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- ItemInfrequent new particle formation over the remote boreal forest of Siberia(Amsterdam [u.a.] : Elsevier Science, 2018) Wiedensohler, A.; Ma, N.; Birmili, W.; Heintzenberg, J.; Ditas, F.; Andreae, M.O.; Panov, A.Aerosol particle number size distributions (PNSD) were investigated to verify, if extremely low-volatility organic vapors (ELVOC) from natural sources alone could induce new particle formation and growth events over the remote boreal forest region of Siberia, hundreds of kilometers away from significant anthropogenic sources. We re-evaluated observations determined at a height of 300 m of the remote observatory ZOTTO (Zotino Tall Tower Observatory, http://www.zottoproject.org). We found that new particle formation events occurred only on 11 days in a 3-year period, suggesting that homogeneous nucleation with a subsequent condensational growth could not be the major process, maintaining the particle number concentration in the planetary boundary layer of the remote boreal forest area of Siberia. © 2018 Elsevier Ltd
- ItemThe Fifth International Workshop on Ice Nucleation phase 2 (FIN-02): Laboratory intercomparison of ice nucleation measurements(Katlenburg-Lindau : Copernicus, 2018) DeMott, Paul J.; Möhler, Ottmar; Cziczo, Daniel J.; Hiranuma, Naruki; Petters, Markus D.; Petters, Sarah S.; Belosi, Franco; Bingemer, Heinz G.; Brooks, Sarah D.; Budke, Carsten; Burkert-Kohn, Monika; Collier, Kristen N.; Danielczok, Anja; Eppers, Oliver; Felgitsch, Laura; Garimella, Sarvesh; Grothe, Hinrich; Herenz, Paul; Hill, Thomas C. J.; Höhler, Kristina; Kanji, Zamin A.; Kiselev, Alexei; Koop, Thomas; Kristensen, Thomas B.; Krüger, Konstantin; Kulkarni, Gourihar; Levin, Ezra J. T.; Murray, Benjamin J.; Nicosia, Alessia; O'Sullivan, Daniel; Peckhaus, Andreas; Polen, Michael J.; Price, Hannah C.; Reicher, Naama; Rothenberg, Daniel A.; Rudich, Yinon; Santachiara, Gianni; Schiebel, Thea; Schrod, Jann; Seifried, Teresa M.; Stratmann, Frank; Sullivan, Ryan C.; Suski, Kaitlyn J.; Szakáll, Miklós; Taylor, Hans P.; Ullrich, Romy; Vergara-Temprado, Jesus; Wagner, Robert; Whale, Thomas F.; Weber, Daniel; Welti, André; Wilson, Theodore W.; Wolf, Martin J.; Zenker, JakeThe second phase of the Fifth International Ice Nucleation Workshop (FIN-02) involved the gathering of a large number of researchers at the Karlsruhe Institute of Technology's Aerosol Interactions and Dynamics of the Atmosphere (AIDA) facility to promote characterization and understanding of ice nucleation measurements made by a variety of methods used worldwide. Compared to the previous workshop in 2007, participation was doubled, reflecting a vibrant research area. Experimental methods involved sampling of aerosol particles by direct processing ice nucleation measuring systems from the same volume of air in separate experiments using different ice nucleating particle (INP) types, and collections of aerosol particle samples onto filters or into liquid for sharing amongst measurement techniques that post-process these samples. In this manner, any errors introduced by differences in generation methods when samples are shared across laboratories were mitigated. Furthermore, as much as possible, aerosol particle size distribution was controlled so that the size limitations of different methods were minimized. The results presented here use data from the workshop to assess the comparability of immersion freezing measurement methods activating INPs in bulk suspensions, methods that activate INPs in condensation and/or immersion freezing modes as single particles on a substrate, continuous flow diffusion chambers (CFDCs) directly sampling and processing particles well above water saturation to maximize immersion and subsequent freezing of aerosol particles, and expansion cloud chamber simulations in which liquid cloud droplets were first activated on aerosol particles prior to freezing. The AIDA expansion chamber measurements are expected to be the closest representation to INP activation in atmospheric cloud parcels in these comparisons, due to exposing particles freely to adiabatic cooling. The different particle types used as INPs included the minerals illite NX and potassium feldspar (K-feldspar), two natural soil dusts representative of arable sandy loam (Argentina) and highly erodible sandy dryland (Tunisia) soils, respectively, and a bacterial INP (Snomax®). Considered together, the agreement among post-processed immersion freezing measurements of the numbers and fractions of particles active at