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2. Size-dependent influence of NOx on the growth rates of organic aerosol particles

Author

Yan, C, Nie, W, Vogel, AL, Dada, L, Lehtipalo, K, Stolzenburg, D, Wagner, R, Rissanen, MP, Xiao, M, Ahonen, L, Fischer, L, Rose, C, Bianchi, F, Gordon, H, Simon, M, Heinritzi, M, Garmash, O, Roldin, P, Dias, A, Ye, P, Hofbauer, V, Amorim, A, Bauer, PS, Bergen, A, Bernhammer, A-K, Breitenlechner, M, Brilke, S, Buchholz, A, Mazon, S Buenrostro, Canagaratna, MR, Chen, X, Ding, A, Dommen, J, Draper, DC, Duplissy, J, Frege, C, Heyn, C, Guida, R, Hakala, J, Heikkinen, L, Hoyle, CR, Jokinen, T, Kangasluoma, J, Kirkby, J, Kontkanen, J, Kürten, A, Lawler, MJ, Mai, H, Mathot, S, Mauldin, RL, Molteni, U, Nichman, L, Nieminen, T, Nowak, J, Ojdanic, A, Onnela, A, Pajunoja, A, Petäjä, T, Piel, F, Quéléver, LLJ, Sarnela, N, Schallhart, S, Sengupta, K, Sipilä, M, Tomé, A, Tröstl, J, Väisänen, O, Wagner, AC, Ylisirniö, A, Zha, Q, Baltensperger, U, Carslaw, KS, Curtius, J, Flagan, RC, Hansel, A, Riipinen, I, Smith, JN, Virtanen, A, Winkler, PM, Donahue, NM, Kerminen, V-M, Kulmala, M, Ehn, M, and Worsnop, DR

Subjects
Climate Action
Abstract

Atmospheric new-particle formation (NPF) affects climate by contributing to a large fraction of the cloud condensation nuclei (CCN). Highly oxygenated organic molecules (HOMs) drive the early particle growth and therefore substantially influence the survival of newly formed particles to CCN. Nitrogen oxide (NOx) is known to suppress the NPF driven by HOMs, but the underlying mechanism remains largely unclear. Here, we examine the response of particle growth to the changes of HOM formation caused by NOx. We show that NOx suppresses particle growth in general, but the suppression is rather nonuniform and size dependent, which can be quantitatively explained by the shifted HOM volatility after adding NOx. By illustrating how NOx affects the early growth of new particles, a critical step of CCN formation, our results help provide a refined assessment of the potential climatic effects caused by the diverse changes of NOx level in forest regions around the globe.

Published
2020

4. Biogenic particles formed in the Himalaya as an important source of free tropospheric aerosols

Author

Bianchi, F., Junninen, H., Bigi, A., Sinclair, V. A., Dada, L., Hoyle, C. R., Zha, Q., Yao, L., Ahonen, L. R., Bonasoni, P., Buenrostro Mazon, S., Hutterli, M., Laj, P., Lehtipalo, K., Kangasluoma, J., Kerminen, V.-M., Kontkanen, J., Marinoni, A., Mirme, S., Molteni, U., Petäjä, T., Riva, M., Rose, C., Sellegri, K., Yan, C., Worsnop, D. R., Kulmala, M., Baltensperger, U., and Dommen, J.

Published
2021
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5. Effect of dimethylamine on the gas phase sulfuric acid concentration measured by Chemical Ionization Mass Spectrometry

Author

Rondo, L, Ehrhart, S, Kürten, A, Adamov, A, Bianchi, F, Breitenlechner, M, Duplissy, J, Franchin, A, Dommen, J, Donahue, NM, Dunne, EM, Flagan, RC, Hakala, J, Hansel, A, Keskinen, H, Kim, J, Jokinen, T, Lehtipalo, K, Leiminger, M, Praplan, A, Riccobono, F, Rissanen, MP, Sarnela, N, Schobesberger, S, Simon, M, Sipilä, M, Smith, JN, Tomé, A, Tröstl, J, Tsagkogeorgas, G, Vaattovaara, P, Winkler, PM, Williamson, C, Wimmer, D, Baltensperger, U, Kirkby, J, Kulmala, M, Petäjä, T, Worsnop, DR, and Curtius, J

Subjects
Earth Sciences, Atmospheric Sciences, CLOUD experiment, nucleation, Chemical Ionization-Atmospheric Pressure interface-Time Of Flight Mass Spectrometer, Chemical Ionization‐Atmospheric Pressure interface‐Time Of Flight Mass Spectrometer, Physical Geography and Environmental Geoscience, Atmospheric sciences, Climate change science
Abstract

Sulfuric acid is widely recognized as a very important substance driving atmospheric aerosol nucleation. Based on quantum chemical calculations it has been suggested that the quantitative detection of gas phase sulfuric acid (H2SO4) by use of Chemical Ionization Mass Spectrometry (CIMS) could be biased in the presence of gas phase amines such as dimethylamine (DMA). An experiment (CLOUD7 campaign) was set up at the CLOUD (Cosmics Leaving OUtdoor Droplets) chamber to investigate the quantitative detection of H2SO4 in the presence of dimethylamine by CIMS at atmospherically relevant concentrations. For the first time in the CLOUD experiment, the monomer sulfuric acid concentration was measured by a CIMS and by two CI-APi-TOF (Chemical Ionization-Atmospheric Pressure interface-Time Of Flight) mass spectrometers. In addition, neutral sulfuric acid clusters were measured with the CI-APi-TOFs. The CLOUD7 measurements show that in the presence of dimethylamine (

Published
2016

8. The standard operating procedure for Airmodus Particle Size Magnifier and nano-Condensation Nucleus Counter

Author

Lehtipalo, K., primary, Ahonen, L.R., additional, Baalbaki, R., additional, Sulo, J., additional, Chan, T., additional, Laurila, T., additional, Dada, L., additional, Duplissy, J., additional, Miettinen, E., additional, Vanhanen, J., additional, Kangasluoma, J., additional, Kulmala, M., additional, Petäjä, T., additional, and Jokinen, T., additional

Published
2022
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9. Biogenic particles formed in the Himalaya as an important source of free tropospheric aerosols

Author

Bianchi, F., Junninen, H., Bigi, A., Sinclair, V., Dada, L., Hoyle, C., Zha, Q., Yao, L., Ahonen, L., Bonasoni, P., Buenrostro Mazon, S., Hutterli, M., Laj, P., Lehtipalo, K., Kangasluoma, J., Kerminen, V.-M., Kontkanen, J., Marinoni, A., Mirme, S., Molteni, U., Petäjä, T., Riva, M., Rose, Clémence, Sellegri, K., Yan, C., Worsnop, D., Kulmala, M., Baltensperger, U., Dommen, J., Institute for Atmospheric and Earth System Research (INAR), Helsingin yliopisto = Helsingfors universitet = University of Helsinki, University of Modena and Reggio Emilia, Laboratory of Atmospheric Chemistry [Paul Scherrer Institute] (LAC), Paul Scherrer Institute (PSI), CNR Institute of Atmospheric Sciences and Climate (ISAC), National Research Council of Italy | Consiglio Nazionale delle Ricerche (CNR), Tofwerk AG, Institut des Géosciences de l’Environnement (IGE), Institut de Recherche pour le Développement (IRD)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), Finnish Meteorological Institute (FMI), University of Tartu, IRCELYON-Catalytic and Atmospheric Reactivity for the Environment (CARE), Institut de recherches sur la catalyse et l'environnement de Lyon (IRCELYON), Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Météorologie Physique (LaMP), Institut national des sciences de l'Univers (INSU - CNRS)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Centre National de la Recherche Scientifique (CNRS), Aerodyne Research Inc., Beijing University of Chemical Technology, University of Helsinki, Consiglio Nazionale delle Ricerche (CNR), Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Institut de Recherche pour le Développement (IRD)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Polar and arctic atmospheric research (PANDA), INAR Physics, Air quality research group, and Global Atmosphere-Earth surface feedbacks

