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    Ion-particle interactions during particle formation and growth at a coniferous forest site in central Europe
    (München : European Geopyhsical Union, 2014) Gonser, S.G.; Klein, F.; Birmili, W.; Größ, J.; Kulmala, M.; Manninen, H.E.; Wiedensohler, A.; Held, A.
    In this work, we examined the interaction of ions and neutral particles during atmospheric new particle formation (NPF) events. The analysis is based on simultaneous field measurements of atmospheric ions and total particles using a neutral cluster and air ion spectrometer (NAIS) across the diameter range 2–25 nm. The Waldstein research site is located in a spruce forest in NE Bavaria, Southern Germany, known for enhanced radon concentrations, presumably leading to elevated ionization rates. Our observations show that the occurrence of the ion nucleation mode preceded that of the total particle nucleation mode during all analyzed NPF events. The time difference between the appearance of 2 nm ions and 2 nm total particles was typically about 20 to 30 min. A cross correlation analysis showed a rapid decrease of the time difference between the ion and total modes during the growth process. Eventually, this time delay vanished when both ions and total particles did grow to larger diameters. Considering the growth rates of ions and total particles separately, total particles exhibited enhanced growth rates at diameters below 15 nm. This observation cannot be explained by condensation or coagulation, because these processes would act more efficiently on charged particles compared to neutral particles. To explain our observations, we propose a mechanism including recombination and attachment of continuously present cluster ions with the ion nucleation mode and the neutral nucleation mode, respectively.
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    Nucleation of jet engine oil vapours is a large source of aviation-related ultrafine particles
    (London : Springer Nature, 2022) Ungeheuer, Florian; Caudillo, Lucía; Ditas, Florian; Simon, Mario; van Pinxteren, Dominik; Kılıç, Doğuşhan; Rose, Diana; Jacobi, Stefan; Kürten, Andreas; Curtius, Joachim; Vogel, Alexander L.
    Large airports are a major source of ultrafine particles, which spread across densely populated residential areas, affecting air quality and human health. Jet engine lubrication oils are detectable in aviation-related ultrafine particles, however, their role in particle formation and growth remains unclear. Here we show the volatility and new-particle-formation ability of a common synthetic jet oil, and the quantified oil fraction in ambient ultrafine particles downwind of Frankfurt International Airport, Germany. We find that the oil mass fraction is largest in the smallest particles (10-18 nm) with 21% on average. Combining ambient particle-phase concentration and volatility of the jet oil compounds, we determine a lower-limit saturation ratio larger than 1 × 105 for ultra-low volatility organic compounds. This indicates that the oil is an efficient nucleation agent. Our results demonstrate that jet oil nucleation is an important mechanism that can explain the abundant observations of high number concentrations of non-refractory ultrafine particles near airports.
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    Leipzig Ice Nucleation chamber Comparison (LINC): Intercomparison of four online ice nucleation counters
    (Katlenburg-Lindau : EGU, 2017) Burkert-Kohn, Monika; Wex, Heike; Welti, André; Hartmann, Susan; Grawe, Sarah; Hellner, Lisa; Herenz, Paul; Atkinson, James D.; Stratmann, Frank; Kanji, Zamin A.