different temperatures following bulk collection of particles into liquid was excellent, with possible temperature uncertainties inferred to be a key factor in determining INP uncertainties. Collection onto filters for rinsing versus directly into liquid in impingers made little difference. For methods that activated collected single particles on a substrate at a controlled humidity at or above water saturation, agreement with immersion freezing methods was good in most cases, but was biased low in a few others for reasons that have not been resolved, but could relate to water vapor competition effects. Amongst CFDC-style instruments, various factors requiring (variable) higher supersaturations to achieve equivalent immersion freezing activation dominate the uncertainty between these measurements, and for comparison with bulk immersion freezing methods. When operated above water saturation to include assessment of immersion freezing, CFDC measurements often measured at or above the upper bound of immersion freezing device measurements, but often underestimated INP concentration in comparison to an immersion freezing method that first activates all particles into liquid droplets prior to cooling (the PIMCA-PINC device, or Portable Immersion Mode Cooling chAmber-Portable Ice Nucleation Chamber), and typically slightly underestimated INP number concentrations in comparison to cloud parcel expansions in the AIDA chamber; this can be largely mitigated when it is possible to raise the relative humidity to sufficiently high values in the CFDCs, although this is not always possible operationally. Correspondence of measurements of INPs among direct sampling and post-processing systems varied depending on the INP type. Agreement was best for Snomax® particles in the temperature regime colder than -10°C, where their ice nucleation activity is nearly maximized and changes very little with temperature. At temperatures warmer than -10°C, Snomax® INP measurements (all via freezing of suspensions) demonstrated discrepancies consistent with previous reports of the instability of its protein aggregates that appear to make it less suitable as a calibration INP at these temperatures. For Argentinian soil dust particles, there was excellent agreement across all measurement methods; measures ranged within 1 order of magnitude for INP number concentrations, active fractions and calculated active site densities over a 25 to 30°C range and 5 to 8 orders of corresponding magnitude change in number concentrations. This was also the case for all temperatures warmer than -25°C in Tunisian dust experiments. In contrast, discrepancies in measurements of INP concentrations or active site densities that exceeded 2 orders of magnitude across a broad range of temperature measurements found at temperatures warmer than -25°C in a previous study were replicated for illite NX. Discrepancies also exceeded 2 orders of magnitude at temperatures of -20 to -25°C for potassium feldspar (K-feldspar), but these coincided with the range of temperatures at which INP concentrations increase rapidly at approximately an order of magnitude per 2°C cooling for K-feldspar. These few discrepancies did not outweigh the overall positive outcomes of the workshop activity, nor the future utility of this data set or future similar efforts for resolving remaining measurement issues. Measurements of the same materials were repeatable over the time of the workshop and demonstrated strong consistency with prior studies, as reflected by agreement of data broadly with parameterizations of different specific or general (e.g., soil dust) aerosol types. The divergent measurements of the INP activity of illite NX by direct versus post-processing methods were not repeated for other particle types, and the Snomax° data demonstrated that, at least for a biological INP type, there is no expected measurement bias between bulk collection and direct immediately processed freezing methods to as warm as -10°C. Since particle size ranges were limited for this workshop, it can be expected that for atmospheric populations of INPs, measurement discrepancies will appear due to the different capabilities of methods for sampling the full aerosol size distribution, or due to limitations on achieving sufficient water supersaturations to fully capture immersion freezing in direct processing instruments. Overall, this workshop presents an improved picture of present capabilities for measuring INPs than in past workshops, and provides direction toward addressing remaining measurement issues.
