf; Aumont, Bernard; Herrmann, Hartmut
    This paper presents a new CAPRAM-GECKOA protocol for mechanism auto-generation of aqueous-phase organic processes. For the development, kinetic data in the literature were reviewed and a database with 464 aqueousphase reactions of the hydroxyl radical with organic compounds and 130 nitrate radical reactions with organic compounds has been compiled and evaluated. Five different methods to predict aqueous-phase rate constants have been evaluated with the help of the kinetics database: gas-aqueous phase correlations, homologous series of various compound classes, radical reactivity comparisons, Evans-Polanyi-type correlations, and structure-activity relationships (SARs). The quality of these prediction methods was tested as well as their suitability for automated mechanism construction. Based on this evaluation, SARs form the basis of the new CAPRAM-GECKO-A protocol. Evans-Polanyi-type correlations have been advanced to consider all available H atoms in a molecule besides the H atoms with only the weakest bond dissociation enthalpies (BDEs). The improved Evans- Polanyi-type correlations are used to predict rate constants for aqueous-phase NO3 and organic compounds reactions. Extensive tests have been performed on essential parameters and on highly uncertain parameters with limited experimental data. These sensitivity studies led to further improvements in the new CAPRAM-GECKO-A protocol but also showed current limitations. Biggest uncertainties were observed in uptake processes and the estimation of Henry's law coefficients as well as radical chemistry, in particular the degradation of alkoxy radicals. Previous estimation methods showed several deficits, which impacted particle growth. For further evaluation, a 1,3,5-trimethylbenzene oxidation experiment has been performed in the aerosol chamber "Leipziger Aerosolkammer" (LEAK) at high relative humidity conditions and compared to a multiphase mechanism using the Master Chemical Mechanism (MCMv3.2) in the gas phase and using a methylglyoxal oxidation scheme of about 600 reactions generated with the new CAPRAM-GECKO-A protocol in the aqueous phase. While it was difficult to evaluate single particle constituents due to concentrations close to the detection limits of the instruments applied, the model studies showed the importance of aqueous-phase chemistry in respect to secondary organic aerosol (SOA) formation and particle growth. The new protocol forms the basis for further CAPRAM mechanism development towards a new version 4.0. Moreover, it can be used as a supplementary tool for aerosol chambers to design and analyse experiments of chemical complexity and help to understand them on a molecular level. © 2019 Author(s).
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    Projecting Antarctica's contribution to future sea level rise from basal ice shelf melt using linear response functions of 16 ice sheet models (LARMIP-2)
    (Göttingen : Copernicus Publ., 2020) Levermann, Anders; Winkelmann, Ricarda; Albrecht, Torsten; Goelzer, Heiko; Golledge, Nicholas R.; Greve, Ralf; Huybrechts, Philippe; Jordan, Jim; Leguy, Gunter; Martin, Daniel; Morlighem, Mathieu; Pattyn, Frank; Pollard, David; Quiquet, Aurelien; Rodehacke, Christian; Seroussi, Helene; Sutter, Johannes; Zhang, Tong; Van Breedam, Jonas; Calov, Reinhard; DeConto, Robert; Dumas, Christophe; Garbe, Julius; Gudmundsson, G. Hilmar; Hoffman, Matthew J.; Humbert, Angelika; Kleiner, Thomas; Lipscomb, William H.; Meinshausen, Malte; Ng, Esmond; Nowicki, Sophie M.J.; Perego, Mauro; Price, Stephen F.; Saito, Fuyuki; Schlegel, Nicole-Jeanne; Sun, Sainan; van de Wal, Roderik S.W.
