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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.
- ItemIntercomparison of air ion spectrometers: An evaluation of results in varying conditions(München : European Geopyhsical Union, 2011) Gagné, S.; Lehtipalo, K.; Manninen, H.E.; Nieminen, T.; Schobesberger, S.; Franchin, A.; Yli-Juuti, T.; Boulon, J.; Sonntag, A.; Mirme, S.; Mirme, A.; Hõrrak, U.; Petäjä, T.; Asmi, E.; Kulmala, M.We evaluated 11 air ion spectrometers from Airel Ltd. after they had spent one year in field measurements as a part of the EUCAARI project: 5 Air Ion Spectrometers (AIS), 5 Neutral cluster and Air Ion Spectrometers (NAIS) and one Airborne NAIS (ANAIS). This is the first time that an ANAIS is evaluated and compared so extensively. The ion spectrometers' mobility and concentration accuracy was evaluated. Their measurements of ambient air were compared between themselves and to reference instruments: a Differential Mobility Particle Sizer (DMPS), a Balanced Scanning Mobility Analyzer (BSMA), and an Ion-DMPS. We report on the simultaneous measurement of a new particle formation (NPF) event by all 11 instruments and the 3 reference instruments. To our knowledge, it is the first time that the size distribution of ions and particles is measured by so many ion spectrometers during a NPF event. The new particle formation rates (~0.2 cm−3 s−1 for ions and ~2 cm−3 s−1 for particles) and growth rates (~25 nm h−1 in the 3–7 nm size range) were calculated for all the instruments. The NAISs and the ANAIS gave higher concentrations and formation rates than the AISs. For example, the AISs agreed with the BSMA within 11 % and 28 % for negative and positive ion concentration respectively, whereas the NAISs agreed within 23 % and 29 %. Finally, based on the results presented here, we give guidelines for data evaluation, when data from different individual ion spectrometers are compared.
- ItemExperimental investigation of ion-ion recombination under atmospheric conditions(München : European Geopyhsical Union, 2015) Franchin, A.; Ehrhart, S.; Leppä, J.; Nieminen, T.; Gagné, S.; Schobesberger, S.; Wimmer, D.; Duplissy, J.; Riccobono, F.; Dunne, E.M.; Rondo, L.; Downard, A.; Bianchi, F.; Kupc, A.; Tsagkogeorgas, G.; Lehtipalo, K.; Manninen, H.E.; Almeida, J.; Amorim, A.; Wagner, P.E.; Hansel, A.; Kirkby, J.; Le Rille, O.; Kürten, A.; Donahue, N.M.; Makhmutov, V.; Mathot, S.; Metzger, A.; Petäjä, T.; Schnitzhofer, R.; Sipilä, M.; Stozhkov, Y.; Tomé, A.; Kerminen, V.-M.; Carslaw, K.; Curtius, J.; Baltensperger, U.; Kulmala, M.We present the results of laboratory measurements of the ion–ion recombination coefficient at different temperatures, relative humidities and concentrations of ozone and sulfur dioxide. The experiments were carried out using the Cosmics Leaving OUtdoor Droplets (CLOUD) chamber at CERN, the walls of which are made of conductive material, making it possible to measure small ions. We produced ions in the chamber using a 3.5 GeV c−1 beam of positively charged pions (π+) generated by the CERN Proton Synchrotron (PS). When the PS was switched off, galactic cosmic rays were the only ionization source in the chamber. The range of the ion production rate varied from 2 to 100 cm−3 s−1, covering the typical range of ionization throughout the troposphere. The temperature ranged from −55 to 20 °C, the relative humidity (RH) from 0 to 70 %, the SO2 concentration from 0 to 40 ppb, and the ozone concentration from 200 to 700 ppb. The best agreement of the retrieved ion–ion recombination coefficient with the commonly used literature value of 1.6 × 10−6 cm3 s−1 was found at a temperature of 5 °C and a RH of 40 % (1.5 ± 0.6) × 10−6 cm3 s−1. At 20 °C and 40 % RH, the retrieved ion–ion recombination coefficient was instead (2.3 ± 0.7) × 10−6 cm3 s−1. We observed no dependency of the ion–ion recombination coefficient on ozone concentration and a weak variation with sulfur dioxide concentration. However, we observed a more than fourfold increase in the ion–ion recombination coefficient with decreasing temperature. We compared our results with three different models and found an overall agreement for temperatures above 0 °C, but a disagreement at lower temperatures. We observed a strong increase in the recombination coefficient for decreasing relative humidities, which has not been reported previously.