- ItemSimultaneous observations of NLCs and MSEs at midlatitudes: Implications for formation and advection of ice particles(Göttingen : Copernicus GmbH, 2018) Gerding, M.; Zöllner, J.; Zecha, M.; Baumgarten, K.; Höffner, J.; Stober, G.; Lübken, F.-J.We combined ground-based lidar observations of noctilucent clouds (NLCs) with collocated, simultaneous radar observations of mesospheric summer echoes (MSEs) in order to compare ice cloud altitudes at a midlatitude site (Kühlungsborn, Germany, 54° N, 12° E). Lidar observations are limited to larger particles ( > 10 nm), while radars are also sensitive to small particles ( < 10 nm), but require sufficient ionization and turbulence at the ice cloud altitudes. The combined lidar and radar data set thus includes some information on the size distribution within the cloud and through this on the of the cloud. The soundings for this study are carried out by the IAP Rayleigh-Mie-Raman (RMR) lidar and the OSWIN VHF radar. On average, there is no difference between the lower edges (lowNLC and lowMSE). The mean difference of the upper edges upNLC and upMSE is g1/4 500 m, which is much less than expected from observations at higher latitudes. In contrast to high latitudes, the MSEs above our location typically do not reach much higher than the NLCs. In addition to earlier studies from our site, this gives additional evidence for the supposition that clouds containing large enough particles to be observed by lidar are not formed locally but are advected from higher latitudes. During the advection process, the smaller particles in the upper part of the cloud either grow and sediment, or they sublimate. Both processes result in a thinning of the layer. High-altitude MSEs, usually indicating nucleation of ice particles, are rarely observed in conjunction with lidar observations of NLCs at Kühlungsborn. © Author(s) 2018.
- ItemEnhanced pore space analysis by use of μ-CT, MIP, NMR, and SIP(Göttingen : Copernicus Publ., 2018) Zhang, Zeyu; Kruschwitz, Sabine; Weller, Andreas; Halisch, MatthiasWe investigate the pore space of rock samples with respect to different petrophysical parameters using various methods, which provide data on pore size distributions, including micro computed tomography (μ-CT), mercury intrusion porosimetry (MIP), nuclear magnetic resonance (NMR), and spectral-induced polarization (SIP). The resulting cumulative distributions of pore volume as a function of pore size are compared. Considering that the methods differ with regard to their limits of resolution, a multiple-length-scale characterization of the pore space is proposed, that is based on a combination of the results from all of these methods. The approach is demonstrated using samples of Bentheimer and Röttbacher sandstone. Additionally, we compare the potential of SIP to provide a pore size distribution with other commonly used methods (MIP, NMR). The limits of resolution of SIP depend on the usable frequency range (between 0.002 and 100 Hz). The methods with similar resolution show a similar behavior of the cumulative pore volume distribution in the overlapping pore size range. We assume that μ-CT and NMR provide the pore body size while MIP and SIP characterize the pore throat size. Our study shows that a good agreement between the pore radius distributions can only be achieved if the curves are adjusted considering the resolution and pore volume in the relevant range of pore radii. The MIP curve with the widest range in resolution should be used as reference.
- ItemVariability of black carbon mass concentrations, sub-micrometer particle number concentrations and size distributions: results of the German Ultrafine Aerosol Network ranging from city street to High Alpine locations(Amsterdam [u.a.] : Elsevier Science, 2018) Sun, J.; Birmili, W.; Hermann, M.; Tuch, T.; Weinhold, K.; Spindler, G.; Schladitz, A.; Bastian, S.; Löschau, G.; Cyrys, J.; Gu, J.; Flentje, H.; Briel, B.; Asbac, C.; Kaminski, H.; Ries, L.; Sohme, R.; Gerwig, H.; Wirtz, K.; Meinhardt, F.; Schwerin, A.; Bath, O.; Ma, N.; Wiedensohler, A.This work reports the first statistical analysis of multi-annual data on tropospheric aerosols from the German Ultrafine Aerosol Network (GUAN). Compared to other networks worldwide, GUAN with 17 measurement locations has the most sites equipped with particle number size distribution (PNSD) and equivalent black carbon (eBC) instruments and the most site categories in Germany ranging from city street/roadside to High Alpine. As we know, the variations of eBC and particle number concentration (PNC) are influenced by several factors such as source, transformation, transport and deposition. The dominant controlling factor for different pollutant parameters might be varied, leading to the different spatio-temporal variations among the measured parameters. Currently, a study of spatio-temporal variations of PNSD and eBC considering the influences of both site categories and spatial scale is still missing. Based on the multi-site dataset of GUAN, the goal of this study is to investigate how pollutant parameters may interfere with spatial characteristics and site categories. © 2019 The Authors