    Ice crystal formation in atmospheric clouds has a strong effect on precipitation, cloud lifetime, cloud radiative properties, and thus the global energy budget. Primary ice formation above 235 K is initiated by nucleation on seed aerosol particles called ice-nucleating particles (INPs). Instruments that measure the ice-nucleating potential of aerosol particles in the atmosphere need to be able to accurately quantify ambient INP concentrations. In the last decade several instruments have been developed to investigate the ice-nucleating properties of aerosol particles and to measure ambient INP concentrations. Therefore, there is a need for intercomparisons to ensure instrument differences are not interpreted as scientific findings. In this study, we intercompare the results from parallel measurements using four online ice nucleation chambers. Seven different aerosol types are tested including untreated and acid-treated mineral dusts (microcline, which is a K-feldspar, and kaolinite), as well as birch pollen washing waters. Experiments exploring heterogeneous ice nucleation above and below water saturation are performed to cover the whole range of atmospherically relevant thermodynamic conditions that can be investigated with the intercompared chambers. The Leipzig Aerosol Cloud Interaction Simulator (LACIS) and the Portable Immersion Mode Cooling chAmber coupled to the Portable Ice Nucleation Chamber (PIMCA-PINC) performed measurements in the immersion freezing mode. Additionally, two continuous-flow diffusion chambers (CFDCs) PINC and the Spectrometer for Ice Nuclei (SPIN) are used to perform measurements below and just above water saturation, nominally presenting deposition nucleation and condensation freezing. The results of LACIS and PIMCA-PINC agree well over the whole range of measured frozen fractions (FFs) and temperature. In general PINC and SPIN compare well and the observed differences are explained by the ice crystal growth and different residence times in the chamber. To study the mechanisms responsible for the ice nucleation in the four instruments, the FF (from LACIS and PIMCA-PINC) and the activated fraction, AF (from PINC and SPIN), are compared. Measured FFs are on the order of a factor of 3 higher than AFs, but are not consistent for all aerosol types and temperatures investigated. It is shown that measurements from CFDCs cannot be assumed to produce the same results as those instruments exclusively measuring immersion freezing. Instead, the need to apply a scaling factor to CFDCs operating above water saturation has to be considered to allow comparison with immersion freezing devices. Our results provide further awareness of factors such as the importance of dispersion methods and the quality of particle size selection for intercomparing online INP counters.
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    Ice-nucleating particle versus ice crystal number concentrationin altocumulus and cirrus layers embedded in Saharan dust: a closure study
    (Katlenburg-Lindau : EGU, 2019) Ansmann, Albert; Mamouri, Rodanthi-Elisavet; Bühl, Johannes; Seifert, Patric; Engelmann, Ronny; Hofer, Julian; Nisantzi, Argyro; Atkinson, James D.; Kanji, Zamin A.; Sierau, Berko; Vrekoussis, Mihalis; Sciare, Jean
    For the first time, a closure study of the relationship between the ice-nucleating particle concentration (INP; INPC) and ice crystal number concentration (ICNC) in altocumulus and cirrus layers, solely based on groundbased active remote sensing, is presented. Such aerosol- cloud closure experiments are required (a) to better understand aerosol-cloud interaction in the case of mixed-phase clouds, (b) to explore to what extent heterogeneous ice nucleation can contribute to cirrus formation, which is usually controlled by homogeneous freezing, and (c) to check the usefulness of available INPC parameterization schemes, applied to lidar profiles of aerosol optical and microphysical properties up to the tropopause level. The INPC-ICNC closure studies were conducted in Cyprus (Limassol and Nicosia) during a 6-week field campaign in March-April 2015 and during the 17-month CyCARE (Cyprus Clouds Aerosol and Rain Experiment) campaign. The focus was on altocumulus and cirrus layers which developed in pronounced Saharan dust layers at heights from 5 to 11 km. As a highlight, a long-lasting cirrus event was studied which was linked to the development of a very strong dust-infused baroclinic storm (DIBS) over Algeria. The DIBS was associated with strong convective cloud development and lifted large amounts of Saharan dust into the upper troposphere, where the dust influenced the evolution of an unusually large anvil cirrus shield and the subsequent transformation into an cirrus uncinus cloud system extending from the eastern Mediterranean to central Asia, and thus over more than 3500 km. Cloud top temperatures of the three discussed closure study cases ranged from - 20 to -57 °C. The INPC was estimated from polarization/Raman lidar observations in combination with published INPC parameterization schemes, whereas the ICNC was retrieved from combined Doppler lidar, aerosol lidar, and cloud radar observations of the terminal velocity of falling ice crystals, radar reflectivity, and lidar backscatter in combination with the modeling of backscattering at the 532 and 8.5 mm wavelengths. A good-to-acceptable agreement between INPC (observed before and after the occurrence of the cloud layer under investigation) and ICNC values was found in the discussed three proof-of-concept closure experiments. In these case studies, INPC and ICNC values matched within an order of magnitude (i.e., within the uncertainty ranges of the INPC and ICNC estimates), and they ranged from 0.1 to 10 L-1 in the altocumulus layers and 1 to 50 L-1 in the cirrus layers observed between 8 and 11 km height. The successful closure experiments corroborate the important role of heterogeneous ice nucleation in atmospheric ice formation processes when mineral dust is present. The observed longlasting cirrus event could be fully explained by the presence of dust, i.e., without the need for homogeneous ice nucleation processes. © 2019 Author(s).
