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- ItemGeoengineering 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).
- ItemClimatic response to anthropogenic sulphate aerosols versus well-mixed greenhouse gases from 1850 to 2000 AD in CLIMBER-2(Abingdon : Taylor and Francis Ltd., 2008) Bauer, E.; Petoukhov, V.; Ganopolski, A.; Eliseev, A.V.The Earth system model CLIMBER-2 is extended by a scheme for calculating the climatic response to anthropogenic sulphur dioxide emissions. The scheme calculates the direct radiative forcing, the first indirect cloud albedo effect, and the second indirect cloud lifetime effect induced by geographically resolved sulphate aerosol burden. The simulated anthropogenic sulphate aerosol burden in the year 2000 amounts to 0.47 TgS. The best guesses for the radiative forcing due to the direct effect are -0.4 W m-2 and for the decrease in short-wave radiation due to all aerosol effects -0.8 W m-2. The simulated global warming by 1 K from 1850 to 2000 caused by anthropogenic greenhouse gases reduces to 0.6 K when the sulphate aerosol effects are included. The model's hydrological sensitivity of 4%/K is decreased by the second indirect effect to 0.8%/K. The quality of the geographically distributed climatic response to the historic emissions of sulphur dioxide and greenhouse gases makes the extended model relevant to computational efficient investigations of future climate change scenarios.
- ItemSpectral surface albedo over Morocco and its impact on radiative forcing of Saharan dust(Abingdon : Taylor & Francis, 2009) Bierwirth, E.; Wendisch, M.; Ehrlich, A.; Heese, B.; Tesche, M.; Althausen, D.; Schladitz, A.; Müller, D.; Otto, S.; Trautmann, T.; Dinter, T.; Von Hoyningen-Huene, W.; Kahn, R.In May-June 2006, airborne and ground-based solar (0.3-2.2 μm) and thermal infrared (4-42 μm) radiation measurements have been performed in Morocco within the Saharan Mineral Dust Experiment (SAMUM). Upwelling and downwelling solar irradiances have been measured using the Spectral Modular Airborne Radiation Measurement System (SMART)-Albedometer. With these data, the areal spectral surface albedo for typical surface types in southeastern Morocco was derived from airborne measurements for the first time. The results are compared to the surface albedo retrieved from collocated satellite measurements, and partly considerable deviations are observed. Using measured surface and atmospheric properties, the spectral and broad-band dust radiative forcing at top-of-atmosphere (TOA) and at the surface has been estimated. The impact of the surface albedo on the solar radiative forcing of Saharan dust is quantified. In the SAMUM case of 19 May 2006, TOA solar radiative forcing varies by 12 W m-2 per 0.1 surface-albedo change. For the thermal infrared component, values of up to +22 W m-2 were derived. The net (solar plus thermal infrared) TOA radiative forcing varies between -19 and +24 W m-2 for a broad-band solar surface albedo of 0.0 and 0.32, respectively. Over the bright surface of southeastern Morocco, the Saharan dust always has a net warming effect. © 2008 The Author Journal compilation © 2008 Blackwell Munksgaard.
- ItemCharging 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).
- ItemModelling soil dust aerosol in the Bodélé depression during the BoDEx campaign(München : European Geopyhsical Union, 2006) Tegen, I.; Heinold, B.; Todd, M.; Helmert, J.; Washington, R.; Dubovik, O.We present regional model simulations of the dust emission events during the Bodélé Dust Experiment (BoDEx) that was carried out in February and March 2005 in Chad. A box model version of the dust emission model is used to test different input parameters for the emission model, and to compare the dust emissions computed with observed wind speeds to those calculated with wind speeds from the regional model simulation. While field observations indicate that dust production occurs via self-abrasion of saltating diatomite flakes in the Bodélé, the emission model based on the assumption of dust production by saltation and using observed surface wind speeds as input parameters reproduces observed dust optical thicknesses well. Although the peak wind speeds in the regional model underestimate the highest wind speeds occurring on 10–12 March 2005, the spatio-temporal evolution of the dust cloud can be reasonably well reproduced by this model. Dust aerosol interacts with solar and thermal radiation in the regional model; it is responsible for a decrease in maximum daytime temperatures by about 5 K at the beginning the dust storm on 10 March 2005. This direct radiative effect of dust aerosol accounts for about half of the measured temperature decrease compared to conditions on 8 March. Results from a global dust model suggest that the dust from the Bodélé is an important contributor to dust crossing the African Savannah region towards the Gulf of Guinea and the equatorial Atlantic, where it can contribute up to 40% to the dust optical thickness.