    The sea level contribution of the Antarctic ice sheet constitutes a large uncertainty in future sea level projections. Here we apply a linear response theory approach to 16 state-of-the-art ice sheet models to estimate the Antarctic ice sheet contribution from basal ice shelf melting within the 21st century. The purpose of this computation is to estimate the uncertainty of Antarctica's future contribution to global sea level rise that arises from large uncertainty in the oceanic forcing and the associated ice shelf melting. Ice shelf melting is considered to be a major if not the largest perturbation of the ice sheet's flow into the ocean. However, by computing only the sea level contribution in response to ice shelf melting, our study is neglecting a number of processes such as surface-mass-balance-related contributions. In assuming linear response theory, we are able to capture complex temporal responses of the ice sheets, but we neglect any self-dampening or self-amplifying processes. This is particularly relevant in situations in which an instability is dominating the ice loss. The results obtained here are thus relevant, in particular wherever the ice loss is dominated by the forcing as opposed to an internal instability, for example in strong ocean warming scenarios. In order to allow for comparison the methodology was chosen to be exactly the same as in an earlier study (Levermann et al., 2014) but with 16 instead of 5 ice sheet models. We include uncertainty in the atmospheric warming response to carbon emissions (full range of CMIP5 climate model sensitivities), uncertainty in the oceanic transport to the Southern Ocean (obtained from the time-delayed and scaled oceanic subsurface warming in CMIP5 models in relation to the global mean surface warming), and the observed range of responses of basal ice shelf melting to oceanic warming outside the ice shelf cavity. This uncertainty in basal ice shelf melting is then convoluted with the linear response functions of each of the 16 ice sheet models to obtain the ice flow response to the individual global warming path. The model median for the observational period from 1992 to 2017 of the ice loss due to basal ice shelf melting is 10.2 mm, with a likely range between 5.2 and 21.3 mm. For the same period the Antarctic ice sheet lost mass equivalent to 7.4mm of global sea level rise, with a standard deviation of 3.7mm (Shepherd et al., 2018) including all processes, especially surface-mass-balance changes. For the unabated warming path, Representative Concentration Pathway 8.5 (RCP8.5), we obtain a median contribution of the Antarctic ice sheet to global mean sea level rise from basal ice shelf melting within the 21st century of 17 cm, with a likely range (66th percentile around the mean) between 9 and 36 cm and a very likely range (90th percentile around the mean) between 6 and 58 cm. For the RCP2.6 warming path, which will keep the global mean temperature below 2 °C of global warming and is thus consistent with the Paris Climate Agreement, the procedure yields a median of 13 cm of global mean sea level contribution. The likely range for the RCP2.6 scenario is between 7 and 24 cm, and the very likely range is between 4 and 37 cm. The structural uncertainties in the method do not allow for an interpretation of any higher uncertainty percentiles.We provide projections for the five Antarctic regions and for each model and each scenario separately. The rate of sea level contribution is highest under the RCP8.5 scenario. The maximum within the 21st century of the median value is 4 cm per decade, with a likely range between 2 and 9 cm per decade and a very likely range between 1 and 14 cm per decade. © Author(s) 2020.
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    Scaling of instability timescales of Antarctic outlet glaciers based on one-dimensional similitude analysis
    (Göttingen : Copernicus GmbH, 2019) Levermann, A.; Feldmann, J.
    Recent observations and ice-dynamic modeling suggest that a marine ice-sheet instability (MISI) might have been triggered in West Antarctica. The corresponding outlet glaciers, Pine Island Glacier (PIG) and Thwaites Glacier (TG), showed significant retreat during at least the last 2 decades. While other regions in Antarctica have the topographic predisposition for the same kind of instability, it is so far unclear how fast these instabilities would unfold if they were initiated. Here we employ the concept of similitude to estimate the characteristic timescales of several potentially MISI-prone outlet glaciers around the Antarctic coast. Our results suggest that TG and PIG have the fastest response time of all investigated outlets, with TG responding about 1.25 to 2 times as fast as PIG, while other outlets around Antarctica would be up to 10 times slower if destabilized. These results have to be viewed in light of the strong assumptions made in their derivation. These include the absence of ice-shelf buttressing, the one-dimensionality of the approach and the uncertainty of the available data. We argue however that the current topographic situation and the physical conditions of the MISI-prone outlet glaciers carry the information of their respective timescale and that this information can be partially extracted through a similitude analysis.
