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- ItemSurface modification of mineral dust particles by sulphuric acid processing: Implications for ice nucleation abilities(München : European Geopyhsical Union, 2011) Reitz, P.; Spindler, C.; Mentel, T.F.; Poulain, L.; Wex, H.; Mildenberger, K.; Niedermeier, D.; Hartmann, S.; Clauss, T.; Stratmann, F.; Sullivan, R.C.; DeMott, P.J.; Petters, M.D.; Sierau, B.; Schneider, J.The ability of coated mineral dust particles to act as ice nuclei (IN) was investigated at LACIS (Leipzig Aerosol Cloud Interaction Simulator) during the FROST1- and FROST2-campaigns (Freezing of dust). Sulphuric acid was condensed on the particles which afterwards were optionally humidified, treated with ammonia vapour and/or heat. By means of aerosol mass spectrometry we found evidence that processing of mineral dust particles with sulphuric acid leads to surface modifications of the particles. These surface modifications are most likely responsible for the observed reduction of the IN activation of the particles. The observed particle mass spectra suggest that different treatments lead to different chemical reactions on the particle surface. Possible chemical reaction pathways and products are suggested and the implications on the IN efficiency of the treated dust particles are discussed.
- ItemChemistry of new particle growth in mixed urban and biogenic emissions - Insights from CARES(München : European Geopyhsical Union, 2014) Setyan, A.; Song, C.; Merkel, M.; Knighton, W.B.; Onasch, T.B.; Canagaratna, M.R.; Worsnop, D.R.; Wiedensohler, A.; Shilling, J.E.; Zhang, Q.Regional new particle formation and growth events (NPEs) were observed on most days over the Sacramento and western Sierra foothills area of California in June 2010 during the Carbonaceous Aerosols and Radiative Effect Study (CARES). Simultaneous particle measurements at both the T0 (Sacramento, urban site) and the T1 (Cool, rural site located ~40 km northeast of Sacramento) sites of CARES indicate that the NPEs usually occurred in the morning with the appearance of an ultrafine mode at ~15 nm (in mobility diameter, Dm, measured by a mobility particle size spectrometer operating in the range 10-858 nm) followed by the growth of this modal diameter to ~50 nm in the afternoon. These events were generally associated with southwesterly winds bringing urban plumes from Sacramento to the T1 site. The growth rate was on average higher at T0 (7.1 ± 2.7 nm h−1) than at T1 (6.2 ± 2.5 nm h−1), likely due to stronger anthropogenic influences at T0. Using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), we investigated the evolution of the size-resolved chemical composition of new particles at T1. Our results indicate that the growth of new particles was driven primarily by the condensation of oxygenated organic species and, to a lesser extent, ammonium sulfate. New particles appear to be fully neutralized during growth, consistent with high NH3 concentration in the region. Nitrogen-containing organic ions (i.e., CHN+, CH4N+, C2H3N+, and C2H4N+) that are indicative of the presence of alkyl-amine species in submicrometer particles enhanced significantly during the NPE days, suggesting that amines might have played a role in these events. Our results also indicate that the bulk composition of the ultrafine mode organics during NPEs was very similar to that of anthropogenically influenced secondary organic aerosol (SOA) observed in transported urban plumes. In addition, the concentrations of species representative of urban emissions (e.g., black carbon, CO, NOx, and toluene) were significantly higher whereas the photo-oxidation products of biogenic VOCs (volatile organic compounds) and the biogenically influenced SOA also increased moderately during the NPE days compared to the non-event days. These results indicate that the frequently occurring NPEs over the Sacramento and Sierra Nevada regions were mainly driven by urban plumes from Sacramento and the San Francisco Bay Area, and that the interaction of regional biogenic emissions with the urban plumes has enhanced the new particle growth. This finding has important implications for quantifying the climate impacts of NPEs on global scale.
- ItemModelling Ag-particle activation and growth in a TSI WCPC model 3785(München : European Geopyhsical Union, 2010) Stratmann, F.; Herrmann, E.; Petäjä, T.; Kulmala, M.In this work, we modelled activation and growth of silver particles in the water-operated TSI model 3785 water condensation particle counter (WCPC). Our objective was to investigate theoretically how various effects influence the counting efficiency of this CPC. Coupled fluid and particle dynamic processes were modelled with the computational fluid dynamics (CFD) code FLUENT in combination with the Fine Particle Model (FPM) to obtain profiles of temperature, vapour concentration, nucleation rate, and particle size. We found that the counting efficiency of the TSI 3785 for small particles might be affected by the presence of larger particles. Moreover, homogeneous nucleation processes can significantly influence counting efficiency.