Subjects
[PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, respiratory system, [SDU.STU.ME]Sciences of the Universe [physics]/Earth Sciences/Meteorology, 114 Physical sciences, complex mixtures
Abstract

Aerosols of biogenic and anthropogenic origin affect the total radiative forcing of global climate. Poor knowledge of the pre-industrial aerosol concentration and composition, in particular of particles formed directly in the atmosphere from gaseous precursors, constitutes a large uncertainty in the anthropogenic radiative forcing. Investigations of new particle formation at pre-industrial-like conditions can contribute to the reduction of this uncertainty. Here we present observations taken at the remote Nepal Climate Observatory Pyramid station at 5,079 m above sea level, a few kilometres from the summit of Everest. We show that up-valley winds funnel gaseous aerosol precursors to higher altitudes. During this transport, these are oxidized into compounds of very low volatility, which rapidly form a large number of aerosol particles. These are then transported into the free troposphere, which suggests that the whole Himalayan region may act as an 'aerosol factory' and contribute substantially to the free tropospheric aerosol population. Aerosol production in this region occurs mainly via organic precursors of biogenic origin with little evidence of the involvement of anthropogenic pollutants. This process is therefore likely to be essentially unchanged since the pre-industrial period, and may have been one of the major sources that contributes to the upper tropospheric aerosol population during that time. Newly formed biogenic particles in the Himalaya increase free-tropospheric background aerosol concentration by a factor of up to two.

Published
2020

10. Size-dependent influence of NOₓ on the growth rates of organic aerosol particles

Author

Yan, C., Nie, W., Vogel, A. L., Dada, L., Lehtipalo, K., Stolzenburg, D., Wagner, R., Rissanen, M. P., Xiao, M., Ahonen, L., Fischer, L., Rose, C., Bianchi, F., Gordon, H., Simon, M., Heinritzi, M., Garmash, O., Roldin, P., Dias, A., Ye, P., Hofbauer, V., Amorim, A., Bauer, P. S., Bergen, A., Bernhammer, A.-K., Breitenlechner, M., Brilke, S., Buchholz, A., Buenrostro Mazon, S., Canagaratna, M. R., Chen, X., Ding, A., Dommen, J., Draper, D. C., Duplissy, J., Frege, C., Heyn, C., Guida, R., Hakala, J., Heikkinen, L., Hoyle, C. R., Jokinen, T., Kangasluoma, J., Kirkby, J., Kontkanen, J., Kürten, A., Lawler, M. J., Mai, H., Mathot, S., Mauldin, R. L., III, Molteni, U., Nichman, L., Nieminen, T., Nowak, J., Ojdanic, A., Onnela, A., Pajunoja, A., Petäjä, T., Piel, F., Quéléver, L. L. J., Sarnela, N., Schallhart, S., Sengupta, K., Sipilä, M., Tomé, A., Tröst, J., Väisänen, O., Wagner, A. C., Ylisirniö, A., Zha, Q., Baltensperger, U., Carslaw, K. S., Curtius, J., Flagan, R. C., Hansel, A., Riipinen, I., Smith, J. N., Virtanen, A., Winkler, P. M., Donahue, N. M., Kerminen, V.-M., Kulmala, M., Ehn, M., and Worsnop, D. R.

Abstract

Atmospheric new-particle formation (NPF) affects climate by contributing to a large fraction of the cloud condensation nuclei (CCN). Highly oxygenated organic molecules (HOMs) drive the early particle growth and therefore substantially influence the survival of newly formed particles to CCN. Nitrogen oxide (NOₓ) is known to suppress the NPF driven by HOMs, but the underlying mechanism remains largely unclear. Here, we examine the response of particle growth to the changes of HOM formation caused by NOₓ. We show that NOₓ suppresses particle growth in general, but the suppression is rather nonuniform and size dependent, which can be quantitatively explained by the shifted HOM volatility after adding NOₓ. By illustrating how NOₓ affects the early growth of new particles, a critical step of CCN formation, our results help provide a refined assessment of the potential climatic effects caused by the diverse changes of NOₓ level in forest regions around the globe.

Published
2020

11. The role of ions in new particle formation in the CLOUD chamber

Author

Wagner, R., Yan, C., Lehtipalo, K., Duplissy, J., Nieminen, T., Kangasluoma, J., Ahonen, L. R., Dada, L., Kontkanen, J., Manninen, H. E., Dias, A., Amorim, A., Bauer, P. S., Bergen, A., Bernhammer, A.-K., Bianchi, F., Brilke, S., Mazon, S. B., Chen, X., Draper, D. C., Fischer, L., Frege, C., Fuchs, C., Garmash, O., Gordon, H., Hakala, J., Heikkinen, L., Heinritzi, M., Hofbauer, V., Hoyle, C. R., Kirkby, J., Kürten, A., Kvashnin, A. N., Laurila, T., Lawler, M. J., Mai, H., Makhmutov, V., Mauldin III, R. L., Molteni, U., Nichman, L., Nie, W., Ojdanic, A., Onnela, A., Piel, F., Quéléver, L. L. J., Rissanen, M. P., Sarnela, N., Schallhart, S., Sengupta, K., Simon, M., Stolzenburg, D., Stozhkov, Y., Tröstl, J., Viisanen, Y., Vogel, A. L., Wagner, A. C., Xiao, M., Ye, P., Baltensperger, U., Curtius, J., Donahue, N. M., Flagan, R. C., Gallagher, M., Hansel, A., Smith, J. N., Tomé, A., Winkler, P. M., Worsnop, D., Ehn, M., Sipilä, M., Kerminen, V.-M., Petäjä, T., Kulmala, M., Department of Physics, Helsinki Institute of Physics, Polar and arctic atmospheric research (PANDA), University of Helsinki, University of Eastern Finland, CERN, University of Lisbon, University of Vienna, Goethe University Frankfurt, University of Innsbruck, University of California Irvine, Paul Scherrer Institute, Department of Applied Physics, Carnegie Mellon University, RAS - P.N. Lebedev Physics Institute, California Institute of Technology, University of Manchester, University of Leeds, Finnish Meteorological Institute, Aalto-yliopisto, Aalto University, and Department of Applied Physics, activities

Subjects
Atmospheric Science, 010504 meteorology & atmospheric sciences, Nucleation, Analytical chemistry, Nanoparticle, ATMOSPHERIC AEROSOL NUCLEATION, Cosmic ray, 010501 environmental sciences, 114 Physical sciences, 01 natural sciences, Ion, Atmosphere, lcsh:Chemistry, chemistry.chemical_compound, SULFURIC-ACID, HETEROGENEOUS NUCLEATION, ddc:550, Cloud condensation nuclei, Nuclear Physics - Experiment, ResearchInstitutes_Networks_Beacons/MERI, BOREAL-FOREST, 0105 earth and related environmental sciences, FREE TROPOSPHERE, GROWTH-RATES, Chemistry, MOLECULAR CLUSTERS, Sulfuric acid, Manchester Environmental Research Institute, lcsh:QC1-999, SIZE MAGNIFIER, lcsh:QD1-999, 13. Climate action, Chemical physics, Particle, NEUTRAL CLUSTER, lcsh:Physics, GALACTIC COSMIC-RAYS
Abstract

