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  • Attoui, Michel; Kangasluoma, Juha (2019)
    Tetraheptylammonium bromide (THABr), tetrabutylammonium bromide (TBABr) and tetraethylammonium bromide (TEABr) dissolved in methanol or water methanol mixtures (similar to 1 mM) produce via positive electrospray atomization and high resolution classification electrical classification standard clean ions (monomer and dier) which are singly charged. THABr is hydrophobic and insoluble in water, TBABr and TEABr are hygroscopic and water soluble (0.6 and 2.8 kg/L respectively). These ions are used to study the effect of hygroscopicity on the activation of aerosol particles in the sub 2 nm range via the detection efficiency measurement of a boosted ultrafine TSI condensation particle counter (3025A). Water solubility of particles seems to play a role in the activation and growth with butanol vapor in the CPC (condensation particle counter) independently of the size.
  • Kangasluoma, Juha; Hering, Susanne; Picard, David; Lewis, Gregory; Enroth, Joonas; Korhonen, Frans; Kulmala, Markku; Sellegri, Karine; Attoui, Michel; Petäjä, Tuukka (2017)
    In this study we characterized the performance of three new particle counters able to detect particles smaller than 3 nm during the Helsinki condensation particle counter (CPC) workshop in summer 2016: the Aerosol Dynamics Inc. (ADI; Berkeley, USA) versatile water condensation particle counter (vWCPC), TSI 3777 nano enhancer (TSI Inc., Shoreview, USA) and modified and boosted TSI 3010-type CPC from Universite Blaise Pascal called a B3010. The performance of all CPCs was first measured with charged tungsten oxide test particles at temperature settings which resulted in supersaturation low enough to not detect any ions produced by a radioactive source. Due to similar measured detection efficiencies, additional comparison between the 3777 and vWCPC were conducted using electrically neutral tungsten oxide test particles and with positively charged tetradodecylammonium bromide. Furthermore, the detection efficiencies of the 3777 and vWCPC were measured with boosted temperature settings yielding supersaturation which was at the onset of homogeneous nucleation for the 3777 or confined within the range of liquid water for the ADI vWCPC. Finally, CPC-specific tests were conducted to probe the response of the 3777 to various inlet flow relative humidities, of the B3010 to various inlet flow rates and of the vWCPC to various particle concentrations. For the 3777 and vWCPC the measured 50% detection diameters (d50s) were in the range of 1.3-2.4 nm for the tungsten oxide particles, depending on the particle charging state and CPC temperature settings, between 2.5 and 3.3 nm for the organic test aerosol, and in the range of 3.2-3.4 nm for tungsten oxide for the B3010.
  • Kangasluoma, J.; Kontkanen, J. (2017)
    The number of experiments characterizing sub-3 nm aerosol particle dynamics has increased significantly over the recent years. In these experiments, it is essential to know/determine size resolved particle number concentrations accurately. Despite particle concentration measurement being relatively simple experiment, it can contain large uncertainties from various sources in the sub-3 nm size range. In this study we aim to identify and examine some of these sources. We simulated four different condensation particle counters (CPCs) (TSI 3777, ADI vWCPC, Airmodus A11 and an ideal CPC with d50 (lowest detection threshold) of 1.5 nm) and one differential mobility analyzer (DMA) (TSI nano DMA) and study the resulting uncertainties when using them to measure three different particle size distributions. First, we show that Poisson counting uncertainty root N represents the standard deviation, sigma, of the number of counted particles in all CPC and DMPS counting experiments. Second, the state-of-the-art DMA-CPC particle sizing system is examined with respect to counting statistics. Third, the performance of the instruments is assumed to be well-known, and instrumental non-idealities and the inversion routine are assessed. Fourth,+/- 0.5 nm offset is inserted to the CPC d50, and its effect on the measured particle concentration is examined. Our results highlight the importance of knowing the CPC d50 accurately to narrow down the particle concentration uncertainty. Furthermore, the results show that the current DMA-CPC measurements are subject to considerable counting uncertainty in low particle concentration environments. Based on the analysis we summarize suggestions for further research and instrumental development for more accurate sub-3 nm particle concentration measurements in the future.
  • Kangasluoma, Juha; Cai, Runlong; Jiang, Jingkun; Deng, Chenjuan; Stolzenburg, Dominik; Ahonen, Lauri R.; Chan, Tommy; Fu, Yueyun; Kim, Changhyuk; Laurila, Tiia M.; Zhou, Ying; Dada, Lubna; Sulo, Juha; Flagan, Richard C.; Kulmala, Markku; Petaja, Tuukka; Lehtipalo, Katrianne (2020)
    Interest in understanding gas-to-particle phase transformation in several disciplines such as at-mospheric sciences, material synthesis, and combustion has led to the development of several distinct instruments that can measure the particle size distributions down to the sizes of large molecules and molecular clusters, at which the initial particle formation and growth takes place. These instruments, which include the condensation particle counter battery, a variety of electrical mobility spectrometers and the particle size magnifier, have been usually characterized in lab-oratory experiments using carefully prepared calibration aerosols. They are then applied, alone or in combination, to study the gas-to-particle transition in experiments that produce particles with a wide range of compositions and other properties. Only a few instrument intercomparisons in either laboratory or field conditions have been reported, raising the question: how accurately can the sub-10 nm particle number size distributions be measured with the currently available instrumentation? Here, we review previous studies in which sub-10 nm particle size distributions have been measured with at least two independent instruments. We present recent data from three sites that deploy the current state-of-the-art instrumentation: Hyytiala, Beijing, and the CLOUD chamber. After discussing the status of the sub-10 nm size distribution measurements, we present a comprehensive uncertainty analysis for these methods that suggests that our present understanding on the sources of uncertainties quite well captures the observed deviations be-tween different instruments in the size distribution measurements. Finally, based on present understanding of the characteristics of a number of systems in which gas-to-particle conversion takes place, and of the instrumental limitations, we suggest guidelines for selecting suitable in-struments for various applications.