- ItemEvaluation of a global aerosol microphysics model against size-resolved particle statistics in the marine atmosphere(München : European Geopyhsical Union, 2007) Spracklen, D.V.; Pringle, K.J.; Carslaw, K.S.; Mann, G.W.; Manktelow, P.; Heintzenberg, J.A statistical synthesis of marine aerosol measurements from experiments in four different oceans is used to evaluate a global aerosol microphysics model (GLOMAP). We compare the model against observed size resolved particle concentrations, probability distributions, and the temporal persistence of different size particles. We attempt to explain the observed sub-micrometre size distributions in terms of sulfate and sea spray and quantify the possible contributions of anthropogenic sulfate and carbonaceous material to the number and mass distribution. The model predicts a bimodal size distribution that agrees well with observations as a grand average over all regions, but there are large regional differences. Notably, observed Aitken mode number concentrations are more than a factor 10 higher than in the model for the N Atlantic but a factor 7 lower than the model in the NW Pacific. We also find that modelled Aitken mode and accumulation mode geometric mean diameters are generally smaller in the model by 10–30%. Comparison with observed free tropospheric Aitken mode distributions suggests that the model underpredicts growth of these particles during descent to the marine boundary layer (MBL). Recent observations of a substantial organic component of free tropospheric aerosol could explain this discrepancy. We find that anthropogenic continental material makes a substantial contribution to N Atlantic MBL aerosol, with typically 60–90% of sulfate across the particle size range coming from anthropogenic sources, even if we analyse air that has spent an average of >120 h away from land. However, anthropogenic primary black carbon and organic carbon particles (at the emission size and quantity assumed here) do not explain the large discrepancies in Aitken mode number. Several explanations for the discrepancy are suggested. The lack of lower atmospheric particle formation in the model may explain low N Atlantic particle concentrations. However, the observed and modelled particle persistence at Cape Grim in the Southern Ocean, does not reveal a diurnal cycle consistent with a photochemically driven local particle source. We also show that a physically based cloud drop activation scheme better explains the observed change in accumulation mode geometric mean diameter with particle number.
- ItemEvaluation of the Lidar/Radiometer Inversion Code (LIRIC) to determine microphysical properties of volcanic and desert dust(München : European Geopyhsical Union, 2013) Wagner, J.; Ansmann, A.; Wandinger, U.; Seifert, P.; Schwarz, A.; Tesche, M.; Chaikovsky, A.; Dubovik, O.The Lidar/Radiometer Inversion Code (LIRIC) combines the multiwavelength lidar technique with sun/sky photometry and allows us to retrieve vertical profiles of particle optical and microphysical properties separately for fine-mode and coarse-mode particles. After a brief presentation of the theoretical background, we evaluate the potential of LIRIC to retrieve the optical and microphysical properties of irregularly shaped dust particles. The method is applied to two very different aerosol scenarios: a strong Saharan dust outbreak towards central Europe and an Eyjafjallajökull volcanic dust event. LIRIC profiles of particle mass concentrations for the coarse-mode as well as for the non-spherical particle fraction are compared with results for the non-spherical particle fraction as obtained with the polarization-lidar-based POLIPHON method. Similar comparisons for fine-mode and spherical particle fractions are presented also. Acceptable agreement between the different dust mass concentration profiles is obtained. LIRIC profiles of optical properties such as particle backscatter coefficient, lidar ratio, Ångström exponent, and particle depolarization ratio are compared with direct Raman lidar observations. Systematic deviations between the LIRIC retrieval products and the Raman lidar measurements of the desert dust lidar ratio, depolarization ratio, and spectral dependencies of particle backscatter and lidar ratio point to the applied spheroidal-particle model as main source for these uncertainties in the LIRIC results.
