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    Charging of mesospheric aerosol particles: The role of photodetachment and photoionization from meteoric smoke and ice particles
    (Göttingen : Copernicus, 2009) Rapp, M.
    Time constants for photodetachment, photoemission, and electron capture are considered for two classes of mesospheric aerosol particles, i.e., meteor smoke particles (MSPs) and pure water ice particles. Assuming that MSPs consist of metal oxides like Fe2O3 or SiO, we find that during daytime conditions photodetachment by solar photons is up to 4 orders of magnitude faster than electron attachment such that MSPs cannot be negatively charged in the presence of sunlight. Rather, even photoemission can compete with electron capture unless the electron density becomes very large (≫1000 cm-3) such that MSPs should either be positively charged or neutral in the case of large electron densities. For pure water ice particles, however, both photodetachment and photoemission are negligible due to the wavelength characteristics of its absorption cross section and because the flux of solar photons has already dropped significantly at such short wavelengths. This means that water ice particles should normally be negatively charged. Hence, our results can readily explain the repeated observation of the coexistence of positive and negative aerosol particles in the polar summer mesopause, i.e., small MSPs should be positively charged and ice particles should be negatively charged. These results have further important implications for our understanding of the nucleation of mesospheric ice particles as well as for the interpretation of incoherent scatter radar observations of MSPs. © 2009 Author(s).
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    Long-term behavior of the concentration of the minor constituents in the mesosphere-a model study
    (Göttingen : Copernicus, 2009) Grygalashvyly, M.; Sonnemann, G.R.; Hartogh, P.
    We investigate the influence the rising concentrations of methane, nitrous oxide and carbon dioxide which have occurred since the pre-industrial era, have had on the chemistry of the mesosphere. For this investigation we use our global 3-D-model COMMA-IAP which was designed for the exploration of the MLT-region and in particular the extended mesopause region. Assumptions and approximations for the trends in the Lyman-flux (needed for the water vapor dissociation rate), methane and the water vapor mixing ratio at the hygropause are necessary to accomplish this study. To approximate the solar Lyman-α flux back to the pre-industrial time, we derived a quadratic fit using the sunspot number record which extends back to 1749 and is the only solar proxy available for the Lyman-α flux prior to 1947. We assume that methane increases with a constant growth rate from the pre-industrial era to the present. An unsolved problem for the model calculations consists of how the water vapor mixing ratio at the hygropause should be specified during this period. We assume that the hygropause was dryer during pre-industrial times than the present. As a consequence of methane oxidation, the model simulation indicates that the middle atmosphere has become more humid as a result of the rising methane concentration, but with some dependence on height and with a small time delay of few years. The solar influence on the water vapor mixing ratio is insignificant below about 80 km in summer high latitudes, but becomes increasingly more important above this altitude. The enhanced water vapor concentration increasesthe hydrogen radical concentration and reduces the mesospheric ozone. A second region of stronger ozone decrease is located in the vicinity of the stratopause. Increases in CO2 concentration enhance slightly the concentration of CO in the mesosphere. However, its influence upon the chemistry is small and its main effect is connected with a cooling of the upper atmosphere. The long-term behavior of water vapor is discussed in particular with respect to its impact on the NLC region.
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    Towards global empirical upscaling of FLUXNET eddy covariance observations: Validation of a model tree ensemble approach using a biosphere model
    (München : European Geopyhsical Union, 2009) Jung, M.; Reichstein, M.; Bondeau, A.
    Global, spatially and temporally explicit estimates of carbon and water fluxes derived from empirical up-scaling eddy covariance measurements would constitute a new and possibly powerful data stream to study the variability of the global terrestrial carbon and water cycle. This paper introduces and validates a machine learning approach dedicated to the upscaling of observations from the current global network of eddy covariance towers (FLUXNET). We present a new model TRee Induction ALgorithm (TRIAL) that performs hierarchical stratification of the data set into units where particular multiple regressions for a target variable hold. We propose an ensemble approach (Evolving tRees with RandOm gRowth, ERROR) where the base learning algorithm is perturbed in order to gain a diverse sequence of different model trees which evolves over time. We evaluate the efficiency of the model tree ensemble (MTE) approach using an artificial data set derived from the Lund-Potsdam-Jena managed Land (LPJmL) biosphere model. We aim at reproducing global monthly gross primary production as simulated by LPJmL from 1998–2005 using only locations and months where high quality FLUXNET data exist for the training of the model trees. The model trees are trained with the LPJmL land cover and meteorological input data, climate data, and the fraction of absorbed photosynthetic active radiation simulated by LPJmL. Given that we know the "true result" in the form of global LPJmL simulations we can effectively study the performance of the MTE upscaling and associated problems of extrapolation capacity. We show that MTE is able to explain 92% of the variability of the global LPJmL GPP simulations. The mean spatial pattern and the seasonal variability of GPP that constitute the largest sources of variance are very well reproduced (96% and 94% of variance explained respectively) while the monthly interannual anomalies which occupy much less variance are less well matched (41% of variance explained). We demonstrate the substantially improved accuracy of MTE over individual model trees in particular for the monthly anomalies and for situations of extrapolation. We estimate that roughly one fifth of the domain is subject to extrapolation while MTE is still able to reproduce 73% of the LPJmL GPP variability here. This paper presents for the first time a benchmark for a global FLUXNET upscaling approach that will be employed in future studies. Although the real world FLUXNET upscaling is more complicated than for a noise free and reduced complexity biosphere model as presented here, our results show that an empirical upscaling from the current FLUXNET network with MTE is feasible and able to extract global patterns of carbon flux variability.