- ItemAccessing heavy allyl-analogous [(TerN)2E]− (E = Sb, Bi) ions and their reactivity towards ECl3(Cambridge : Soc., 2015) Hinz, Alexander; Schulz, Axel; Villinger, AlexanderThe attempted preparation of the biradicaloid [E(μ-NTer)]2 (E = Sb, Bi) yielded salts of the anion [(TerN)2E]−. These heteroatom allyl analogues could be further utilized in the reaction with pnictogen(III) chlorides to form the first 1,3-dichloro-1-bisma-3-stiba-2,4-diazane [ClSb(μ-NTer)2BiCl].
- ItemUltracompact three-dimensional tubular conductivity microsensors for ionic and biosensing applications(Washington, DC : American Chemical Society, 2014) Martinez-Cisneros, C.S.; Sanchez, S.; Xi, W.; Schmidt, O.G.We present ultracompact three-dimensional tubular structures integrating Au-based electrodes as impedimetric microsensors for the in-flow determination of mono- and divalent ionic species and HeLa cells. The microsensors show an improved performance of 2 orders of magnitude (limit of detection = 0.1 nM for KCl) compared to conventional planar conductivity detection systems integrated in microfluidic platforms and the capability to detect single HeLa cells in flowing phosphate buffered saline. These highly integrated conductivity tubular sensors thus open new possibilities for lab-in-a-tube devices for bioapplications such as biosensing and bioelectronics.
- ItemSingle molecule magnet with an unpaired electron trapped between two lanthanide ions inside a fullerene(London : Nature Publishing Group, 2017) Liu, F.; Krylov, D.S.; Spree, L.; Avdoshenko, S.M.; Samoylova, N.A.; Rosenkranz, M.; Kostanyan, A.; Greber, T.; Wolter, A.U.B.; Büchner, B.; Popov, A.A.Increasing the temperature at which molecules behave as single-molecule magnets is a serious challenge in molecular magnetism. One of the ways to address this problem is to create the molecules with strongly coupled lanthanide ions. In this work, endohedral metallofullerenes Y 2 @C 80 and Dy 2 @C 80 are obtained in the form of air-stable benzyl monoadducts. Both feature an unpaired electron trapped between metal ions, thus forming a single-electron metal-metal bond. Giant exchange interactions between lanthanide ions and the unpaired electron result in single-molecule magnetism of Dy 2 @C 80 (CH 2 Ph) with a record-high 100 s blocking temperature of 18 K. All magnetic moments in Dy 2 @C 80 (CH 2 Ph) are parallel and couple ferromagnetically to form a single spin unit of 21 μ B with a dysprosium-electron exchange constant of 32 cm -1. The barrier of the magnetization reversal of 613 K is assigned to the state in which the spin of one Dy centre is flipped.
- ItemIon dynamics in electron beam-plasma interaction: Particle-in-cell simulations(Göttingen : Copernicus, 2014) Baumgärtel, K.Electron beam-plasma interaction including ions is studied by particle-in-cell (PIC) simulations using a one-dimensional, electrostatic code. Evidence for Langmuir wave decay is given for sufficiently energetic beams, as in previous Vlasov-Maxwell simulations. The mechanism for the generation of localized finite-amplitude ion density fluctuations is analyzed. Amplitude modulation due to interference between the beam-generated Langmuir waves causes random wave localization including strong transient spikes in field intensity which create bursty ion density structures via ponderomotive forces. More dense beams may quench the decay instability and generate low-frequency variations dominated by the wave number of the fastest growing Langmuir mode.
- ItemRocket measurements of positive ions during polar mesosphere winter echo conditions(München : European Geopyhsical Union, 2006) Brattli, A.; Blix, T.A.; Lie-Svendsen, Ø.; Hoppe, U.-P.; Lübken, F.-J.; Rapp, M.; Singer, W.; Latteck, R.; Friedrich, M.On 18 January 2005, two small, instrumented rockets were launched from Andøya Rocket Range (69.3° N, 16° E) during conditions with Polar Mesosphere Winter Echoes (PMWE). Each of the rockets was equipped with a Positive Ion Probe (PIP) and a Faraday rotation/differential absorption experiment, and was launched as part of a salvo of meteorological rockets measuring temperature and wind using falling spheres and chaff. Layers of PMWE were detected between 55 and 77 km by the 53.5 MHz ALWIN radar. The rockets were launched during a solar proton event, and measured extremely high ion densities, of order 1010 m−3, in the region where PMWE were observed. The density measurements were analyzed with the wavelet transform technique. At large length scales, ~103 m, the power spectral density can be fitted with a k−3 wave number dependence, consistent with saturated gravity waves. Outside the PMWE layers the k−3 spectrum extends down to approximately 102 m where the fluctuations are quickly damped and disappear into the instrumental noise. Inside the PMWE layers the spectrum at smaller length scales is well fitted with a k−5/3 dependence over two decades of scales. The PMWE are therefore clearly indicative of turbulence, and the data are consistent with the turbulent dissipation of breaking gravity waves. We estimate a lower limit for the turbulent energy dissipation rate of about 10−2 W/kg in the upper (72 km) layer.