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    Overview of the Chemistry-Aerosol Mediterranean Experiment/Aerosol Direct Radiative Forcing on the Mediterranean Climate (ChArMEx/ADRIMED) summer 2013 campaign
    (München : European Geopyhsical Union, 2016) Mallet, M.; Dulac, F.; Formenti, P.; Nabat, P.; Sciare, J.; Roberts, G.; Pelon, J.; Ancellet, G.; Tanré, D.; Parol, F.; Denjean, C.; Brogniez, G.; di Sarra, A.; Alados-Arboledas, L.; Arndt, J.; Auriol, F.; Blarel, L.; Bourrianne, T.; Chazette, P.; Chevaillier, S.; Claeys, M.; D'Anna, B.; Derimian, Y.; Desboeufs, K.; Di Iorio, T.; Doussin, J.-F.; Durand, P.; Féron, A.; Freney, E.; Gaimoz, C.; Goloub, P.; Gómez-Amo, J.L.; Granados-Muñoz, M.J.; Grand, N.; Hamonou, E.; Jankowiak, I.; Jeannot, M.; Léon, J.-F.; Maillé, M.; Mailler, S.; Meloni, D.; Menut, L.; Momboisse, G.; Nicolas, J.; Podvin, T.; Pont, V.; Rea, G.; Renard, J.-B.; Roblou, L.; Schepanski, K.; Schwarzenboeck, A.; Sellegri, K.; Sicard, M.; Solmon, F.; Somot, S.; Torres, B.; Totems, J.; Triquet, S.; Verdier, N.; Verwaerde, C.; Waquet, F.; Wenger, J.; Zapf, P.
    The Chemistry-Aerosol Mediterranean Experiment (ChArMEx; is a collaborative research program federating international activities to investigate Mediterranean regional chemistry-climate interactions. A special observing period (SOP-1a) including intensive airborne measurements was performed in the framework of the Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region (ADRIMED) project during the Mediterranean dry season over the western and central Mediterranean basins, with a focus on aerosol-radiation measurements and their modeling. The SOP-1a took place from 11 June to 5 July 2013. Airborne measurements were made by both the ATR-42 and F-20 French research aircraft operated from Sardinia (Italy) and instrumented for in situ and remote-sensing measurements, respectively, and by sounding and drifting balloons, launched in Minorca. The experimental setup also involved several ground-based measurement sites on islands including two ground-based reference stations in Corsica and Lampedusa and secondary monitoring sites in Minorca and Sicily. Additional measurements including lidar profiling were also performed on alert during aircraft operations at EARLINET/ACTRIS stations at Granada and Barcelona in Spain, and in southern Italy. Remote-sensing aerosol products from satellites (MSG/SEVIRI, MODIS) and from the AERONET/PHOTONS network were also used. Dedicated meso-scale and regional modeling experiments were performed in relation to this observational effort. We provide here an overview of the different surface and aircraft observations deployed during the ChArMEx/ADRIMED period and of associated modeling studies together with an analysis of the synoptic conditions that determined the aerosol emission and transport. Meteorological conditions observed during this campaign (moderate temperatures and southern flows) were not favorable to producing high levels of atmospheric pollutants or intense biomass burning events in the region. However, numerous mineral dust plumes were observed during the campaign, with the main sources located in Morocco, Algeria and Tunisia, leading to aerosol optical depth (AOD) values ranging between 0.2 and 0.6 (at 440 nm) over the western and central Mediterranean basins. One important point of this experiment concerns the direct observations of aerosol extinction onboard the ATR-42, using the CAPS system, showing local maxima reaching up to 150 M m-1 within