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 Hyytiälä, 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., published version, peerReviewed

Published
2017

12. Size-dependent influence of NO x on the growth rates of organic aerosol particles

Author

Yan, C., primary, Nie, W., additional, Vogel, A. L., additional, Dada, L., additional, Lehtipalo, K., additional, Stolzenburg, D., additional, Wagner, R., additional, Rissanen, M. P., additional, Xiao, M., additional, Ahonen, L., additional, Fischer, L., additional, Rose, C., additional, Bianchi, F., additional, Gordon, H., additional, Simon, M., additional, Heinritzi, M., additional, Garmash, O., additional, Roldin, P., additional, Dias, A., additional, Ye, P., additional, Hofbauer, V., additional, Amorim, A., additional, Bauer, P. S., additional, Bergen, A., additional, Bernhammer, A.-K., additional, Breitenlechner, M., additional, Brilke, S., additional, Buchholz, A., additional, Mazon, S. Buenrostro, additional, Canagaratna, M. R., additional, Chen, X., additional, Ding, A., additional, Dommen, J., additional, Draper, D. C., additional, Duplissy, J., additional, Frege, C., additional, Heyn, C., additional, Guida, R., additional, Hakala, J., additional, Heikkinen, L., additional, Hoyle, C. R., additional, Jokinen, T., additional, Kangasluoma, J., additional, Kirkby, J., additional, Kontkanen, J., additional, Kürten, A., additional, Lawler, M. J., additional, Mai, H., additional, Mathot, S., additional, Mauldin, R. L., additional, Molteni, U., additional, Nichman, L., additional, Nieminen, T., additional, Nowak, J., additional, Ojdanic, A., additional, Onnela, A., additional, Pajunoja, A., additional, Petäjä, T., additional, Piel, F., additional, Quéléver, L. L. J., additional, Sarnela, N., additional, Schallhart, S., additional, Sengupta, K., additional, Sipilä, M., additional, Tomé, A., additional, Tröstl, J., additional, Väisänen, O., additional, Wagner, A. C., additional, Ylisirniö, A., additional, Zha, Q., additional, Baltensperger, U., additional, Carslaw, K. S., additional, Curtius, J., additional, Flagan, R. C., additional, Hansel, A., additional, Riipinen, I., additional, Smith, J. N., additional, Virtanen, A., additional, Winkler, P. M., additional, Donahue, N. M., additional, Kerminen, V.-M., additional, Kulmala, M., additional, Ehn, M., additional, and Worsnop, D. R., additional

Published
2020
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13. Overview of the antarctic circumnavigation expedition: Study of preindustrial-like aerosols and their climate effects (ACE-SPACE)

Author

Schmale, J, Baccarini, A, Thurnherr, I, Henning, S, Efraim, A, Regayre, L, Bolas, C, Hartmann, M, Welti, A, Lehtipalo, K, Aemisegger, F, Tatzelt, C, Landwehr, S, Modini, RL, Tummon, F, Johnson, JS, Harris, N, Schnaiter, M, Toffoli, A, Derkani, M, Bukowiecki, N, Stratmann, F, Dommen, J, Sperger, UB, Wernli, H, Rosenfeld, D, Gysel-Beer, M, Carslaw, KS, Schmale, J, Baccarini, A, Thurnherr, I, Henning, S, Efraim, A, Regayre, L, Bolas, C, Hartmann, M, Welti, A, Lehtipalo, K, Aemisegger, F, Tatzelt, C, Landwehr, S, Modini, RL, Tummon, F, Johnson, JS, Harris, N, Schnaiter, M, Toffoli, A, Derkani, M, Bukowiecki, N, Stratmann, F, Dommen, J, Sperger, UB, Wernli, H, Rosenfeld, D, Gysel-Beer, M, and Carslaw, KS

Abstract

The first results from ACE-SPACE highlight that the Southern Ocean is a region with highly heterogeneous aerosol properties. The areas around the strong westerly wind belt are characterized by significant sea spray contributions to the total particle and CCN number concentrations in the MBL. Future work will link detailed wave and wind observations to sea spray production. In the Ross and Amundsen Sea polynyas (leg 2), biogenic emissions appear to play an important role for CCN abundance. There are a number of open questions associated with this observation. First, even though this particular region was probed during a phytoplankton bloom period, it was not the only region with microbial activity but showed the clearest link to high CCN concentrations. Hence, either DMS production from dimethylsulfoniopropionate in the water and/or DMS fluxes into the atmosphere were enhanced. Second, the major pathway of how MSA is added to the particle phase remains to be identified. There are two possibilities: It can condense from the gas into the particle phase, or it can be added during cloud processing. The latter process would be consistent with the reduced efficiency of wet removal because of droplet evaporation or snowflake sublimation in the cold and dry airmasses from Antarctica. Our results also indicate that the absence of MSA-related processes in the aerosol model could explain the underestimation of CCN concentration, particularly in high aerosol-MSA regions. Given that the number of CCN influence Nd, this is an important issue to solve, especially close to the coast of Antarctica where clouds could impact the surface snow mass balance by influencing both the surface energy budget and precipitation. Further studies are planned that more closely investigate the linkages between CCN number concentrations and model simulations that take DMS emissions fluxes and particle phase MSA into account. A comparison of satellite-retrieved Nd90 and ship-based measurements of CCN s

Published
2019

14. Effect of ions on sulfuric acid-water binary particle formation: 2. Experimental data and comparison with QC-normalized classical nucleation theory

Author

Duplissy J., Merikanto J., Franchin A., Tsagkogeorgas G., Kangasluoma J., Wimmer D., Vuollekoski H., Schobesberger S., Lehtipalo K., Flagan R. C., Brus D., Donahue N. M., Vehkamäki H., Almeida J., Amorim A., Barmet P., Bianchi F., Breitenlechner M., Dunne E. M., Guida R., Henschel H., Junninen H., Kirkby J., Kürten A., and Kupc A.

Published
2016
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15. New particle formation in the sulfuric acid-dimethylamine-water system:Reevaluation of CLOUD chamber measurements and comparison to an aerosol nucleation and growth model

Author

Kürten, A., Li, C., Bianchi, F., Curtius, J., Dias, A., Donahue, N. M., Duplissy, J., Flagan, R. C., Hakala, J., Jokinen, T., Kirkby, J., Kulmala, M., Laaksonen, Ari, Lehtipalo, K., Makhmutov, V., Onnela, A., Rissanen, M. P., Simon, M., Sipilä, M., Stozhkov, Y., Tröstl, J., Ye, P., McMurry, P. H., Institute for Atmospheric and Earth System Research (INAR), and Polar and arctic atmospheric research (PANDA)

Subjects
ION-INDUCED NUCLEATION, ATMOSPHERIC PARTICLES, FREE-ENERGIES, CI-API-TOF, CHEMICAL-IONIZATION, ddc:550, BOUNDARY-LAYER, ELECTRICAL MOBILITY, 114 Physical sciences, OXIDATION-PRODUCTS, FORMATION RATES, IONIZATION MASS-SPECTROMETER
Abstract

A recent CLOUD (Cosmics Leaving OUtdoor Droplets) chamber study showed that sulfuric acid and dimethylamine produce new aerosols very efficiently, and yield particle formation rates that are compatible with boundary layer observations. These previously published new particle formation (NPF) rates are re-analyzed in the present study with an advanced method. The results show that the NPF rates at 1.7 nm are more than a factor of 10 faster than previously published due to earlier approximations in correcting particle measurements made at larger detection threshold. The revised NPF rates agree almost perfectly with calculated rates from a kinetic aerosol model at different sizes (1.7 nm and 4.3 nm mobility diameter). In addition, modeled and measured size distributions show good agreement over a wide range (up to ca. 30 nm). Furthermore, the aerosol model is modified such that evaporation rates for some clusters can be taken into account; these evaporation rates were previously published from a flow tube study. Using this model, the findings from the present study and the flow tube experiment can be brought into good agreement. This confirms that nucleation proceeds at rates that are compatible with collision-controlled (a.k.a. kinetically-controlled) new particle formation for the conditions during the CLOUD7 experiment (278 K, 38% RH, sulfuric acid concentration between 1×106 and 3×107 cm-3 and dimethylamine mixing ratio of ~40 pptv). Finally, the simulation of atmospheric new particle formation reveals that even tiny mixing ratios of dimethylamine (0.1 pptv) yield NPF rates that could explain significant boundary layer particle formation. This highlights the need for improved speciation and quantification techniques for atmospheric gas-phase amine measurements.