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    Understanding the uncertainty in global forest carbon turnover
    (Katlenburg-Lindau [u.a.] : Copernicus, 2020) Pugh, Thomas A.M.; Rademacher, Tim; Shafer, Sarah L.; Steinkamp, Jörg; Barichivich, Jonathan; Beckage, Brian; Haverd, Vanessa; Harper, Anna; Heinke, Jens; Nishina, Kazuya; Rammig, Anja; Sato, Hisashi; Arneth, Almut; Hantson, Stijn; Hickler, Thomas; Kautz, Markus; Quesada, Benjamin; Smith, Benjamin; Thonicke, Kirsten
    The length of time that carbon remains in forest biomass is one of the largest uncertainties in the global carbon cycle, with both recent historical baselines and future responses to environmental change poorly constrained by available observations. In the absence of large-scale observations, models used for global assessments tend to fall back on simplified assumptions of the turnover rates of biomass and soil carbon pools. In this study, the biomass carbon turnover times calculated by an ensemble of contemporary terrestrial biosphere models (TBMs) are analysed to assess their current capability to accurately estimate biomass carbon turnover times in forests and how these times are anticipated to change in the future. Modelled baseline 1985-2014 global average forest biomass turnover times vary from 12.2 to 23.5 years between TBMs. TBM differences in phenological processes, which control allocation to, and turnover rate of, leaves and fine roots, are as important as tree mortality with regard to explaining the variation in total turnover among TBMs. The different governing mechanisms exhibited by each TBM result in a wide range of plausible turnover time projections for the end of the century. Based on these simulations, it is not possible to draw robust conclusions regarding likely future changes in turnover time, and thus biomass change, for different regions. Both spatial and temporal uncertainty in turnover time are strongly linked to model assumptions concerning plant functional type distributions and their controls. Thirteen model-based hypotheses of controls on turnover time are identified, along with recommendations for pragmatic steps to test them using existing and novel observations. Efforts to resolve uncertainty in turnover time, and thus its impacts on the future evolution of biomass carbon stocks across the world's forests, will need to address both mortality and establishment components of forest demography, as well as allocation of carbon to woody versus non-woody biomass growth. © 2020 SPIE. All rights reserved.
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    Regional projections of temperature and precipitation changes: Robustness and uncertainty aspects
    (Stuttgart : Gebrueder Borntraeger Verlagsbuchhandlung, 2017) Piniewski, M.; Mezghani, A.; Szczésniak, M.; Kundzewicz, Z.W.
    This study presents the analysis of bias-corrected projections of changes in temperature and precipitation in the Vistula and Odra basins, covering approximately 90% of the Polish territory and small parts of neighbouring countries in Central and Eastern Europe. The ensemble of climate projections consists of nine regional climate model simulations from the EURO-CORDEX ensemble for two future periods 2021-2050 and 2071-2100, assuming two representative concentration pathways (RCPs) 4.5 and 8.5. The robustness is measured by the ensemble models' agreement on significant changes.We found a robust increase in the annual mean of daily minimum and maximum temperature, by 1-1.4 °C in the near future and by 1.9-3.8 °C in the far future (areal-means of the ensemble mean values). Higher increases are consistently associated with minimum temperature and the gradient of change goes from SWto NE regions. Seasonal projections of both temperature variables reflect lower robustness and suggest a higher future increase in winter temperatures than in other seasons, notably in the far future under RCP 8.5 (by more than 1 °C). However, changes in annual means of precipitation are uncertain and not robust in any of the analysed cases, even though the climate models agree well on the increase. This increase is intensified with rising global temperatures and varies from 5.5% in the near future under RCP 4.5 to 15.2%in the far future under RCP 8.5. Spatial variability is substantial, although quite variable between individual climate model simulations. Although seasonal means of precipitation are projected to considerably increase in all four combinations of RCPs and projection horizons for winter and spring, the high model spread reduces considerably the robustness, especially for the far future. In contrast, the ensemble members agree well that overall, the summer and autumn (with exception of the far future under RCP 8.5) precipitation will not undergo statistically significant changes.
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    Uncertainty of biomass contributions from agriculture and forestry to renewable energy resources under climate change
    (Stuttgart : Gebrueder Borntraeger Verlagsbuchhandlung, 2015) Gutsch, M.; Lasch-Born, P.; Lüttger, A.B.; Suckow, F.; Murawski, A.; Pilz, T.
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    Abrupt transitions in time series with uncertainties
    (London : Nature Publishing Group, 2018) Goswami, B.; Boers, N.; Rheinwalt, A.; Marwan, N.; Heitzig, J.; Breitenbach, S.F.M.; Kurths, J.
    Identifying abrupt transitions is a key question in various disciplines. Existing transition detection methods, however, do not rigorously account for time series uncertainties, often neglecting them altogether or assuming them to be independent and qualitatively similar. Here, we introduce a novel approach suited to handle uncertainties by representing the time series as a time-ordered sequence of probability density functions. We show how to detect abrupt transitions in such a sequence using the community structure of networks representing probabilities of recurrence. Using our approach, we detect transitions in global stock indices related to well-known periods of politico-economic volatility. We further uncover transitions in the El Niño-Southern Oscillation which coincide with periods of phase locking with the Pacific Decadal Oscillation. Finally, we provide for the first time an 'uncertainty-aware' framework which validates the hypothesis that ice-rafting events in the North Atlantic during the Holocene were synchronous with a weakened Asian summer monsoon.