- ItemCalibration of LACIS as a CCN detector and its use in measuring activation and hygroscopic growth of atmospheric aerosol particles(München : European Geopyhsical Union, 2006) Wex, H.; Kiselev, A.; Ziese, M.; Stratmann, F.A calibration for LACIS (Leipzig Aerosol Cloud Interaction Simulator) for its use as a CCN (cloud condensation nuclei) detector has been developed. For this purpose, sodium chloride and ammonium sulfate particles of known sizes were generated and their grown sizes were detected at the LACIS outlet. From these signals, the effective critical super-saturation was derived as a function of the LACIS wall temperature. With this, LACIS is calibrated for its use as a CCN detector. The applicability of LACIS for measurements of the droplet activation, and also of the hygroscopic growth of atmospheric aerosol particles was tested. The activation of the urban aerosol particles used in the measurements was found to occur at a critical super-saturation of 0.46% for particles with a dry diameter of 75 nm, and at 0.42% for 85 nm, respectively. Hygroscopic growth was measured for atmospheric aerosol particles with dry diameters of 150, 300 and 350 nm at relative humidities of 98 and 99%, and it was found that the larger dry particles contained a larger soluble volume fraction of about 0.85, compared to about 0.6 for the 150 nm particles.
- ItemColumnar modelling of nucleation burst evolution in the convective boundary layer - First results from a feasibility study, Part I: Modelling approach(München : European Geopyhsical Union, 2006) Hellmuth, O.A high-order modelling approach to interpret "continental-type" particle formation bursts in the anthropogenically influenced convective boundary layer (CBL) is proposed. The model considers third-order closure for planetary boundary layer turbulence, sulphur and ammonia chemistry as well as aerosol dynamics. In Paper I of four papers, previous observations of ultrafine particle evolution are reviewed, model equations are derived, the model setup for a conceptual study on binary and ternary homogeneous nucleation is defined and shortcomings of process parameterisation are discussed. In the subsequent Papers II, III and IV simulation results, obtained within the framework of a conceptual study on the CBL evolution and new particle formation (NPF), will be presented and compared with observational findings.
- ItemColumnar modelling of nucleation burst evolution in the convective boundary layer - First results from a feasibility study, Part IV: A compilation of previous observations for valuation of simulation results from a columnar modelling study(München : European Geopyhsical Union, 2006) Hellmuth, O.In the preceding Papers I, II and III a revised columnar high-order modelling approach to model gas-aerosol-turbulence interactions in the convective boundary layer (CBL) was proposed, and simulation results of two synthetic nucleation scenarios (binary vs. ternary) on new particle formation (NPF) in the anthropogenically influenced CBL were presented and discussed. The purpose of the present finishing Paper IV is twofold: Firstly, an attempt is made to compile previous observational findings on NPF bursts in the CBL, obtained from a number of field experiments. Secondly, the scenario simulations discussed in Paper III will be evaluated with respect to the role of CBL turbulence in NPF burst evolution. It was demonstrated, that completely different nucleation mechanisms can lead to the occurrence of NPF bursts in the surface layer, but the corresponding evolution patterns strongly differ with respect to the origin, amplitude and phase of the NPF burst as well as with respect to the time-height evolution of turbulent vertical fluxes and double correlation terms of physicochemical and aerosoldynamical variables. The large differences between the binary and ternary case scenario indicate, that ammonia (NH3) can not be considered as a time-independent tuning parameter in nucleation modelling. Its contribution to the evolution of the NPF burst pattern is much more complicated and reflects the influence of CBL turbulence as well as the strong non-linearity of the ternary nucleation rate. The impact of water (H2O) vapour on the nucleation rate is quite varying depending on the considered nucleation mechanism. According to the classical theory of binary nucleation involving H2O and sulphuric acid (H2SO4), H2O vapour favours NPF, according to the classical theory of ternary nuncleation involving H2O, H2SO4 and NH3 and according to organic nucleation via chemical reactions involving stabilised Criegee intermediates (SCIs), H2O vapour disfavours nucleation, and according to the parameterisation of the collision-controlled binary nucleation rate proposed by Weber et al. (1996), H2O vapour does not explicitly affect the particle formation. Since the H2SO4 concentration is overpredicted in the simulations presented in Paper III, the nucleation rates are too high compared to previous estimations. Therefore, the results are not directly comparable to measurements. Especially NPF events, where organics are suspected to play a key role, such as those observed at the boreal forest station in Hyytiälä (Southern Finland) or at Hohenpeissenberg (mountain site in Southern Germany), can not be explained by employing simple sulphur/ammonia chemistry. However, some valuable hints regarding the role of CBL turbulence in NPF can be obtained. In the literature a number of observations on the link between turbulence and NPF can be found, whose burst patterns support a strong contribution of CBL turbulence to the NPF burst evolution simulated here. Observations, that do not correspond to the scenarios are discussed with respect to possible reasons for the differences between model and observation. The model simulations support some state-of-the-art hypotheses on the contribution of CBL turbulence to NPF. Considering the application of box models, the present study shows, that CBL turbulence, not explicitly considered in such models, can strongly affect the spatio-temporal NPF burst evolution. The columnar high-order model presented here is a helpful tool to elucidate gas-aerosol-turbulence interactions, especially the genesis of NPF bursts in the CBL. An advanced description of the cluster formation and condensation growth is required as well as a comprehensive verification/validation study using observed high-order moments. Further scenario simulations remain to be performed.