Published
2018

16. Causes and importance of new particle formation in the present-day and pre-industrial atmospheres

Author

Gordon, H, Kirkby, J, Baltensperger, U, Bianchi, F, Breitenlechner, M, Curtius, J, Dias, A, Dommen, J, Donahue, NM, Dunne, EM, Duplissy, J, Ehrhart, S, Flagan, RC, Frege, C, Fuchs, C, Hansel, A, Hoyle, CR, Kulmala, M, Kürten, A, Lehtipalo, K, Makhmutov, V, Molteni, U, Rissanen, MP, Stozkhov, Y, Tröstl, J, Tsagkogeorgas, G, Wagner, R, Williamson, C, Wimmer, D, Winkler, PM, Yan, C, and Carslaw, KS

Abstract

New particle formation has been estimated to produce around half of cloud-forming particles in the present-day atmosphere, via gas-to-particle conversion. Here we assess the importance of new particle formation (NPF) for both the present-day and the pre-industrial atmospheres. We use a global aerosol model with parametrisations of NPF from previously published CLOUD chamber experiments involving sulphuric acid, ammonia, organic molecules and ions. We find that NPF produces around 67% of cloud condensation nuclei at 0.2% supersaturation (CCN0.2%) at the level of low clouds in the pre-industrial atmosphere (estimated uncertainty range 45-84%) and 54% in the present day (estimated uncertainty range 38-66%). Concerning causes, we find that the importance of biogenic volatile organic compounds (BVOCs) in NPF and CCN formation is greater than previously thought. Removing BVOCs and hence all secondary organic aerosol from our model reduces low-cloud-level CCN concentrations at 0.2% supersaturation by 26% in the present-day atmosphere and 41% in the pre-industrial. Around three-quarters of this reduction is due to the tiny fraction of the oxidation products of BVOCs that have sufficiently low volatility to be involved in NPF and early growth. Furthermore, we estimate that 40% of pre-industrial CCN0.2% are formed via ion-induced NPF, compared with 27% in the present-day, although we caution that the ion-induced fraction of NPF involving BVOCs is poorly measured at present. Our model suggests that the effect of changes in cosmic ray intensity on CCN is small and unlikely to be comparable to the effect of large variations in natural primary aerosol emissions.

Published
2017

17. Effect of ions on sulfuric acid-water binary particle formation II: Experimental data and comparison with QC-normalized classical nucleation theory

Author

Duplissy, Jonathan, Merikanto, J., Franchin, A., Tsagkogeorgas, G., Kangasluoma, J., Wimmer, D., Vuollekoski, H., Schobesberger, S., Lehtipalo, K., Flagan, R.C., Brus, D., Donahue, N.M., Vehkämäki, H., Almeida, J., Amorim, A., Barmet, P., Bianchi, F., Breitenlechner, M., Dunne, E.M., Guida, R., Henschel, H., Junninen, H., Kirkby, J., Kürten, A., Kupc, A., Määttänen, Anni, Makhmutov, V., Mathot, S., Nieminen, T., Onnela, A., Praplan, A.P., Riccobono, F., Rondo, L., Steiner, G., Tome, A., Walther, H., Baltensperger, U., Carslaw, K.S., Dommen, J., Hansel, A., Petäjä, T., Sipilä, M., Stratmann, F., Vrtala, A., Wagner, P.E., Worsnop, D.R., Curtius, J., Kulmala, M., Helsinki Institute of Physics (HIP), University of Helsinki, Department of Physics [Helsinki], Falculty of Science [Helsinki], University of Helsinki-University of Helsinki, Finnish Meteorological Institute (FMI), Leibniz Institute for Tropospheric Research (TROPOS), Institute for Atmospheric and Environmental Sciences [Frankfurt/Main] (IAU), Goethe-University Frankfurt am Main, Department of Atmospheric Sciences [Seattle], University of Washington [Seattle], Departments of Environmental Science and Engineering and Chemical Engineering, California Institute of Technology (CALTECH), Center for Atmospheric Particle Studies [Pittsburgh] (CAPS), Carnegie Mellon University [Pittsburgh] (CMU), CERN Theoretical Physics Department, CERN [Genève], CENTRA-SIM, IDL-Faculdade de Ciencias da Universidade de Lisboa, Laboratory of Atmospheric Chemistry [Paul Scherrer Institute] (LAC), Paul Scherrer Institute (PSI), Department Construction, Traffic and Environment, Canton of Aargau, Institute for Atmospheric and Climate Science [Zürich] (IAC), Eidgenössische Technische Hochschule - Swiss Federal Institute of Technology [Zürich] (ETH Zürich), Institut für Ionenphysik und Angewandte Physik - Institute for Ion Physics and Applied Physics [Innsbruck], Leopold Franzens Universität Innsbruck - University of Innsbruck, School of Earth and Environment [Leeds] (SEE), University of Leeds, Aerosol Physics and Environmental Physics [Vienna], University of Vienna [Vienna], PLANETO - LATMOS, Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Solar and Cosmic Ray Research Laboratory [Moscow], P. N. Lebedev Physical Institute of the Russian Academy of Sciences [Moscow] (LPI RAS), Russian Academy of Sciences [Moscow] (RAS)-Russian Academy of Sciences [Moscow] (RAS), Helsingin yliopisto = Helsingfors universitet = University of Helsinki, and Helsingin yliopisto = Helsingfors universitet = University of Helsinki-Helsingin yliopisto = Helsingfors universitet = University of Helsinki

Subjects
[PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], binary particle formation, ion-induced nucleation, sulfuric acid, [SDU.ASTR.EP]Sciences of the Universe [physics]/Astrophysics [astro-ph]/Earth and Planetary Astrophysics [astro-ph.EP], classical nucleation theory
Abstract

International audience; We report comprehensive, demonstrably contaminant-free measurements of binary particle formation rates by sulfuric acid and water for neutral and ion-induced pathways conducted in the European Organization for Nuclear Research Cosmics Leaving Outdoor Droplets chamber. The recently developed Atmospheric Pressure interface-time of flight-mass spectrometer was used to detect contaminants in charged clusters and to identify runs free of any contaminants. Four parameters were varied to cover ambient conditions: sulfuric acid concentration (105 to 109 mol cm−3), relative humidity (11% to 58%), temperature (207 K to 299 K), and total ion concentration (0 to 6800 ions cm−3). Formation rates were directly measured with novel instruments at sizes close to the critical cluster size (mobility size of 1.3 nm to 3.2 nm). We compare our results with predictions from Classical Nucleation Theory normalized by Quantum Chemical calculation (QC-normalized CNT), which is described in a companion paper. The formation rates predicted by the QC-normalized CNT were extended from critical cluster sizes to measured sizes using the UHMA2 sectional particle microphysics model. Our results show, for the first time, good agreement between predicted and measured particle formation rates for the binary (neutral and ion-induced) sulfuric acid-water system. Formation rates increase with RH, sulfuric acid, and ion concentrations and decrease with temperature at fixed RH and sulfuric acid concentration. Under atmospheric conditions, neutral particle formation dominates at low temperatures, while ion-induced particle formation dominates at higher temperatures. The good agreement between the theory and our comprehensive data set gives confidence in using the QC-normalized CNT as a powerful tool to study neutral and ion-induced binary particle formation in atmospheric modeling.