the dust plume. Non-negligible aerosol extinction (about 50 M m-1) has also been observed within the marine boundary layer (MBL). By combining the ATR-42 extinction coefficient observations with absorption and scattering measurements, we performed a complete optical closure revealing excellent agreement with estimated optical properties. This additional information on extinction properties has allowed calculation of the dust single scattering albedo (SSA) with a high level of confidence over the western Mediterranean. Our results show a moderate variability from 0.90 to 1.00 (at 530 nm) for all flights studied compared to that reported in the literature on this optical parameter. Our results underline also a relatively low difference in SSA with values derived near dust sources. In parallel, active remote-sensing observations from the surface and onboard the F-20 aircraft suggest a complex vertical structure of particles and distinct aerosol layers with sea spray and pollution located within the MBL, and mineral dust and/or aged North American smoke particles located above (up to 6-7 km in altitude). Aircraft and balloon-borne observations allow one to investigate the vertical structure of the aerosol size distribution showing particles characterized by a large size (> 10 μm in diameter) within dust plumes. In most of cases, a coarse mode characterized by an effective diameter ranging between 5 and 10 μm, has been detected above the MBL. In terms of shortwave (SW) direct forcing, in situ surface and aircraft observations have been merged and used as inputs in 1-D radiative transfer codes for calculating the aerosol direct radiative forcing (DRF). Results show significant surface SW instantaneous forcing (up to -90 W m-2 at noon). Aircraft observations provide also original estimates of the vertical structure of SW and LW radiative heating revealing significant instantaneous values of about 5° K per day in the solar spectrum (for a solar angle of 30°) within the dust layer. Associated 3-D modeling studies from regional climate (RCM) and chemistry transport (CTM) models indicate a relatively good agreement for simulated AOD compared with observations from the AERONET/PHOTONS network and satellite data, especially for long-range dust transport. Calculations of the 3-D SW (clear-sky) surface DRF indicate an average of about -10 to -20 W m-2 (for the whole period) over the Mediterranean Sea together with maxima (-50 W m-2) over northern Africa. The top of the atmosphere (TOA) DRF is shown to be highly variable within the domain, due to moderate absorbing properties of dust and changes in the surface albedo. Indeed, 3-D simulations indicate negative forcing over the Mediterranean Sea and Europe and positive forcing over northern Africa. Finally, a multi-year simulation, performed for the 2003 to 2009 period and including an ocean-atmosphere (O-A) coupling, underlines the impact of the aerosol direct radiative forcing on the sea surface temperature, O-A fluxes and the hydrological cycle over the Mediterranean.
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    Modelling 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.
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    Formation and growth of nucleated particles into cloud condensation nuclei: Model-measurement comparison
    (München : European Geopyhsical Union, 2013) Westervelt, D.M.; Pierce, J.R.; Riipinen, I.; Trivitayanurak, W.; Hamed, A.; Kulmala, M.; Laaksonen, A.; Decesari, S.; Adams, P.J.
