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- ItemComplex refractive indices of Saharan dust samples at visible and near UV wavelengths: A laboratory study(München : European Geopyhsical Union, 2012) Wagner, R.; Ajtai, T.; Kandler, K.; Lieke, K.; Linke, C.; Müller, T.; Schnaiter, M.; Vragel, M.We have retrieved the wavelength-dependent imaginary parts of the complex refractive index for five different Saharan dust aerosol particles of variable mineralogical composition at wavelengths between 305 and 955 nm. The dust particles were generated by dispersing soil samples into a laboratory aerosol chamber, typically yielding particle sizes with mean diameters ranging from 0.3 to 0.4 μm and maximum diameters from 2 to 4 μm. The extinction and absorption coefficients as well as the number size distribution of the dust particles were simultaneously measured by various established techniques. An inversion scheme based on a spheroidal dust model was employed to deduce the refractive indices. The retrieved imaginary parts of the complex refractive index were in the range from 0.003 to 0.005, 0.005 to 0.011, and 0.016 to 0.050 at the wavelengths 955, 505, and 305 nm. The hematite content of the dust particles was determined by electron-microscopical single particle analysis. Hematite volume fractions in the range from 1.1 to 2.7% were found for the different dusts, a range typical for atmospheric mineral dust. We have performed a sensitivity study to assess how accurately the retrieved imaginary refractive indices could be reproduced by calculations with mixing rule approximations using the experimentally determined hematite contents as input.
- ItemNumerical simulations of mixing conditions and aerosol dynamics in the CERN CLOUD chamber(München : European Geopyhsical Union, 2012) Voigtländer, J.; Duplissy, J.; Rondo, L.; Kürten, A.; Stratmann, F.To study the effect of galactic cosmic rays on aerosols and clouds, the Cosmics Leaving OUtdoor Droplets (CLOUD) project was established. Experiments are carried out at a 26.1 m3 tank at CERN (Switzerland). In the experiments, the effect of ionizing radiation on H2SO4 particle formation and growth is investigated. To evaluate the experimental configuration, the experiment was simulated using a coupled multidimensional computational fluid dynamics (CFD) – particle model. In the model the coupled fields of gas/vapor species, temperature, flow velocity and particle properties were computed to investigate mixing state and mixing times of the CLOUD tank's contents. Simulation results show that a 1-fan configuration, as used in first experiments, may not be sufficient to ensure a homogeneously mixed chamber. To mix the tank properly, two fans and sufficiently high fan speeds are necessary. The 1/e response times for instantaneous changes of wall temperature and saturation ratio were found to be in the order of few minutes. Particle nucleation and growth was also simulated and particle number size distribution properties of the freshly nucleated particles (particle number, mean size, standard deviation of the assumed log-normal distribution) were found to be distributed over the tank's volume similar to the gas species.
- ItemCombining cloud radar and radar wind profiler for a value added estimate of vertical air motion and particle terminal velocity within clouds(Göttingen : Copernicus GmbH, 2018) Radenz, M.; Bühl, J.; Lehmann, V.; Görsdorf, U.; Leinweber, R.Vertical-stare observations from a 482MHz radar wind profiler and a 35GHz cloud radar are combined on the level of individual Doppler spectra to measure vertical air motions in clear air, clouds and precipitation. For this purpose, a separation algorithm is proposed to remove the influence of falling particles from the wind profiler Doppler spectra and to calculate the terminal fall velocity of hydrometeors. The remaining error of both vertical air motion and terminal fall velocity is estimated to be better than 0.1ms-1 using numerical simulations. This combination of instruments allows direct measurements of in-cloud vertical air velocity and particle terminal fall velocity by means of ground-based remote sensing. The possibility of providing a profile every 10s with a height resolution of < 100m allows further insight into the process scale of in-cloud dynamics. The results of the separation algorithm are illustrated by two case studies, the first covering a deep frontal cloud and the second featuring a shallow mixed-phase cloud.
- 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.