Published
2016

19. Hygroscopicity of nanoparticles produced from homogeneous nucleation in the CLOUD experiments

Author

Kim, J., Ahlm, Lars, Yli-Juuti, T., Lawler, M., Keskinen, H., Tröstl, J., Schobesberger, S., Duplissy, J., Amorim, A., Bianchi, F., Donahue, N. M., Flagan, R. C., Hakala, J., Heinritzi, M., Jokinen, T., Kürten, A., Laaksonen, A., Lehtipalo, K., Miettinen, P., Petäjä, T., Rissanen, M. P., Rondo, L., Sengupta, K., Simon, M., Tomé, A., Williamson, C., Wimmer, D., Winkler, P. M., Ehrhart, S., Ye, P., Kirkby, J., Curtius, J., Baltensperger, U., Kulmala, M., Lehtinen, K. E. J., Smith, J. N., Riipinen, Ilona, Virtanen, A., Kim, J., Ahlm, Lars, Yli-Juuti, T., Lawler, M., Keskinen, H., Tröstl, J., Schobesberger, S., Duplissy, J., Amorim, A., Bianchi, F., Donahue, N. M., Flagan, R. C., Hakala, J., Heinritzi, M., Jokinen, T., Kürten, A., Laaksonen, A., Lehtipalo, K., Miettinen, P., Petäjä, T., Rissanen, M. P., Rondo, L., Sengupta, K., Simon, M., Tomé, A., Williamson, C., Wimmer, D., Winkler, P. M., Ehrhart, S., Ye, P., Kirkby, J., Curtius, J., Baltensperger, U., Kulmala, M., Lehtinen, K. E. J., Smith, J. N., Riipinen, Ilona, and Virtanen, A.

Abstract

Sulfuric acid, amines and oxidized organics have been found to be important compounds in the nucleation and initial growth of atmospheric particles. Because of the challenges involved in determining the chemical composition of objects with very small mass, however, the properties of the freshly nucleated particles and the detailed pathways of their formation processes are still not clear. In this study,we focus on a challenging size range, i.e., particles that have grown to diameters of 10 and 15 nm following nucleation, and measure their water uptake. Water uptake is useful information for indirectly obtaining chemical composition of aerosol particles. We use a nanometer-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) at sub-saturated conditions (ca. 90% relative humidity at 293 K) to measure the hygroscopicity of particles during the seventh Cosmics Leaving OUtdoor Droplets (CLOUD7) campaign performed at CERN in 2012. In CLOUD7, the hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid-dimethylamine, and sulfuric acid-organics derived from alpha-pinene oxidation. The hygroscopicity parameter kappa decreased with increasing particle size, indicating decreasing acidity of particles. No clear effect of the sulfuric acid concentration on the hygroscopicity of 10 nm particles produced from sulfuric acid and dimethylamine was observed, whereas the hygroscopicity of 15 nm particles sharply decreased with decreasing sulfuric acid concentrations. In particular, when the concentration of sulfuric acid was 5.1 x 10(6) molecules cm(-3) in the gas phase, and the dimethylamine mixing ratio was 11.8 ppt, the measured kappa of 15 nm particles was 0.31 +/- 0.01: close to the value reported for dimethylaminium sulfate (DMAS) (kappa(DMAS) similar to 0.28). Furthermore, the difference in kappa between sulfuric acid and sulfuric acid-dimethylamine experiments increased with increasing particle size. The kappa values of

Published
2016
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20. Modeling the thermodynamics and kinetics of sulfuric acid-dimethylamine-water nanoparticle growth in the CLOUD chamber

Author

Ahlm, Lars, Yli-Juuti, T., Schobesberger, S., Praplan, A. P., Kim, J., Tikkanen, O. -P., Lawler, M. J., Smith, J. N., Trostl, J., Acosta Navarro, Juan Camilo, Baltensperger, U., Bianchi, F., Donahue, N. M., Duplissy, J., Franchin, A., Jokinen, T., Keskinen, H., Kirkby, J., Kuerten, A., Laaksonen, A., Lehtipalo, K., Petaja, T., Riccobono, F., Rissanen, M. P., Rondo, L., Schallhart, S., Simon, M., Winkler, P. M., Worsnop, D. R., Virtanen, A., Riipinen, I., Ahlm, Lars, Yli-Juuti, T., Schobesberger, S., Praplan, A. P., Kim, J., Tikkanen, O. -P., Lawler, M. J., Smith, J. N., Trostl, J., Acosta Navarro, Juan Camilo, Baltensperger, U., Bianchi, F., Donahue, N. M., Duplissy, J., Franchin, A., Jokinen, T., Keskinen, H., Kirkby, J., Kuerten, A., Laaksonen, A., Lehtipalo, K., Petaja, T., Riccobono, F., Rissanen, M. P., Rondo, L., Schallhart, S., Simon, M., Winkler, P. M., Worsnop, D. R., Virtanen, A., and Riipinen, I.

Abstract

Dimethylamine (DMA) has a stabilizing effect on sulfuric acid (SA) clusters, and the SA and DMA molecules and clusters likely play important roles in both aerosol particle formation and growth in the atmosphere. We use the monodisperse particle growth model for acid-base chemistry in nanoparticle growth (MABNAG) together with direct and indirect observations from the CLOUD4 and CLOUD7 experiments in the cosmics leaving outdoor droplets (CLOUD) chamber at CERN to investigate the size and composition evolution of freshly formed particles consisting of SA, DMA, and water as they grow to 20nm in dry diameter. Hygroscopic growth factors are measured using a nano-hygroscopicity tandem differential mobility analyzer (nano-HTDMA), which combined with simulations of particle water uptake using the thermodynamic extended-aerosol inorganics model (E-AIM) constrain the chemical composition. MABNAG predicts a particle-phase ratio between DMA and SA molecules of 1.1-1.3 for a 2nm particle and DMA gas-phase mixing ratios between 3.5 and 80 pptv. These ratios agree well with observations by an atmospheric-pressure interface time-of-flight (APi-TOF) mass spectrometer. Simulations with MABNAG, direct observations of the composition of clusters <2nm, and indirect observations of the particle composition indicate that the acidity of the nucleated particles decreases as they grow from approximate to 1 to 20nm. However, MABNAG predicts less acidic particles than suggested by the indirect estimates at 10nm diameter using the nano-HTDMA measurements, and less acidic particles than observed by a thermal desorption chemical ionization mass spectrometer (TDCIMS) at 10-30nm. Possible explanations for these discrepancies are discussed.