    Aerosol nucleation occurs frequently in the atmosphere and is an important source of particle number. Observations suggest that nucleated particles are capable of growing to sufficiently large sizes that they act as cloud condensation nuclei (CCN), but some global models have reported that CCN concentrations are only modestly sensitive to large changes in nucleation rates. Here we present a novel approach for using long-term size distribution observations to evaluate a global aerosol model's ability to predict formation rates of CCN from nucleation and growth events. We derive from observations at five locations nucleation-relevant metrics such as nucleation rate of particles at diameter of 3 nm (J3), diameter growth rate (GR), particle survival probability (SP), condensation and coagulation sinks, and CCN formation rate (J100). These quantities are also derived for a global microphysical model, GEOS-Chem-TOMAS, and compared to the observations on a daily basis. Using GEOS-Chem-TOMAS, we simulate nucleation events predicted by ternary (with a 10−5 tuning factor) or activation nucleation over one year and find that the model slightly understates the observed annual-average CCN formation mostly due to bias in the nucleation rate predictions, but by no more than 50% in the ternary simulations. At the two locations expected to be most impacted by large-scale regional nucleation, Hyytiälä and San Pietro Capofiume, predicted annual-average CCN formation rates are within 34 and 2% of the observations, respectively. Model-predicted annual-average growth rates are within 25% across all sites but also show a slight tendency to underestimate the observations, at least in the ternary nucleation simulations. On days that the growing nucleation mode reaches 100 nm, median single-day survival probabilities to 100 nm for the model and measurements range from less than 1–6% across the five locations we considered; however, this does not include particles that may eventually grow to 100 nm after the first day. This detailed exploration of new particle formation and growth dynamics adds support to the use of global models as tools for assessing the contribution of microphysical processes such as nucleation to the total number and CCN budget.
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    Potential of polarization lidar to provide profiles of CCN-and INP-relevant aerosol parameters
    (München : European Geopyhsical Union, 2016) Mamouri, Rodanthi-Elisavet; Ansmann, Albert
    We investigate the potential of polarization lidar to provide vertical profiles of aerosol parameters from which cloud condensation nucleus (CCN) and ice nucleating particle (INP) number concentrations can be estimated. We show that height profiles of particle number concentrations n50, dry considering dry aerosol particles with radius  > 50 nm (reservoir of CCN in the case of marine and continental non-desert aerosols), n100, dry (particles with dry radius  >  100 nm, reservoir of desert dust CCN), and of n250, dry (particles with dry radius  >  250 nm, reservoir of favorable INP), as well as profiles of the particle surface area concentration sdry (used in INP parameterizations) can be retrieved from lidar-derived aerosol extinction coefficients σ with relative uncertainties of a factor of 1.5–2 in the case of n50, dry and n100, dry and of about 25–50 % in the case of n250, dry and sdry. Of key importance is the potential of polarization lidar to distinguish and separate the optical properties of desert aerosols from non-desert aerosol such as continental and marine particles. We investigate the relationship between σ, measured at ambient atmospheric conditions, and n50, dry for marine and continental aerosols, n100, dry for desert dust particles, and n250, dry and sdry for three aerosol types (desert, non-desert continental, marine) and for the main lidar wavelengths of 355, 532, and 1064 nm. Our study is based on multiyear Aerosol Robotic Network (AERONET) photometer observations of aerosol optical thickness and column-integrated particle size distribution at Leipzig, Germany, and Limassol, Cyprus, which cover all realistic aerosol mixtures. We further include AERONET data from field campaigns in Morocco, Cabo Verde, and Barbados, which provide pure dust and pure marine aerosol scenarios. By means of a simple CCN parameterization (with n50, dry or n100, dry as input) and available INP parameterization schemes (with n250, dry and sdry as input) we finally compute profiles of the CCN-relevant particle number concentration nCCN and the INP number concentration nINP. We apply the method to a lidar observation of a heavy dust outbreak crossing Cyprus and a case dominated by continental aerosol pollution.