- ItemVariability of air ion concentrations in urban Paris(München : European Geopyhsical Union, 2015) Dos Santos, V.N.; Herrmann, E.; Manninen, H.E.; Hussein, T.; Hakala, J.; Nieminen, T.; Aalto, P.P.; Merkel, M.; Wiedensohler, A.; Kulmala, M.; Petäjä, T.; Hämeri, K.Air ion concentrations influence new particle formation and consequently the global aerosol as potential cloud condensation nuclei. We aimed to evaluate air ion concentrations and characteristics of new particle formation events (NPF) in the megacity of Paris, France, within the MEGAPOLI (Megacities: Emissions, urban, regional and Global Atmospheric Pollution and climate effects, and Integrated tools for assessment and mitigation) project. We measured air ion number size distributions (0.8–42 nm) with an air ion spectrometer and fine particle number concentrations (> 6 nm) with a twin differential mobility particle sizer in an urban site of Paris between 26 June 2009 and 4 October 2010. Air ions were size classified as small (0.8–2 nm), intermediate (2–7 nm), and large (7–20 nm). The median concentrations of small and large ions were 670 and 680 cm−3, respectively, (sum of positive and negative polarities), whereas the median concentration of intermediate ions was only 20 cm−3, as these ions were mostly present during new particle formation bursts, i.e. when gas-to-particle conversion produced fresh aerosol particles from gas phase precursors. During peaks in traffic-related particle number, the concentrations of small and intermediate ions decreased, whereas the concentrations of large ions increased. Seasonal variations affected the ion population differently, with respect to their size and polarity. NPF was observed in 13 % of the days, being most frequent in spring and late summer (April, May, July, and August). The results also suggest that NPF was favoured on the weekends in comparison to workdays, likely due to the lower levels of condensation sinks in the mornings of weekends (CS weekdays 09:00: 18 × 10−3 s−1; CS weekend 09:00: 8 × 10−3 s−1). The median growth rates (GR) of ions during the NPF events varied between 3 and 7 nm h−1, increasing with the ion size and being higher on workdays than on weekends for intermediate and large ions. The median GR of small ions on the other hand were rather similar on workdays and weekends. In general, NPF bursts changed the diurnal cycle of particle number as well as intermediate and large ions by causing an extra peak between 09:00 and 14:00. On average, during the NPF bursts the concentrations of intermediate ions were 8.5–10 times higher than on NPF non-event days, depending on the polarity, and the concentrations of large ions and particles were 1.5–1.8 and 1.2 times higher, respectively. Because the median concentrations of intermediate ions were considerably higher on NPF event days in comparison to NPF non-event days, the results indicate that intermediate ion concentrations could be used as an indication for NPF in Paris. The results suggest that NPF was a source of ions and aerosol particles in Paris and therefore contributed to both air quality degradation and climatic effects, especially in the spring and summer.
- ItemChemical composition of cloud water in the puerto rican tropical trade wind cumuli(Dordrecht : Springer, 2009) Gioda, A.; Mayol-Bracero, O.L.; Morales-García, F.; Collett, J.; Decesari, S.; Emblico, L.; Facchini, M.C.; Morales-De Jesús, R.J.; Mertes, S.; Borrmann, S.; Walter, S.; Schneider, J.As part of the Rain In Cumulus over the Ocean Experiment (RICO) and the Puerto Rico Aerosol and Cloud Study (PRACS), cloud water was collected at East Peak (EP) in Puerto Rico. The main objective of this study was to determine the concentrations of water-soluble species (Cl-, NO3 -, SO4 2-, NH4 +, Ca 2+, H+, Mg2+, K+, and Na +) in water samples taken from clouds influenced by tropical trade winds. The most abundant inorganic species were Na+ (average 465 μeq l-1) and Cl- (434 μeq l-1), followed by Mg2+ (105 μeq l-1), SO4 2- (61 μeq l-1), and NO3 - (25 μeq l -1). High concentrations of nss-SO4 2 (28 μeq l-1), NO3 - (86 μeq l-1), and H+ (14.5 μeq l-1) were measured with a shift in air masses origin from the North Atlantic to North American continent, which reflected a strong anthropogenic influence on cloud chemistry at EP. Long-range transport of particles and acid gases seems to be the factor responsible for fluctuations in concentrations and pH of cloud water at East Peak. When under trade wind influences the liquid phase concentrations of all inorganic substances were similar to those found in clouds in other clean maritime environments. © 2008 Springer Science+Business Media B.V.