- ItemMeasurements of aerosol and CCN properties in the Mackenzie River delta (Canadian Arctic) during spring-summer transition in May 2014(Katlenburg-Lindau : EGU, 2018) Herenz, Paul; Wex, Heike; Henning, Silvia; Kristensen, Thomas Bjerring; Rubach, Florian; Roth, Anja; Borrmann, Stephan; Bozem, Heiko; Schulz, Hannes; Stratmann, FrankWithin the framework of the RACEPAC (Radiation-Aerosol-Cloud Experiment in the Arctic Circle) project, the Arctic aerosol, arriving at a ground-based station in Tuktoyaktuk (Mackenzie River delta area, Canada), was characterized during a period of 3 weeks in May 2014. Basic meteorological parameters and particle number size distributions (PNSDs) were observed and two distinct types of air masses were found. One type were typical Arctic haze air masses, termed accumulation-type air masses, characterized by a monomodal PNSD with a pronounced accumulation mode at sizes above 100 nm. These air masses were observed during a period when back trajectories indicate an air mass origin in the north-east of Canada. The other air mass type is characterized by a bimodal PNSD with a clear minimum around 90ĝ€†nm and with an Aitken mode consisting of freshly formed aerosol particles. Back trajectories indicate that these air masses, termed Aitken-type air masses, originated from the North Pacific. In addition, the application of the PSCF receptor model shows that air masses with their origin in active fire areas in central Canada and Siberia, in areas of industrial anthropogenic pollution (Norilsk and Prudhoe Bay Oil Field) and the north-west Pacific have enhanced total particle number concentrations (N CN). Generally, N CN ranged from 20 to 500 cmg'3, while cloud condensation nuclei (CCN) number concentrations were found to cover a range from less than 10 up to 250 cmg'3 for a supersaturation (SS) between 0.1 and 0.7 %. The hygroscopicity parameter of the CCN was determined to be 0.23 on average and variations in were largely attributed to measurement uncertainties.
Furthermore, simultaneous PNSD measurements at the ground station and on the Polar 6 research aircraft were performed. We found a good agreement of ground-based PNSDs with those measured between 200 and 1200 m. During two of the four overflights, particle number concentrations at 3000 m were found to be up to 20 times higher than those measured below 2000 m; for one of these two flights, PNSDs measured above 2000 m showed a different shape than those measured at lower altitudes. This is indicative of long-range transport from lower latitudes into the Arctic that can advect aerosol from different regions in different heights. - ItemSALSA2.0: The sectional aerosol module of the aerosol-chemistry-climate model ECHAM6.3.0-HAM2.3-MOZ1.0(Katlenburg-Lindau : Copernicus, 2018) Kokkola, Harri; Kühn, Thomas; Laakso, Anton; Bergman, Tommi; Lehtinen, Kari E. J.; Mielonen, Tero; Arola, Antti; Stadtler, Scarlet; Korhonen, Hannele; Ferrachat, Sylvaine; Lohmann, Ulrike; Neubauer, David; Tegen, Ina; Siegenthaler-Le Drian, Colombe; Schultz, Martin G.; Bey, Isabelle; Stier, Philip; Daskalakis, Nikos; Heald, Colette L.; Romakkaniemi, SamiIn this paper, we present the implementation and evaluation of the aerosol microphysics module SALSA2.0 in the framework of the aerosol-chemistry-climate model ECHAM-HAMMOZ. It is an alternative microphysics module to the default modal microphysics scheme M7 in ECHAM-HAMMOZ. The SALSA2.0 implementation within ECHAM-HAMMOZ is evaluated against observations of aerosol optical properties, aerosol mass, and size distributions, comparing also to the skill of the M7 implementation. The largest differences between the implementation of SALSA2.0 and M7 are in the methods used for calculating microphysical processes, i.e., nucleation, condensation, coagulation, and hydration. These differences in the microphysics are reflected in the results so that the largest differences between SALSA2.0 and M7 are evident over regions where the aerosol size distribution is heavily modified by the microphysical processing of aerosol particles. Such regions are, for example, highly polluted regions and regions strongly affected by biomass burning. In addition, in a simulation of the 1991 Mt. Pinatubo eruption in which a stratospheric sulfate plume was formed, the global burden and the effective radii of the stratospheric aerosol are very different in SALSA2.0 and M7. While SALSA2.0 was able to reproduce the observed time evolution of the global burden of sulfate and the effective radii of stratospheric aerosol, M7 strongly overestimates the removal of coarse stratospheric particles and thus underestimates the effective radius of stratospheric aerosol. As the mode widths of M7 have been optimized for the troposphere and were not designed to represent stratospheric aerosol, the ability of M7 to simulate the volcano plume was improved by modifying the mode widths, decreasing the standard deviations of the accumulation and coarse modes from 1.59 and 2.0, respectively, to 1.2 similar to what was observed after the Mt. Pinatubo eruption. Overall, SALSA2.0 shows promise in improving the aerosol description of ECHAM-HAMMOZ and can be further improved by implementing methods for aerosol processes that are more suitable for the sectional method, e.g., size-dependent emissions for aerosol species and size-resolved wet deposition.