- ItemColumnar modelling of nucleation burst evolution in the convective boundary layer - First results from a feasibility study, Part III: Preliminary results on physicochemical model performance using two "clean air mass" reference scenarios(München : European Geopyhsical Union, 2006) Hellmuth, O.In Paper I of four papers, a revised columnar high-order model to investigate gas-aerosol-turbulence interactions in the convective boundary layer (CBL) was proposed. In Paper II, the model capability to predict first-, second- and third-order moments of meteorological variables in the CBL was demonstrated using available observational data. In the present Paper III, the high-order modelling concept is extended to sulphur and ammonia chemistry as well as to aerosol dynamics. Based on the previous CBL simulation, a feasibility study is performed using two "clean air mass" scenarios with an emission source at the ground but low aerosol background concentration. Such scenarios synoptically correspond to the advection of fresh post-frontal air in an anthropogenically influenced region. The aim is to evaluate the time-height evolution of ultrafine condensation nuclei (UCNs) and to elucidate the interactions between meteorological and physicochemical variables in a CBL column. The scenarios differ in the treatment of new particle formation (NPF), whereas homogeneous nucleation according to the classical nucleation theory (CNT) is considered. The first scenario considers nucleation of a binary system consisting of water vapour and sulphuric acid (H2SO4) vapour, the second one nucleation of a ternary system additionally involving ammonia (NH3). Here, the two synthetic scenarios are discussed in detail, whereas special attention is payed to the role of turbulence in the formation of the typical UCN burst behaviour, that can often be observed in the surface layer. The intercomparison of the two scenarios reveals large differences in the evolution of the UCN number concentration in the surface layer as well as in the time-height cross-sections of first-order moments and double correlation terms. Although in both cases the occurrence of NPF bursts could be simulated, the burst characteristics and genesis of the bursts are completely different. It is demonstrated, that observations from the surface layer alone are not conclusive to elucidate the origin of newly formed particles. This is also true with respect to the interpretation of box modelling studies. The binary and ternary NPF bursts observed in the surface layer differ with respect to burst amplitude and phase. New particles simulated in the binary scenario are formed in the forenoon in the upper part of the growing CBL, followed by turbulence-induced top-down transport. Hence, with respect to the burst observation site in the surface layer, new particles are formed ex situ. In opposite to this, the ternary case reveals a much more complex pattern. Here, NPF is initiated in the early morning hours in the surface layer, when temperature (T) is low and relative humidity (RH), sulphur dioxide (SO2) and NH3 concentrations are high, hence new particles are formed in situ. Shortly after that, ex situ NPF in the free troposphere sets in, followed by entrainment and top-down diffusion of newly formed particles into the surface layer. Altogether, these processes mainly contribute to the formation of a strong burst in the morning hours in the ternary scenario. While the time-height cross-section of the binary nucleation rate resembles a "blob"-like evolution pattern, the ternary one resembles a "sucking tube"-like pattern. The time-height cross-sections of the flux pattern and double correlations could be plausibly interpreted in terms of CBL turbulence and entrainment/detrainment processes both in the binary and in the ternary case. Although the present approach is a pure conceptual one, it shows the feasibility to simulate gas-aerosol-turbulence interactions in the CBL. Prior to a dedicated verification/validation study, further attempts are necessary to consider a more advanced description of the formation and activation of thermodynamically stable clusters according to modern concepts proposed by Kulmala et al. (2000), Kulmala (2003) and Kulmala et al. (2004a).
- ItemSmall-scale mixing processes enhancing troposphere-to-stratosphere transport by pyro-cumulonimbus storms(Göttingen : Copernicus GmbH, 2007) Luderer, G.; Trentmann, J.; Hungershöfer, K.; Herzog, M.; Fromm, M.; Andreae, M.O.Deep convection induced by large forest fires is an efficient mechanism for transport of aerosol particles and trace gases into the upper troposphere and lower stratosphere (UT/LS). For many pyro-cumulonimbus clouds (pyroCbs) as well as other cases of severe convection without fire forcing, radiometric observations of cloud tops in the thermal infrared (IR) reveal characteristic structures, featuring a region of relatively high brightness temperatures (warm center) surrounded by a U-shaped region of low brightness temperatures. We performed a numerical simulation of a specific case study of pyroCb using a non-hydrostatic cloud resolving model with a two-moment cloud microphysics parameterization and a prognostic turbulence scheme. The model is able to reproduce the thermal IR structure as observed from satellite radiometry. Our findings establish a close link between the observed temperature pattern and small-scale mixing processes atop and downwind of the overshooting dome of the pyroCb. Such small-scale mixing processes are strongly enhanced by the formation and breaking of a stationary gravity wave induced by the overshoot. They are found to increase the stratospheric penetration of the smoke by up to almost 30 K and thus are of major significance for irreversible transport of forest fire smoke into the lower stratosphere.