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    Estimating carbon emissions from African wildfires
    (München : European Geopyhsical Union, 2009) Lehsten, V.; Tansey, K.; Balzter, H.; Thonicke, K.; Spessa, A.; Weber, U.; Smith, B.; Arneth, A.
    We developed a technique for studying seasonal and interannual variation in pyrogenic carbon emissions from Africa using a modelling approach that scales burned area estimates from L3JRC, a map recently generated from remote sensing of burn scars instead of active fires. Carbon fluxes were calculated by the novel fire model SPITFIRE embedded within the dynamic vegetation model framework LPJ-GUESS, using daily climate input. For the time period from 2001 to 2005 an average area of 195.5±24×104 km2 was burned annually, releasing an average of 723±70 Tg C to the atmosphere; these estimates for the biomass burned are within the range of previously published estimates. Despite the fact that the majority of wildfires are ignited by humans, strong relationships between climatic conditions (particularly precipitation), net primary productivity and overall biomass burnt emerged. Our investigation of the relationships between burnt area and carbon emissions and their potential drivers available litter and precipitation revealed uni-modal responses to annual precipitation, with a maximum around 1000 mm for burned area and emissions, or 1200 mm for litter availability. Similar response patterns identified in savannahs worldwide point to precipitation as a chief determinant for short-term variation in fire regime. A considerable variability that cannot be explained by fire-precipitation relationships alone indicates the existence of additional factors that must be taken into account.
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    Design and performance of an automatic regenerating adsorption aerosol dryer for continuous operation at monitoring sites
    (München : European Geopyhsical Union, 2009) Tuch, T.M.; Haudek, A.; Müller, T.; Nowak, A.; Wex, H.; Wiedensohler, A.
    Sizes of aerosol particles depend on the relative humidity of their carrier gas. Most monitoring networks require therefore that the aerosol is dried to a relative humidity below 50% r.H. to ensure comparability of measurements at different sites. Commercially available aerosol dryers are often not suitable for this purpose at remote monitoring sites. Adsorption dryers need to be regenerated frequently and maintenance-free single column Nafion dryers are not designed for high aerosol flow rates. We therefore developed an automatic regenerating adsorption aerosol dryer with a design flow rate of 1 m3/h. Particle transmission efficiency of this dryer has been determined during a 3 week experiment. The lower 50% cut-off was found to be smaller than 3 nm at the design flow rate of the instrument. Measured transmission efficiencies are in good agreement with theoretical calculations. One dryer has been successfully deployed in the Amazon river basin. We present data from this monitoring site for the first 6 months of measurements (February 2008–August 2008). Apart from one unscheduled service, this dryer did not require any maintenance during this time period. The average relative humidity of the dried aerosol was 27.1+/−7.5% r.H. compared to an average ambient relative humidity of nearly 80% and temperatures around 30°C. This initial deployment demonstrated that these dryers are well suitable for continuous operation at remote monitoring sites under adverse ambient conditions.
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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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    Saharan dust transport and deposition towards the tropicalnorthern Atlantic
    (Göttingen : Copernicus, 2009) Schepanski, K.; Tegen, I.; MacKe, A.
    We present a study of Saharan dust export towards the tropical North Atlantic using the regional dust emission, transport and deposition model LM-MUSCAT. Horizontal and vertical distribution of dust optical thickness, concentration, and dry and wet deposition rates are used to describe seasonality of dust export and deposition towards the eastern Atlantic for three typical months in different seasons. Deposition rates strongly depend on the vertical dust distribution, which differs with seasons. Furthermore the contribution of dust originating from the Bod́eĺe Depression to Saharan dust over the Atlantic is investigated. A maximum contribution of Bod́eĺe dust transported towards the Cape Verde Islands is evident in winter when the Bod́eĺe source area is most active and dominant with regard to activation frequency and dust emission. Limitations of using satellite retrievals to estimate dust deposition are highlighted.