Published
2016
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21. A chamber study of the influence of boreal BVOC emissions and sulfuric acid on nanoparticle formation rates at ambient concentrations

Author

University of Helsinki, Department of Physics, Dal Maso, M., Liao, L., Wildt, J., Kiendler-Scharr, A., Kleist, E., Tillmann, R., Sipilä, M., Hakala, J., Lehtipalo, K., Ehn, M., Kerminen, V. -M., Kulmala, M., Worsnop, D., Mentel, T., University of Helsinki, Department of Physics, Dal Maso, M., Liao, L., Wildt, J., Kiendler-Scharr, A., Kleist, E., Tillmann, R., Sipilä, M., Hakala, J., Lehtipalo, K., Ehn, M., Kerminen, V. -M., Kulmala, M., Worsnop, D., and Mentel, T.

Abstract

Aerosol formation from biogenic and anthropogenic precursor trace gases in continental background areas affects climate via altering the amount of available cloud condensation nuclei. Significant uncertainty still exists regarding the agents controlling the formation of aerosol nanoparticles. We have performed experiments in the Julich plant-atmosphere simulation chamber with instrumentation for the detection of sulfuric acid and nanoparticles, and present the first simultaneous chamber observations of nanoparticles, sulfuric acid, and realistic levels and mixtures of biogenic volatile compounds (BVOCs). We present direct laboratory observations of nanoparticle formation from sulfuric acid and realistic BVOC precursor vapour mixtures performed at atmospherically relevant concentration levels. We directly measured particle formation rates separately from particle growth rates. From this, we established that in our experiments, the formation rate was proportional to the product of sulfuric acid and biogenic VOC emission strength. The formation rates were consistent with a mechanism in which nucleating BVOC oxidation products are rapidly formed and activate with sulfuric acid. The growth rate of nanoparticles immediately after birth was best correlated with estimated products resulting from BVOC ozonolysis.

Published
2016

22. Effect of ions on sulfuric acid-water binary particle formation : 2. Experimental data and comparison with QC-normalized classical nucleation theory

Author

Duplissy, J., Merikanto, J., Franchin, A., Tsagkogeorgas, G., Kangasluoma, J., Wimmer, D., Vuollekoski, H., Schobesberger, S., Lehtipalo, K., Flagan, R. C., Brus, D., Donahue, N. M., Vehkamaki, H., Almeida, J., Amorim, A., Barmet, P., Bianchi, F., Breitenlechner, M., Dunne, E. M., Guida, R., Henschel, Henning, Junninen, H., Kirkby, J., Kuerten, A., Kupc, A., Maattanen, A., Makhmutov, V., Mathot, S., Nieminen, T., Onnela, A., Praplan, A. P., Riccobono, F., Rondo, L., Steiner, G., Tome, A., Walther, H., Baltensperger, U., Carslaw, K. S., Dommen, J., Hansel, A., Petaja, T., Sipila, M., Stratmann, F., Vrtala, A., Wagner, P. E., Worsnop, D. R., Curtius, J., Kulmala, M., Duplissy, J., Merikanto, J., Franchin, A., Tsagkogeorgas, G., Kangasluoma, J., Wimmer, D., Vuollekoski, H., Schobesberger, S., Lehtipalo, K., Flagan, R. C., Brus, D., Donahue, N. M., Vehkamaki, H., Almeida, J., Amorim, A., Barmet, P., Bianchi, F., Breitenlechner, M., Dunne, E. M., Guida, R., Henschel, Henning, Junninen, H., Kirkby, J., Kuerten, A., Kupc, A., Maattanen, A., Makhmutov, V., Mathot, S., Nieminen, T., Onnela, A., Praplan, A. P., Riccobono, F., Rondo, L., Steiner, G., Tome, A., Walther, H., Baltensperger, U., Carslaw, K. S., Dommen, J., Hansel, A., Petaja, T., Sipila, M., Stratmann, F., Vrtala, A., Wagner, P. E., Worsnop, D. R., Curtius, J., and Kulmala, M.

Published
2016

23. Modeling the thermodynamics and kinetics of sulfuric acid-dimethylamine-water nanoparticle growth in the CLOUD chamber

Author

Ahlm, L., primary, Yli-Juuti, T., additional, Schobesberger, S., additional, Praplan, A. P., additional, Kim, J., additional, Tikkanen, O.-P., additional, Lawler, M. J., additional, Smith, J. N., additional, Tröstl, J., additional, Acosta Navarro, J. C., additional, Baltensperger, U., additional, Bianchi, F., additional, Donahue, N. M., additional, Duplissy, J., additional, Franchin, A., additional, Jokinen, T., additional, Keskinen, H., additional, Kirkby, J., additional, Kürten, A., additional, Laaksonen, A., additional, Lehtipalo, K., additional, Petäjä, T., additional, Riccobono, F., additional, Rissanen, M. P., additional, Rondo, L., additional, Schallhart, S., additional, Simon, M., additional, Winkler, P. M., additional, Worsnop, D. R., additional, Virtanen, A., additional, and Riipinen, I., additional

Published
2016
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24. A chamber study of the influence of boreal BVOC emissions and sulfuric acid on nanoparticle formation rates at ambient concentrations

Author

Dal Maso, M., primary, Liao, L., additional, Wildt, J., additional, Kiendler-Scharr, A., additional, Kleist, E., additional, Tillmann, R., additional, Sipilä, M., additional, Hakala, J., additional, Lehtipalo, K., additional, Ehn, M., additional, Kerminen, V.-M., additional, Kulmala, M., additional, Worsnop, D., additional, and Mentel, T., additional

Published
2016
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26. Hygroscopicity of nanoparticles produced from homogeneous nucleation in the CLOUD experiments

Author

Kim, J., primary, Ahlm, L., additional, Yli-Juuti, T., additional, Lawler, M., additional, Keskinen, H., additional, Tröstl, J., additional, Schobesberger, S., additional, Duplissy, J., additional, Amorim, A., additional, Bianchi, F., additional, Donahue, N. M., additional, Flagan, R. C., additional, Hakala, J., additional, Heinritzi, M., additional, Jokinen, T., additional, Kürten, A., additional, Laaksonen, A., additional, Lehtipalo, K., additional, Miettinen, P., additional, Petäjä, T., additional, Rissanen, M. P., additional, Rondo, L., additional, Sengupta, K., additional, Simon, M., additional, Tomé, A., additional, Williamson, C., additional, Wimmer, D., additional, Winkler, P. M., additional, Ehrhart, S., additional, Ye, P., additional, Kirkby, J., additional, Curtius, J., additional, Baltensperger, U., additional, Kulmala, M., additional, Lehtinen, K. E. J., additional, Smith, J. N., additional, Riipinen, I., additional, and Virtanen, A., additional

Published
2016
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27. Elemental composition and clustering behaviour of alpha-pinene oxidation products for different oxidation conditions

Author

University of Helsinki, Department of Physics, University of Helsinki, Helsinki Institute of Physics, Praplan, A. P., Schobesberger, S., Bianchi, F., Rissanen, M. P., Ehn, M., Jokinen, Tuija, Junninen, H., Adamov, A., Amorim, A., Dommen, J., Duplissy, J., Hakala, J., Hansel, A., Heinritzi, M., Kangasluoma, J., Kirkby, J., Krapf, M., Kürten, A., Lehtipalo, K., Riccobono, F., Rondo, L., Sarnela, N., Simon, M., Tome, A., Tröstl, J., Winkler, P. M., Williamson, C., Ye, P., Curtius, J., Baltensperger, U., Donahue, N. M., Kulmala, Markku, Worsnop, D. R., University of Helsinki, Department of Physics, University of Helsinki, Helsinki Institute of Physics, Praplan, A. P., Schobesberger, S., Bianchi, F., Rissanen, M. P., Ehn, M., Jokinen, Tuija, Junninen, H., Adamov, A., Amorim, A., Dommen, J., Duplissy, J., Hakala, J., Hansel, A., Heinritzi, M., Kangasluoma, J., Kirkby, J., Krapf, M., Kürten, A., Lehtipalo, K., Riccobono, F., Rondo, L., Sarnela, N., Simon, M., Tome, A., Tröstl, J., Winkler, P. M., Williamson, C., Ye, P., Curtius, J., Baltensperger, U., Donahue, N. M., Kulmala, Markku, and Worsnop, D. R.