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    Comparing contact and immersion freezing from continuous flow diffusion chambers
    (München : European Geopyhsical Union, 2016) Nagare, Baban; Marcolli, Claudia; Welti, André; Stetzer, Olaf; Lohmann, Ulrike
    Ice nucleating particles (INPs) in the atmosphere are responsible for glaciating cloud droplets between 237 and 273 K. Different mechanisms of heterogeneous ice nucleation can compete under mixed-phase cloud conditions. Contact freezing is considered relevant because higher ice nucleation temperatures than for immersion freezing for the same INPs were observed. It has limitations because its efficiency depends on the number of collisions between cloud droplets and INPs. To date, direct comparisons of contact and immersion freezing with the same INP, for similar residence times and concentrations, are lacking. This study compares immersion and contact freezing efficiencies of three different INPs. The contact freezing data were obtained with the ETH CoLlision Ice Nucleation CHamber (CLINCH) using 80 µm diameter droplets, which can interact with INPs for residence times of 2 and 4 s in the chamber. The contact freezing efficiency was calculated by estimating the number of collisions between droplets and particles. Theoretical formulations of collision efficiencies gave too high freezing efficiencies for all investigated INPs, namely AgI particles with 200 nm electrical mobility diameter, 400 and 800 nm diameter Arizona Test Dust (ATD) and kaolinite particles. Comparison of freezing efficiencies by contact and immersion freezing is therefore limited by the accuracy of collision efficiencies. The concentration of particles was 1000 cm−3 for ATD and kaolinite and 500, 1000, 2000 and 5000 cm−3 for AgI. For concentrations  <  5000 cm−3, the droplets collect only one particle on average during their time in the chamber. For ATD and kaolinite particles, contact freezing efficiencies at 2 s residence time were smaller than at 4 s, which is in disagreement with a collisional contact freezing process but in accordance with immersion freezing or adhesion freezing. With “adhesion freezing”, we refer to a contact nucleation process that is enhanced compared to immersion freezing due to the position of the INP on the droplet, and we discriminate it from collisional contact freezing, which assumes an enhancement due to the collision of the particle with the droplet. For best comparison with contact freezing results, immersion freezing experiments of the same INPs were performed with the continuous flow diffusion chamber Immersion Mode Cooling chAmber–Zurich Ice Nucleation Chamber (IMCA–ZINC) for a 3 s residence time. In IMCA–ZINC, each INP is activated into a droplet in IMCA and provides its surface for ice nucleation in the ZINC chamber. The comparison of contact and immersion freezing results did not confirm a general enhancement of freezing efficiency for contact compared with immersion freezing experiments. For AgI particles the onset of heterogeneous freezing in CLINCH was even shifted to lower temperatures compared with IMCA–ZINC. For ATD, freezing efficiencies for contact and immersion freezing experiments were similar. For kaolinite particles, contact freezing became detectable at higher temperatures than immersion freezing. Using contact angle information between water and the INP, it is discussed how the position of the INP in or on the droplets may influence its ice nucleation activity.
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    Ice-nucleating particle concentrations unaffected by urban air pollution in Beijing, China
    (Katlenburg-Lindau : EGU, 2018) Chen, Jie; Wu, Zhijun; Augustin-Bauditz, Stefanie; Grawe, Sarah; Hartmann, Markus; Pei, Xiangyu; Liu, Zirui; Ji, Dongsheng; Wex, Heike
    Exceedingly high levels of PM2.5 with complex chemical composition occur frequently in China. It has been speculated whether anthropogenic PM2.5 may significantly contribute to ice-nucleating particles (INP). However, few studies have focused on the ice-nucleating properties of urban particles. In this work, two ice-nucleating droplet arrays have been used to determine the atmospheric number concentration of INP (NINP) in the range from -6 to -25 °C in Beijing. No correlations between NINP and either PM2.5 or black carbon mass concentrations were found, although both varied by more than a factor of 30 during the sampling period. Similarly, there were no correlations between NINP and either total particle number concentration or number concentrations for particles with diameters > 500 nm. Furthermore, there was no clear difference between day and night samples. All these results indicate that Beijing air pollution did not increase or decrease INP concentrations in the examined temperature range above values observed in nonurban areas; hence, the background INP concentrations might not be anthropogenically influenced as far as urban air pollution is concerned, at least in the examined temperature range.