- ItemA parameterization of the heterogeneous hydrolysis of N2O5 for mass-based aerosol models: Improvement of particulate nitrate prediction(Katlenburg-Lindau : EGU, 2018) Chen, Ying; Wolke, Ralf; Ran, Liang; Birmili, Wolfram; Spindler, Gerald; Schröder, Wolfram; Su, Hang; Cheng, Yafang; Tegen, Ina; Wiedensohler, AlfredThe heterogeneous hydrolysis of N2O5 on the surface of deliquescent aerosol leads to HNO3 formation and acts as a major sink of NOx in the atmosphere during night-time. The reaction constant of this heterogeneous hydrolysis is determined by temperature (T), relative humidity (RH), aerosol particle composition, and the surface area concentration (S). However, these parameters were not comprehensively considered in the parameterization of the heterogeneous hydrolysis of N2O5 in previous mass-based 3-D aerosol modelling studies. In this investigation, we propose a sophisticated parameterization (NewN2O5) of N2O5 heterogeneous hydrolysis with respect to T, RH, aerosol particle compositions, and S based on laboratory experiments. We evaluated closure between NewN2O5 and a state-of-the-art parameterization based on a sectional aerosol treatment. The comparison showed a good linear relationship (R Combining double low line 0.91) between these two parameterizations. NewN2O5 was incorporated into a 3-D fully online coupled model, COSMO-Muscat, with the mass-based aerosol treatment. As a case study, we used the data from the HOPE Melpitz campaign (10-25 September 2013) to validate model performance. Here, we investigated the improvement of nitrate prediction over western and central Europe. The modelled particulate nitrate mass concentrations ([NO3-]) were validated by filter measurements over Germany (Neuglobsow, Schmücke, Zingst, and Melpitz). The modelled [NO3-] was significantly overestimated for this period by a factor of 5-19, with the corrected NH3 emissions (reduced by 50 %) and the original parameterization of N2O5 heterogeneous hydrolysis. The NewN2O5 significantly reduces the overestimation of [NO3-] by ∼ 35 %. Particularly, the overestimation factor was reduced to approximately 1.4 in our case study (12, 17-18 and 25 September 2013) when [NO3-] was dominated by local chemical formations. In our case, the suppression of organic coating was negligible over western and central Europe, with an influence on [NO3-] of less than 2 % on average and 20 % at the most significant moment. To obtain a significant impact of the organic coating effect, N2O5, SOA, and NH3 need to be present when RH is high and T is low. However, those conditions were rarely fulfilled simultaneously over western and central Europe. Hence, the organic coating effect on the reaction probability of N2O5 may not be as significant as expected over western and central Europe.
- ItemModeling of wave-induced irradiance variability in the upper ocean mixed layer(München : European Geopyhsical Union, 2012) Hieronymi, M.; Macke, A.; Zielinski, O.A Monte Carlo based radiative transfer model has been developed for calculating the availability of solar radiation within the top 100 m of the ocean. The model is optimized for simulations of spatial high resolution downwelling irradiance Ed fluctuations that arise from the lensing effect of waves at the water surface. In a first step the accuracy of simulation results has been verified by measurements of the oceanic underwater light field and through intercomparison with an established radiative transfer model. Secondly the potential depth-impact of nonlinear shaped single waves, from capillary to swell waves, is assessed by considering the most favorable conditions for light focusing, i.e. monochromatic light at 490 nm, very clear oceanic water with a low chlorophyll a content of 0.1 mg m−3 and high sun elevation. Finally light fields below irregular wave profiles accounting for realistic sea states were simulated. Our simulation results suggest that under open ocean conditions light flashes with 50% irradiance enhancements can appear down to 35 m depth, and light variability in the range of ±10% compared to the mean Ed is still possible in 100 m depth.
- ItemImpact of water uptake and mixing state on submicron particle deposition in the human respiratory tract (HRT) based on explicit hygroscopicity measurements at HRT-like conditions(Katlenburg-Lindau : EGU, 2022) Man, Ruiqi; Wu, Zhijun; Zong, Taomou; Voliotis, Aristeidis; Qiu, Yanting; Größ, Johannes; van Pinxteren, Dominik; Zeng, Limin; Herrmann, Hartmut; Wiedensohler, Alfred; Hu, MinParticle hygroscopicity plays a key role in determining the particle deposition in the human respiratory tract (HRT). In this study, the effects of hygroscopicity and mixing state on regional and total deposition doses on the basis of the particle number concentration for children, adults, and the elderly were quantified using the Multiple-Path Particle Dosimetry model, based on the size-resolved particle hygroscopicity measurements at HRT-like conditions (relative humidity = 98 %) performed in the North China Plain. The measured particle population with an external mixing state was dominated by hygroscopic particles (number fraction = (91.5 ± 5.7) %, mean ± standard deviation (SD); the same below). Particle hygroscopic growth in the HRT led to a reduction by around 24 % in the total doses of submicron particles for all age groups. Such a reduction was mainly caused by the growth of hygroscopic particles and was more pronounced in the pulmonary and tracheobronchial regions. Regardless of hygroscopicity, the elderly group of people had the highest total dose among three age groups, while children received the maximum total deposition rate. With 270 nm in diameter as the boundary, the total deposition doses of