- ItemLong-term cloud condensation nuclei number concentration, particle number size distribution and chemical composition measurements at regionally representative observatories(Katlenburg-Lindau : EGU, 2018) Schmale, Julia; Henning, Silvia; Decesari, Stefano; Henzing, Bas; Keskinen, Helmi; Sellegri, Karine; Ovadnevaite, Jurgita; Pöhlker, Mira L.; Brito, Joel; Bougiatioti, Aikaterini; Kristensson, Adam; Kalivitis, Nikos; Stavroulas, Iasonas; Carbone, Samara; Jefferson, Anne; Park, Minsu; Schlag, Patrick; Iwamoto, Yoko; Aalto, Pasi; Äijälä, Mikko; Bukowiecki, Nicolas; Ehn, Mikael; Frank, Göran; Fröhlich, Roman; Frumau, Arnoud; Herrmann, Erik; Herrmann, Hartmut; Holzinger, Rupert; Kos, Gerard; Kulmala, Markku; Mihalopoulos, Nikolaos; Nenes, Athanasios; O'Dowd, Colin; Petäjä, Tuukka; Picard, David; Pöhlker, Christopher; Pöschl, Ulrich; Poulain, Laurent; Prévôt, André Stephan Henry; Swietlicki, Erik; Andreae, Meinrat O.; Artaxo, Paulo; Wiedensohler, Alfred; Ogren, John; Matsuki, Atsushi; Yum, Seong Soo; Stratmann, Frank; Baltensperger, Urs; Gysel, MartinAerosol-cloud interactions (ACI) constitute the single largest uncertainty in anthropogenic radiative forcing. To reduce the uncertainties and gain more confidence in the simulation of ACI, models need to be evaluated against observations, in particular against measurements of cloud condensation nuclei (CCN). Here we present a data set - ready to be used for model validation - of long-term observations of CCN number concentrations, particle number size distributions and chemical composition from 12 sites on 3 continents. Studied environments include coastal background, rural background, alpine sites, remote forests and an urban surrounding. Expectedly, CCN characteristics are highly variable across site categories. However, they also vary within them, most strongly in the coastal background group, where CCN number concentrations can vary by up to a factor of 30 within one season. In terms of particle activation behaviour, most continental stations exhibit very similar activation ratios (relative to particles 20nm) across the range of 0.1 to 1.0% supersaturation. At the coastal sites the transition from particles being CCN inactive to becoming CCN active occurs over a wider range of the supersaturation spectrum. Several stations show strong seasonal cycles of CCN number concentrations and particle number size distributions, e.g. at Barrow (Arctic haze in spring), at the alpine stations (stronger influence of polluted boundary layer air masses in summer), the rain forest (wet and dry season) or Finokalia (wildfire influence in autumn). The rural background and urban sites exhibit relatively little variability throughout the year, while short-term variability can be high especially at the urban site. The average hygroscopicity parameter, calculated from the chemical composition of submicron particles was highest at the coastal site of Mace Head (0.6) and lowest at the rain forest station ATTO (0.2-0.3). We performed closure studies based on -Köhler theory to predict CCN number concentrations. The ratio of predicted to measured CCN concentrations is between 0.87 and 1.4 for five different types of . The temporal variability is also well captured, with Pearson correlation coefficients exceeding 0.87. Information on CCN number concentrations at many locations is important to better characterise ACI and their radiative forcing. But long-term comprehensive aerosol particle characterisations are labour intensive and costly. Hence, we recommend operating migrating-CCNCs to conduct collocated CCN number concentration and particle number size distribution measurements at individual locations throughout one year at least to derive a seasonally resolved hygroscopicity parameter. This way, CCN number concentrations can only be calculated based on continued particle number size distribution information and greater spatial coverage of long-term measurements can be achieved.