Abstract

This study presents the difference between oxidised organic compounds formed by alpha-pinene oxidation under various conditions in the CLOUD environmental chamber: (1) pure ozonolysis (in the presence of hydrogen as hydroxyl radical (OH) scavenger) and (2) OH oxidation (initiated by nitrous acid (HONO) photolysis by ultraviolet light) in the absence of ozone. We discuss results from three Atmospheric Pressure interface Time-of-Flight (APi-TOF) mass spectrometers measuring simultaneously the composition of naturally charged as well as neutral species (via chemical ionisation with nitrate). Natural chemical ionisation takes place in the CLOUD chamber and organic oxidised compounds form clusters with nitrate, bisulfate, bisulfate/sulfuric acid clusters, ammonium, and dimethylaminium, or get protonated. The results from this study show that this process is selective for various oxidised organic compounds with low molar mass and ions, so that in order to obtain a comprehensive picture of the elemental composition of oxidation products and their clustering behaviour, several instruments must be used. We compare oxidation products containing 10 and 20 carbon atoms and show that highly oxidised organic compounds are formed in the early stages of the oxidation.

Published
2015

28. On the composition of ammonia-sulfuric-acid ion clusters during aerosol particle formation

Author

University of Helsinki, Department of Physics, University of Helsinki, Helsinki Institute of Physics, Schobesberger, S., Franchin, A., Bianchi, F., Rondo, L., Duplissy, J., Kuerten, A., Ortega Colomer, Ismael Kenneth, Metzger, A., Schnitzhofer, R., Almeida, J., Amorim, A., Dommen, J., Dunne, E. M., Ehn, M., Gagne, S., Ickes, L., Junninen, H., Hansel, A., Kerminen, V-M, Kirkby, J., Kupc, A., Laaksonen, A., Lehtipalo, K., Mathot, S., Onnela, A., Petaja, T., Riccobono, F., Santos, F. D., Sipila, M., Tome, A., Tsagkogeorgas, G., Viisanen, Y., Wagner, P. E., Wimmer, D., Curtius, J., Donahue, N. M., Baltensperger, U., Kulmala, M., Worsnop, D. R., University of Helsinki, Department of Physics, University of Helsinki, Helsinki Institute of Physics, Schobesberger, S., Franchin, A., Bianchi, F., Rondo, L., Duplissy, J., Kuerten, A., Ortega Colomer, Ismael Kenneth, Metzger, A., Schnitzhofer, R., Almeida, J., Amorim, A., Dommen, J., Dunne, E. M., Ehn, M., Gagne, S., Ickes, L., Junninen, H., Hansel, A., Kerminen, V-M, Kirkby, J., Kupc, A., Laaksonen, A., Lehtipalo, K., Mathot, S., Onnela, A., Petaja, T., Riccobono, F., Santos, F. D., Sipila, M., Tome, A., Tsagkogeorgas, G., Viisanen, Y., Wagner, P. E., Wimmer, D., Curtius, J., Donahue, N. M., Baltensperger, U., Kulmala, M., and Worsnop, D. R.

Published
2015

29. Major contribution of neutral clusters to new particle formation at the interface between the boundary layer and the free troposphere

Author

University of Helsinki, Department of Physics, University of Helsinki, Helsinki Institute of Physics, Rose, C., Sellegri, K., Asmi, E., Hervo, M., Freney, E., Colomb, A., Junninen, H., Duplissy, J., Sipilä, Mikko, Kontkanen, J., Lehtipalo, K., Kulmala, Markku, University of Helsinki, Department of Physics, University of Helsinki, Helsinki Institute of Physics, Rose, C., Sellegri, K., Asmi, E., Hervo, M., Freney, E., Colomb, A., Junninen, H., Duplissy, J., Sipilä, Mikko, Kontkanen, J., Lehtipalo, K., and Kulmala, Markku

Abstract

The formation of new aerosol particles in the atmosphere is a key process influencing the aerosol number concentration as well as the climate, in particular at high altitude, where the newly formed particles directly influence cloud formation. However, free tropospheric new particle formation (NPF) is poorly documented due to logistic limitations and complex atmospheric dynamics around high-altitude stations that make the observation of this day-time process challenging. Recent improvements in measurement techniques make now possible the detection of neutral clusters down to similar to 1 nm sizes, which opens new horizons in our understanding of the nucleation process. Indeed, only the charged fraction of clusters has been reported in the upper troposphere up to now. Here we report day-time concentrations of charged and neutral clusters (1 to 2.5 nm mobility diameter) recorded at the interface between the boundary layer (BL) and the FT as well as in the FT at the altitude site of Puy de Dome (1465 m a.s.l.), central France, between 10 and 29 February 2012. Our findings demonstrate that in the FT, and especially at the interface between the BL and the FT, the formation of 1.5 nm neutral clusters significantly exceeds the one of ionic clusters during NPF events, clearly indicating that they dominate in the nucleation process. We also observe that the total cluster concentration significantly increases during NPF events compared to the other days, which was not clearly observed for the charged cluster population in the past. During the studied period, the nucleation process does not seem to be sulfuric acid-limited and could be promoted by the transport of pollutants to the upper troposphere, coupled with low temperatures.

Published
2015

32. Direct Observations of Atmospheric Aerosol Nucleation

Author

Kulmala M, Kontkanen J, Junninen H, Lehtipalo K, Manninen HE, Nieminen T, Petaja T, Sipila M, Sipila Mikko, Schobesberger S, Rantala P, Franchin A, Jokinen T, Jarvinen E, Aijala M, Kangasluoma J, Hakala J, Aalto PP, Paasonen P, Mikkila J, Vanhanen J, Aalto J, Hakola H, Makkonen U, Ruuskanen T, Mauldin RL, Duplissy J, Vehkamaki H, Back J, Kortelainen A, Riipinen I, Kurten T, Johnston MV, Smith JN, Ehn M, Mentel TF, Lehtinen KEJ, Laaksonen A, Kerminen VM, and Worsnop

Published
2013

34. EUCAARI ion spectrometer measurements at 12 European sites \u2013 analysis of new particle formation events

Author

Manninen, H. E, Nieminen, T, Asmi, E, Gagn, S, Hxe4kkinen, S, Lehtipalo, K, Aalto, P, Vana, M, Mirme, A, Mirme, S, Hrrak, U, Plass-Dlmer, C, Stange, G, Kiss, G, Hoffer, A, Txf6xf6, N, Moerman, M, Henzing, B, de Leeuw, G, Brinkenberg, M, Kouvarakis, G. N, Bougiatioti, A, Mihalopoulos, N, O'Dowd, C, Ceburnis, D, Arneth, A, Svenningsson, B, Swietlicki, E, Tarozzi, L, Decesari, S, Facchini, M. C, Birmili, W, Sonntag, A, Wiedensohler, A, Boulon, J, and Sellegri, Kulmala, M