  • Steiner, G.; Franchin, A.; Kangasluoma, J.; Kerminen, V. -M.; Kulmala, M.; Petäjä, T. (2017)
    Measuring aerosols and molecular clusters below the 3 nm size limit is essential to increase our understanding of new particle formation. Instruments for the detection of sub-3 nm aerosols and clusters exist and need to be carefully calibrated and characterized. So far calibrations and laboratory tests have been carried out using mainly electrically charged aerosols, as they are easier to handle experimentally. However, the charging state of the cluster is an important variable to take into account. Furthermore, instrument characterization performed with charged aerosols could be biased, preventing a correct interpretation of data when electrically neutral sub-3 nm aerosols are involved. This article presents the first steps to generate electrically neutral molecular clusters as standards for calibration. We show two methods: One based on the neutralization of well-known molecular clusters (mobility standards) by ions generated in a switchable aerosol neutralizer. The second is based on the controlled neutralization of mobility standards with mobility standards of opposite polarity in a recombination cell. We highlight the challenges of these two techniques and, where possible, point out solutions. In addition, we give an outlook on the next steps toward generating well-defined neutral molecular clusters with a known chemical composition and concentration.
  • Kangasluoma, Juha; Attoui, Michael (2019)
    This review discusses the developments in aerosol instrumentation that have led to the current vapor condensation based instruments capable of detecting sub-3 nm particles. We begin from selected reports prior to the year 1991, which have advanced the technology or understanding in condensation particle counting toward sub-3 nm sizes, and continue to more in depth review of the past efforts after 1991. We discuss how the developments in the calibration methods have progressed the development of particle counting techniques, and review briefly the sub-3 nm calibration experiments and cluster production methods used in calibration experiments. Based on these reviews, we identify several technological and scientific advances for the future to improve the accuracy, understanding, and technology of sub-3 nm particle counting. Copyright (c) 2019 American Association for Aerosol Research
  • Wagner, Robert; Yan, Chao; Lehtipalo, Katrianne; Duplissy, Jonathan; Nieminen, Tuomo; Kangasluoma, Juha; Ahonen, Lauri R.; Dada, Lubna; Kontkanen, Jenni; Manninen, Hanna E.; Dias, Antonio; Amorim, Antonio; Bauer, Paulus S.; Bergen, Anton; Bernhammer, Anne-Kathrin; Bianchi, Federico; Brilke, Sophia; Mazon, Stephany Buenrostro; Chen, Xuemeng; Draper, Danielle C.; Fischer, Lukas; Frege, Carla; Fuchs, Claudia; Garmash, Olga; Gordon, Hamish; Hakala, Jani; Heikkinen, Liine; Heinritzi, Martin; Hofbauer, Victoria; Hoyle, Christopher R.; Kirkby, Jasper; Kurten, Andreas; Kvashnin, Alexander N.; Laurila, Tiia; Lawler, Michael J.; Mai, Huajun; Makhmutov, Vladimir; Mauldin III, Roy L.; Molteni, Ugo; Nichman, Leonid; Nie, Wei; Ojdanic, Andrea; Onnela, Antti; Piel, Felix; Quelever, Lauriane L. J.; Rissanen, Matti P.; Sarnela, Nina; Schallhart, Simon; Sengupta, Kamalika; Simon, Mario; Stolzenburg, Dominik; Stozhkov, Yuri; Trostl, Jasmin; Viisanen, Yrjö; Vogel, Alexander L.; Wagner, Andrea C.; Xiao, Mao; Ye, Penglin; Baltensperger, Urs; Curtius, Joachim; Donahue, Neil M.; Flagan, Richard C.; Gallagher, Martin; Hansel, Armin; Smith, James N.; Tome, Antonio; Winkler, Paul M.; Worsnop, Douglas; Ehn, Mikael; Sipilä, Mikko; Kerminen, Veli-Matti; Petäjä, Tuukka; Kulmala, Markku (2017)
    The formation of secondary particles in the atmosphere accounts for more than half of global cloud condensation nuclei. Experiments at the CERN CLOUD (Cosmics Leaving OUtdoor Droplets) chamber have underlined the importance of ions for new particle formation, but quantifying their effect in the atmosphere remains challenging. By using a novel instrument setup consisting of two nanoparticle counters, one of them equipped with an ion filter, we were able to further investigate the ion-related mechanisms of new particle formation. In autumn 2015, we carried out experiments at CLOUD on four systems of different chemical compositions involving monoterpenes, sulfuric acid, nitrogen oxides, and ammonia. We measured the influence of ions on the nucleation rates under precisely controlled and atmospherically relevant conditions. Our results indicate that ions enhance the nucleation process when the charge is necessary to stabilize newly formed clusters, i.e., in conditions in which neutral clusters are unstable. For charged clusters that were formed by ion-induced nucleation, we were able to measure, for the first time, their progressive neutralization due to recombination with oppositely charged ions. A large fraction of the clusters carried a charge at 1.5 nm diameter. However, depending on particle growth rates and ion concentrations, charged clusters were largely neutralized by ion-ion recombination before they grew to 2.5 nm. At this size, more than 90% of particles were neutral. In other words, particles may originate from ion-induced nucleation, although they are neutral upon detection at diameters larger than 2.5 nm. Observations at Hyytiala, Finland, showed lower ion concentrations and a lower contribution of ion-induced nucleation than measured at CLOUD under similar conditions. Although this can be partly explained by the observation that ion-induced fractions decrease towards lower ion concentrations, further investigations are needed to resolve the origin of the discrepancy.