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    Planetary geostrophic equations for the atmosphere with evolution of the barotropic flow
    (Amsterdam : Elsevier, 2009) Dolaptchiev, S.I.; Klein, R.
    Atmospheric phenomena such as the quasi-stationary Rossby waves, teleconnection patterns, ultralong persistent blockings and the polar/subtropical jet are characterized by planetary spatial scales, i.e. scales of the order of the earth's radius. This motivates our interest in the relevant physical processes acting on the planetary scales. Using an asymptotic approach, we systematically derive reduced model equations valid for atmospheric motions with planetary spatial scales and a temporal scale of the order of about 1 week. We assume variations of the background potential temperature comparable in magnitude with those adopted in the classical quasi-geostrophic theory. At leading order, the resulting equations include the planetary geostrophic balance. In order to apply these equations to the atmosphere, one has to prescribe a closure for the vertically averaged pressure. We present an evolution equation for this component of the pressure which was derived in a systematic way from the asymptotic analysis. Relative to the prognostic closures adopted in existing reduced-complexity planetary models, this new dynamical closure may provide for more realistic increased large-scale, long-time variability in future implementations. © 2008 Elsevier B.V. All rights reserved.
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    Geoengineering climate by stratospheric sulfur injections: Earth system vulnerability to technological failure
    (Dordrecht [u.a.] : Springer, 2009) Brovkin, V.; Petoukhov, V.; Claussen, M.; Bauer, E.; Archer, D.; Jaeger, C.
    We use a coupled climate-carbon cycle model of intermediate complexity to investigate scenarios of stratospheric sulfur injections as a measure to compensate for CO2-induced global warming. The baseline scenario includes the burning of 5,000 GtC of fossil fuels. A full compensation of CO2-induced warming requires a load of about 13 MtS in the stratosphere at the peak of atmospheric CO2 concentration. Keeping global warming below 2°C reduces this load to 9 MtS. Compensation of CO 2 forcing by stratospheric aerosols leads to a global reduction in precipitation, warmer winters in the high northern latitudes and cooler summers over northern hemisphere landmasses. The average surface ocean pH decreases by 0.7, reducing the calcifying ability of marine organisms. Because of the millennial persistence of the fossil fuel CO2 in the atmosphere, high levels of stratospheric aerosol loading would have to continue for thousands of years until CO2 was removed from the atmosphere. A termination of stratospheric aerosol loading results in abrupt global warming of up to 5°C within several decades, a vulnerability of the Earth system to technological failure. © 2008 The Author(s).
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    Origin of aerosol particles in the mid-latitude and subtropical upper troposphere and lowermost stratosphere from cluster analysis of CARIBIC data
    (München : European Geopyhsical Union, 2009) Köppe, M.; Hermann, M.; Brenninkmeijer, C.A.M.; Heintzenberg, J.; Schlager, H.; Schuck, T.; Slemr, F.; Sprung, D.; van Velthoven, P.F.J.; Wiedensohler, A.; Zahn, A.; Ziereis, H.
    The origin of aerosol particles in the upper troposphere and lowermost stratosphere over the Eurasian continent was investigated by applying cluster analysis methods to in situ measured data. Number concentrations of submicrometer aerosol particles and trace gas mixing ratios derived by the CARIBIC (Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container) measurement system on flights between Germany and South-East Asia were used for this analysis. Four cluster analysis methods were applied to a test data set and their capability of separating the data points into scientifically reasonable clusters was assessed. The best method was applied to seasonal data subsets for summer and winter resulting in five cluster or air mass types: stratosphere, tropopause, free troposphere, high clouds, and boundary layer influenced. Other source clusters, like aircraft emissions could not be resolved in the present data set with the used methods. While the cluster separation works satisfactory well for the summer data, in winter interpretation is more difficult, which is attributed to either different vertical transport pathways or different chemical lifetimes in both seasons. The geographical distribution of the clusters together with histograms for nucleation and Aitken mode particles within each cluster are presented. Aitken mode particle number concentrations show a clear vertical gradient with the lowest values in the lowermost stratosphere (750–2820 particles/cm3 STP, minimum of the two 25% – and maximum of the two 75%-percentiles of both seasons) and the highest values for the boundary-layer-influenced air (4290–22 760 particles/cm3 STP). Nucleation mode particles are also highest in the boundary-layer-influenced air (1260–29 500 particles/cm3 STP), but are lowest in the free troposphere (0–450 particles/cm3 STP). The given submicrometer particle number concentrations represent the first large-scale seasonal data sets for the upper troposphere and lowermost stratosphere over the Eurasian continent.