- ItemThe Ice Selective Inlet: A novel technique for exclusive extraction of pristine ice crystals in mixed-phase clouds(München : European Geopyhsical Union, 2015) Kupiszewski, P.; Weingartner, E.; Vochezer, P.; Schnaiter, M.; Bigi, A.; Gysel, M.; Rosati, B.; Toprak, E.; Mertes, S.; Baltensperger, U.Climate predictions are affected by high uncertainties partially due to an insufficient knowledge of aerosol–cloud interactions. One of the poorly understood processes is formation of mixed-phase clouds (MPCs) via heterogeneous ice nucleation. Field measurements of the atmospheric ice phase in MPCs are challenging due to the presence of much more numerous liquid droplets. The Ice Selective Inlet (ISI), presented in this paper, is a novel inlet designed to selectively sample pristine ice crystals in mixed-phase clouds and extract the ice residual particles contained within the crystals for physical and chemical characterization. Using a modular setup composed of a cyclone impactor, droplet evaporation unit and pumped counterflow virtual impactor (PCVI), the ISI segregates particles based on their inertia and phase, exclusively extracting small ice particles between 5 and 20 μm in diameter. The setup also includes optical particle spectrometers for analysis of the number size distribution and shape of the sampled hydrometeors. The novelty of the ISI is a droplet evaporation unit, which separates liquid droplets and ice crystals in the airborne state, thus avoiding physical impaction of the hydrometeors and limiting potential artefacts. The design and validation of the droplet evaporation unit is based on modelling studies of droplet evaporation rates and computational fluid dynamics simulations of gas and particle flows through the unit. Prior to deployment in the field, an inter-comparison of the optical particle size spectrometers and a characterization of the transmission efficiency of the PCVI was conducted in the laboratory. The ISI was subsequently deployed during the Cloud and Aerosol Characterization Experiment (CLACE) 2013 and 2014 – two extensive international field campaigns encompassing comprehensive measurements of cloud microphysics, as well as bulk aerosol, ice residual and ice nuclei properties. The campaigns provided an important opportunity for a proof of concept of the inlet design. In this work we present the setup of the ISI, including the modelling and laboratory characterization of its components, as well as field measurements demonstrating the ISI performance and validating the working principle of the inlet. Finally, measurements of biological aerosol during a Saharan dust event (SDE) are presented, showing a first indication of enrichment of bio-material in sub-2 μm ice residuals.
- ItemChemical composition of ambient aerosol, ice residues and cloud droplet residues in mixed-phase clouds: single particle analysis during the Cloud and Aerosol Characterization Experiment (CLACE 6)(München : European Geopyhsical Union, 2010) Kamphus, M.; Ettner-Mahl, M.; Klimach, T.; Drewnick, F.; Keller, L.; Cziczo, D.J.; Mertes, S.; Borrmann, S.; Curtius, J.Two different single particle mass spectrometers were operated in parallel at the Swiss High Alpine Research Station Jungfraujoch (JFJ, 3580 m a.s.l.) during the Cloud and Aerosol Characterization Experiment (CLACE 6) in February and March 2007. During mixed phase cloud events ice crystals from 5–20 μm were separated from larger ice aggregates, non-activated, interstitial aerosol particles and supercooled droplets using an Ice-Counterflow Virtual Impactor (Ice-CVI). During one cloud period supercooled droplets were additionally sampled and analyzed by changing the Ice-CVI setup. The small ice particles and droplets were evaporated by injection into dry air inside the Ice-CVI. The resulting ice and droplet residues (IR and DR) were analyzed for size and composition by the two single particle mass spectrometers: a custom-built Single Particle Laser-Ablation Time-of-Flight Mass Spectrometer (SPLAT) and a commercial Aerosol Time-of-Flight Mass Spectrometer (ATOFMS, TSI Model 3800). During CLACE 6 the SPLAT instrument characterized 355 individual IR that produced a mass spectrum for at least one polarity and the ATOFMS measured 152 IR. The mass spectra were binned in classes, based on the combination of dominating substances, such as mineral dust, sulfate, potassium and elemental carbon or organic material. The derived chemical information from the ice residues is compared to the JFJ ambient aerosol that was sampled while the measurement station was out of clouds (several thousand particles analyzed by SPLAT and ATOFMS) and to the composition of the residues of supercooled cloud droplets (SPLAT: 162 cloud droplet residues analyzed, ATOFMS: 1094). The measurements showed that mineral dust was strongly enhanced in the ice particle residues. Close to all of the SPLAT spectra from ice residues did contain signatures from mineral compounds, albeit connected with varying amounts of soluble compounds. Similarly, close to all of the ATOFMS IR spectra show a mineral or metallic component. Pure sulfate and nitrate containing particles were depleted in the ice residues. Sulfate and nitrate was found to dominate the droplet residues (~90% of the particles). The results from the two different single particle mass spectrometers were generally in agreement. Differences in the results originate from several causes, such as the different wavelength of the desorption and ionisation lasers and different size-dependent particle detection efficiencies.