particles smaller than this diameter were overestimated, and those of larger particles were underestimated, assuming no particle hygroscopic growth in the HRT. From the perspective of the daily variation, the deposition rates of hygroscopic particles with an average of (2.88 ± 0.81) × 109 particles h-1 during the daytime were larger than those at night ((2.32 ± 0.24) × 109 particles h-1). On the contrary, hydrophobic particles interpreted as freshly emitted soot and primary organic aerosols exhibited higher deposition rates at nighttime ((3.39 ± 1.34) × 108 particles h-1) than those in the day ((2.58 ± 0.76) × 108 particles h-1). The traffic emissions during the rush hours enhanced the deposition rate of hydrophobic particles. This work provides a more explicit assessment of the impact of hygroscopicity and mixing state on the deposition pattern of submicron particles in the HRT. Copyright:
- ItemEvaluation of long-range transport and deposition of desert dust with the CTM MOCAGE(Milton Park : Taylor & Francis, 2017) Martet, M.; Peuch, V-H.; Laurent, B.; Marticorena, B.; Bergametti, G.Desert dust modelling and forecasting attract growing interest, due to the numerous impacts of dusts on climate, numerical weather prediction, health, ecosystems, transportation, as well as on many industrial activities. The validation of numerical tools is a very important activity in this context, and we present here an example of such an effort, combining in situ (horizontal visibility in SYNOP messages, IMPROVE database) and remote-sensing data (satellite imagery, AERONET aerosol optical thickness data). Interestingly, these measurements are available routinely, and not only in the context of dedicated measurements campaign; thus, they can be used in an operational context to monitor the performances of operational forecasting systems. MOCAGE is the chemistry-transport model of Météo-France, used operationally to forecast the three-dimensional transport of dusts and their deposition. Two very long-range transport episodes of dust have been studied: one case of Saharan dust transported to East America through Asia and Pacific observed in November 2004 and one case of Saharan dust transported from West Africa to Caribbean Islands in May 2007. Episodes of geographical extension had seldom been studied, and they provide a very selective reference to compare the modelled desert dusts with. The representation of dusts in MOCAGE appears to be realistic in these two very different cases. In turn, the model simulations are used to make the link between the complementary information provided by the different measurements tools, providing a fully consistent picture of the entire episodes. The evolution of the aerosol size distribution during the episodes has also been studied. With no surprise, our study underlines that deposition processes are very sensitive to the size of dust particles. If the atmospheric cycle, in terms of mass, is very much under the influence of larger particles (some micrometres and above), only the finer particles actually travel over thousands of kilometres. This illustrates the need for an accurate representation of size distributions for this aerosol component in numerical models and advocates for using a size-resolved (bin) approach as sinks, and particularly, deposition do not affect the emitted log-normal distributions symmetrically on both sides of the median diameter. Overall, the results presented in this study provide an evaluation of Météo-France operational dust forecasting system MOCAGE.
- ItemHomogeneous and heterogeneous ice nucleation at LACIS: Operating principle and theoretical studies(München : European Geopyhsical Union, 2011) Hartmann, S.; Niedermeier, D.; Voigtländer, J.; Clauss, T.; Shaw, R.A.; Wex, H.; Kiselev, A.; Stratmann, F.At the Leipzig Aerosol Cloud Interaction Simulator (LACIS) experiments investigating homogeneous and heterogeneous nucleation of ice (particularly immersion freezing in the latter case) have been carried out. Here both the physical LACIS setup and the numerical model developed to design experiments at LACIS and interpret their results are presented in detail. Combining results from the numerical model with experimental data, it was found that for the experimental parameter space considered, classical homogeneous ice nucleation theory is able to predict the freezing behavior of highly diluted ammonium sulfate solution droplets, while classical heterogeneous ice nucleation theory, together with the assumption of a constant contact angle, fails to predict the immersion freezing behavior of surrogate mineral dust particles (Arizona Test Dust, ATD). The main reason for this failure is the compared to experimental data apparently overly strong temperature dependence of the nucleation rate coefficient. Assuming, in the numerical model, Classical Nucleation Theory (CNT) for homogeneous ice nucleation and a CNT-based parameterization for the nucleation rate coefficient in the immersion freezing mode, recently published by our group, it was found that even for a relatively effective ice nucleating agent such as pure ATD, there is a temperature range where homogeneous ice nucleation is dominant. The main explanation is the apparently different temperature dependencies of the two freezing mechanisms. Finally, reviewing the assumptions made during the derivation of the CNT-based parameterization for immersion freezing, it was found that the assumption of constant temperature during ice nucleation and the chosen ice nucleation time were justified, underlining the applicability of the method to determine the fitting coefficients in the parameterization equation.
- ItemCharacterization 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.