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- ItemIon-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.
- ItemEffects of aerosol size and coating thickness on the molecular detection using extractive electrospray ionization(Katlenburg-Lindau : European Geosciences Union, 2021) Lee, Chuan Ping; Surdu, Mihnea; Bell, David M.; Lamkaddam, Houssni; Wang, Mingyi; Ataei, Farnoush; Hofbauer, Victoria; Lopez, Brandon; Donahue, Neil M.; Dommen, Josef; Prevot, Andre S. H.; Slowik, Jay G.; Wang, Dongyu; Baltensperger, Urs; El Haddad, ImadExtractive electrospray ionization (EESI) has been a well-known technique for high-throughput online molecular characterization of chemical reaction products and intermediates, detection of native biomolecules, in vivo metabolomics, and environmental monitoring with negligible thermal and ionization-induced fragmentation for over two decades. However, the EESI extraction mechanism remains uncertain. Prior studies disagree on whether particles between 20 and 400nm diameter are fully extracted or if the extraction is limited to the surface layer. Here, we examined the analyte extraction mechanism by assessing the influence of particle size and coating thickness on the detection of the molecules therein. We find that particles are extracted fully: organics-coated NH4NO3 particles with a fixed core volume (156 and 226nm in diameter without coating) showed constant EESI signals for NH4NO3 independent of the shell coating thickness, while the signals of the secondary organic molecules comprising the shell varied proportionally to the shell volume. We also found that the EESI sensitivity exhibited a strong size dependence, with an increase in sensitivity by 1-3 orders of magnitude as particle size decreased from 300 to 30nm. This dependence varied with the electrospray (ES) droplet size, the particle size and the residence time for coagulation in the EESI inlet, suggesting that the EESI sensitivity was influenced by the coagulation coefficient between particles and ES droplets. Overall, our results indicate that, in the EESI, particles are fully extracted by the ES droplets regardless of the chemical composition, when they are collected by the ES droplets. However, their coalescence is not complete and depends strongly on their size. This size dependence is especially relevant when EESI is used to probe size-varying particles as is the case in aerosol formation and growth studies with size ranges below 100nm. © 2021 The Author(s).
- ItemObservation of viscosity transition in α-pinene secondary organic aerosol(München : European Geopyhsical Union, 2016) Järvinen, Emma; Ignatius, Karoliina; Nichman, Leonid; Kristensen, Thomas B.; Fuchs, Claudia; Hoyle, Christopher R.; Höppel, Niko; Corbin, Joel C.; Craven, Jill; Duplissy, Jonathan; Ehrhart, Sebastian; El Haddad, Imad; Frege, Carla; Gordon, Hamish; Jokinen, Tuija; Kallinger, Peter; Kirkby, Jasper; Kiselev, Alexei; Naumann, Karl-Heinz; Petäjä, Tuukka; Pinterich, Tamara; Prevot, Andre S.H.; Saathoff, Harald; Schiebel, Thea; Sengupta, Kamalika; Simon, Mario; Slowik, Jay G.; Tröstl, Jasmin; Virtanen, Annele; Vochezer, Paul; Vogt, Steffen; Wagner, Andrea C.; Wagner, Robert; Williamson, Christina; Winkler, Paul M.; Yan, Chao; Baltensperger, Urs; Donahue, Neil M.; Flagan, Rick C.; Gallagher, Martin; Hansel, Armin; Kulmala, Markku; Stratmann, Frank; Worsnop, Douglas R.; Möhler, Ottmar; Leisner, Thomas; Schnaiter, MartinUnder certain conditions, secondary organic aerosol (SOA) particles can exist in the atmosphere in an amorphous solid or semi-solid state. To determine their relevance to processes such as ice nucleation or chemistry occurring within particles requires knowledge of the temperature and relative humidity (RH) range for SOA to exist in these states. In the Cosmics Leaving Outdoor Droplets (CLOUD) experiment at The European Organisation for Nuclear Research (CERN), we deployed a new in situ optical method to detect the viscous state of α-pinene SOA particles and measured their transition from the amorphous highly viscous state to states of lower viscosity. The method is based on the depolarising properties of laboratory-produced non-spherical SOA particles and their transformation to non-depolarising spherical particles at relative humidities near the deliquescence point. We found that particles formed and grown in the chamber developed an asymmetric shape through coagulation. A transition to a spherical shape was observed as the RH was increased to between 35 % at −10 °C and 80 % at −38 °C, confirming previous calculations of the viscosity-transition conditions. Consequently, α-pinene SOA particles exist in a viscous state over a wide range of ambient conditions, including the cirrus region of the free troposphere. This has implications for the physical, chemical, and ice-nucleation properties of SOA and SOA-coated particles in the atmosphere.
- ItemMicrophysical and optical properties of dust and tropical biomass burning aerosol layers in the Cape Verde region - an overview of the airborne in situ and lidar measurements during SAMUM-2(Milton Park : Taylor & Francis, 2017) Weinzierl, Bernadett; Sauer, Daniel; Esselborn, Michael; Petzold, Andreas; Veira, Andreas; Rose, Maximilian; Mund, Susanne; Wirth, Martin; Ansmann, Albert; Tesche, Matthias; Gross, Silke; Freudenthaler, VolkerIn the framework of the Saharan Mineral Dust Experiment (SAMUM) airborne High Spectral Resolution Lidar and in situ measurements of the particle size, aerosol mixing state and absorption coefficient were conducted. Here, the properties of mineral dust and tropical biomass burning layers in the Cape Verde region in January/February 2008 are investigated and compared with the properties of fresh dust observed in May/June 2006 close the Sahara. In the Cape Verde area, we found a complex stratification with dust layers covering the altitude range below 2 km and biomass burning layers aloft. The aerosol type of the individual layers was classified based on depolarization and lidar ratios and, in addition, on in situ measured Ångström exponents of absorption åap. The dust layers had a depth of 1.3 ± 0.4 km and showed a median åap of 3.95. The median effective diameter Deff was 2.5 μm and the dust layers over Cape Verde yielded clear signals of aging: large particles were depleted due to gravitational settling and the accumulation mode diameter was shifted towards larger sizes as a result of coagulation. The tropical biomass layers had a depth of 2.0 ± 1.1 km and were characterized by a median åap of 1.34. They always contained a certain amount of large dust particles and showed a median Deff of 1.1 μm and a fine mode Deff,fine of 0.33. The dust and biomass burning layers had a median aerosol optical depth (AOD) of 0.23 and 0.09, respectively. The median contributions to the AOD of the total atmospheric column below 10 km were 75 and 37%, respectively.