- ItemSize distribution and optical properties of mineral dust aerosols transported in the western Mediterranean(München : European Geopyhsical Union, 2016) Denjean, C.; Cassola, F.; Mazzino, A.; Triquet, S.; Chevaillier, S.; Grand, N.; Bourrianne, T.; Momboisse, G.; Sellegri, K.; Schwarzenbock, A.; Freney, E.; Mallet, M.; Formenti, P.This study presents in situ aircraft measurements of Saharan mineral dust transported over the western Mediterranean basin in June–July 2013 during the ChArMEx/ADRIMED (the Chemistry-Aerosol Mediterranean Experiment/Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region) airborne campaign. Dust events differing in terms of source region (Algeria, Tunisia and Morocco), time of transport (1–5 days) and height of transport were sampled. Mineral dust were transported above the marine boundary layer, which conversely was dominated by pollution and marine aerosols. The dust vertical structure was extremely variable and characterized by either a single layer or a more complex and stratified structure with layers originating from different source regions. Mixing of mineral dust with pollution particles was observed depending on the height of transport of the dust layers. Dust layers carried a higher concentration of pollution particles below 3 km above sea level (a.s.l.) than above 3 km a.s.l., resulting in a scattering Ångström exponent up to 2.2 below 3 km a.s.l. However, the optical properties of the dust plumes remained practically unchanged with respect to values previously measured over source regions, regardless of the altitude. Moderate absorption of light by the dust plumes was observed with values of aerosol single scattering albedo at 530 nm ranging from 0.90 to 1.00. Concurrent calculations from the aerosol chemical composition revealed a negligible contribution of pollution particles to the absorption properties of the dust plumes that was due to a low contribution of refractory black carbon in regards to the fraction of dust and sulfate particles. This suggests that, even in the presence of moderate pollution, likely a persistent feature in the Mediterranean, the optical properties of the dust plumes could be assumed similar to those of native dust in radiative transfer simulations, modelling studies and satellite retrievals over the Mediterranean. Measurements also showed that the coarse mode of mineral dust was conserved even after 5 days of transport in the Mediterranean, which contrasts with the gravitational depletion of large particles observed during the transport of dust plumes over the Atlantic. Simulations with the WRF mesoscale meteorological model highlighted a strong vertical turbulence within the dust layers that could prevent deposition of large particles during their atmospheric transport. This has important implications for the dust radiative effects due to surface dimming, atmospheric heating and cloud formation. The results presented here add to the observational data set necessary for evaluating the role of mineral dust on the regional climate and rainfall patterns in the western Mediterranean basin and understanding their atmospheric transport at global scale.
- ItemFracture-induced softening for large-scale ice dynamics(München : European Geopyhsical Union, 2014) Albrecht, T.; Levermann, A.Floating ice shelves can exert a retentive and hence stabilizing force onto the inland ice sheet of Antarctica. However, this effect has been observed to diminish by the dynamic effects of fracture processes within the protective ice shelves, leading to accelerated ice flow and hence to a sea-level contribution. In order to account for the macroscopic effect of fracture processes on large-scale viscous ice dynamics (i.e., ice-shelf scale) we apply a continuum representation of fractures and related fracture growth into the prognostic Parallel Ice Sheet Model (PISM) and compare the results to observations. To this end we introduce a higher order accuracy advection scheme for the transport of the two-dimensional fracture density across the regular computational grid. Dynamic coupling of fractures and ice flow is attained by a reduction of effective ice viscosity proportional to the inferred fracture density. This formulation implies the possibility of non-linear threshold behavior due to self-amplified fracturing in shear regions triggered by small variations in the fracture-initiation threshold. As a result of prognostic flow simulations, sharp across-flow velocity gradients appear in fracture-weakened regions. These modeled gradients compare well in magnitude and location with those in observed flow patterns. This model framework is in principle expandable to grounded ice streams and provides simple means of investigating climate-induced effects on fracturing (e.g., hydro fracturing) and hence on the ice flow. It further constitutes a physically sound basis for an enhanced fracture-based calving parameterization.
- ItemIce nucleation efficiency of AgI: review and new insights(München : European Geopyhsical Union, 2016) Marcolli, Claudia; Nagare, Baban; Welti, André; Lohmann, UlrikeAgI is one of the best-investigated ice-nucleating substances. It has relevance for the atmosphere since it is used for glaciogenic cloud seeding. Theoretical and experimental studies over the last 60 years provide a complex picture of silver iodide as an ice-nucleating agent with conflicting and inconsistent results. This review compares experimental ice nucleation studies in order to analyze the factors that influence the ice nucleation ability of AgI. The following picture emerges from this analysis: the ice nucleation ability of AgI seems to be enhanced when the AgI particle is on the surface of a droplet, which is indeed the position that a particle takes when it can freely move in a droplet. The ice nucleation by particles with surfaces exposed to air depends on water adsorption. AgI surfaces seem to be most efficient at nucleating ice when they are exposed to relative humidity at or even above water saturation. For AgI particles that are completely immersed in water, the freezing temperature increases with increasing AgI surface area. Higher threshold freezing temperatures seem to correlate with improved lattice matches as can be seen for AgI–AgCl solid solutions and 3AgI·NH4I·6H2O, which have slightly better lattice matches with ice than AgI and also higher threshold freezing temperatures. However, the effect of a good lattice match is annihilated when the surfaces have charges. Also, the ice nucleation ability seems to decrease during dissolution of AgI particles. This introduces an additional history and time dependence for ice nucleation in cloud chambers with short residence times.