Published
2010

37. Hygroscopicity of nanoparticles produced from homogeneous nucleation in the CLOUD experiments

Author

Kim, J., primary, Ahlm, L., additional, Yli-Juuti, T., additional, Lawler, M., additional, Keskinen, H., additional, Tröstl, J., additional, Schobesberger, S., additional, Duplissy, J., additional, Amorim, A., additional, Bianchi, F., additional, Donahue, N. M., additional, Flagan, R. C., additional, Hakala, J., additional, Heinritzi, M., additional, Jokinen, T., additional, Kürten, A., additional, Laaksonen, A., additional, Lehtipalo, K., additional, Miettinen, P., additional, Petäjä, T., additional, Rissanen, M. P., additional, Rondo, L., additional, Sengupta, K., additional, Simon, M., additional, Tomé, A., additional, Williamson, C., additional, Wimmer, D., additional, Winkler, P. M., additional, Ehrhart, S., additional, Ye, P., additional, Kirkby, J., additional, Curtius, J., additional, Kulmala, M., additional, Lehtinen, K. E. J., additional, Smith, J. N., additional, Riipinen, I., additional, and Virtanen, A., additional

Published
2015
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38. Technical Note: Using DEG-CPCs at upper tropospheric temperatures

Author

Wimmer, D., primary, Lehtipalo, K., additional, Nieminen, T., additional, Duplissy, J., additional, Ehrhart, S., additional, Almeida, J., additional, Rondo, L., additional, Franchin, A., additional, Kreissl, F., additional, Bianchi, F., additional, Manninen, H. E., additional, Kulmala, M., additional, Curtius, J., additional, and Petäjä, T., additional

Published
2015
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39. Experimental investigation of ion–ion recombination under atmospheric conditions

Author

Franchin, A., primary, Ehrhart, S., additional, Leppä, J., additional, Nieminen, T., additional, Gagné, S., additional, Schobesberger, S., additional, Wimmer, D., additional, Duplissy, J., additional, Riccobono, F., additional, Dunne, E. M., additional, Rondo, L., additional, Downard, A., additional, Bianchi, F., additional, Kupc, A., additional, Tsagkogeorgas, G., additional, Lehtipalo, K., additional, Manninen, H. E., additional, Almeida, J., additional, Amorim, A., additional, Wagner, P. E., additional, Hansel, A., additional, Kirkby, J., additional, Kürten, A., additional, Donahue, N. M., additional, Makhmutov, V., additional, Mathot, S., additional, Metzger, A., additional, Petäjä, T., additional, Schnitzhofer, R., additional, Sipilä, M., additional, Stozhkov, Y., additional, Tomé, A., additional, Kerminen, V.-M., additional, Carslaw, K., additional, Curtius, J., additional, Baltensperger, U., additional, and Kulmala, M., additional

Published
2015
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41. Elemental composition and clustering behaviour of α-pinene oxidation products for different oxidation conditions

Author

Praplan, A. P., primary, Schobesberger, S., additional, Bianchi, F., additional, Rissanen, M. P., additional, Ehn, M., additional, Jokinen, T., additional, Junninen, H., additional, Adamov, A., additional, Amorim, A., additional, Dommen, J., additional, Duplissy, J., additional, Hakala, J., additional, Hansel, A., additional, Heinritzi, M., additional, Kangasluoma, J., additional, Kirkby, J., additional, Krapf, M., additional, Kürten, A., additional, Lehtipalo, K., additional, Riccobono, F., additional, Rondo, L., additional, Sarnela, N., additional, Simon, M., additional, Tomé, A., additional, Tröstl, J., additional, Winkler, P. M., additional, Williamson, C., additional, Ye, P., additional, Curtius, J., additional, Baltensperger, U., additional, Donahue, N. M., additional, Kulmala, M., additional, and Worsnop, D. R., additional

Published
2015
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43. Experimental investigation of ion-ion recombination at atmospheric conditions

Author

Franchin, A., primary, Ehrhart, S., additional, Leppä, J., additional, Nieminen, T., additional, Gagné, S., additional, Schobesberger, S., additional, Wimmer, D., additional, Duplissy, J., additional, Riccobono, F., additional, Dunne, E., additional, Rondo, L., additional, Downard, A., additional, Bianchi, F., additional, Kupc, A., additional, Tsagkogeorgas, G., additional, Lehtipalo, K., additional, Manninen, H. E., additional, Almeida, J., additional, Amorim, A., additional, Wagner, P. E., additional, Hansel, A., additional, Kirkby, J., additional, Kürten, A., additional, Donahue, N. M., additional, Makhmutov, V., additional, Mathot, S., additional, Metzger, A., additional, Petäjä, T., additional, Schnitzhofer, R., additional, Sipilä, M., additional, Stozhkov, Y., additional, Tomé, A., additional, Kerminen, V.-M., additional, Carslaw, K., additional, Curtius, J., additional, Baltensperger, U., additional, and Kulmala, M., additional

Published
2015
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44. On the composition of ammonia–sulfuric-acid ion clusters during aerosol particle formation

Author

Schobesberger, S., primary, Franchin, A., additional, Bianchi, F., additional, Rondo, L., additional, Duplissy, J., additional, Kürten, A., additional, Ortega, I. K., additional, Metzger, A., additional, Schnitzhofer, R., additional, Almeida, J., additional, Amorim, A., additional, Dommen, J., additional, Dunne, E. M., additional, Ehn, M., additional, Gagné, S., additional, Ickes, L., additional, Junninen, H., additional, Hansel, A., additional, Kerminen, V.-M., additional, Kirkby, J., additional, Kupc, A., additional, Laaksonen, A., additional, Lehtipalo, K., additional, Mathot, S., additional, Onnela, A., additional, Petäjä, T., additional, Riccobono, F., additional, Santos, F. D., additional, Sipilä, M., additional, Tomé, A., additional, Tsagkogeorgas, G., additional, Viisanen, Y., additional, Wagner, P. E., additional, Wimmer, D., additional, Curtius, J., additional, Donahue, N. M., additional, Baltensperger, U., additional, Kulmala, M., additional, and Worsnop, D. R., additional

Published
2015
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45. EUCAARI ion spectrometer measurements at 12 European sites-analysis of new particle formation events

Author

Manninen, H.E., Nieminen, T., Asmi, E., Gagné, S., Häkkinen, S., Lehtipalo, K., Aalto, P., Vana, M., Mirme, A., Mirme, S., Hõrrak, U., Plass-Dülmer, C., Stange, G., Kiss, G., Hoffer, A., Töro, N., Moerman, M., Henzing, B., Leeuw, G. de, Brinkenberg, M., Kouvarakis, G.N., Bougiatioti, A., Mihalopoulos, N., O'Dowd, C., Ceburnis, D., Arneth, A., Svenningsson, B., Swietlicki, E., Tarozzi, L., Decesari, S., Facchini, M.C., Birmili, W., Sonntag, A., Wiedensohler, A., Boulon, J., Sellegri, K., Laj, P., Gysel, M., Bukowiecki, N., Weingartner, E., Wehrle, G., Laaksonen, A., Hamed, A., Joutsensaari, J., Petäjä, T., Kerminen, V.-M., Kulmala, M., and TNO Bouw en Ondergrond

Subjects
Earth & Environment, spatial variation, cloud microphysics, Environment, air quality, temporal variation, particle motion, volcanic cloud, UES - Urban Environment & Safety, spectrometer, EELS - Earth, Environmental and Life Sciences, cloud condensation nucleus, ground-based measurement
Abstract

We present comprehensive results on continuous atmospheric cluster and particle measurements in the size range ∼1-42 nm within the European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) project. We focused on characterizing the spatial and temporal variation of new particle formation events and relevant particle formation parameters across Europe. Different types of air ion and cluster mobility spectrometers were deployed at 12 field sites across Europe from March 2008 to May 2009. The measurements were conducted in a wide variety of environments, including coastal and continental locations as well as sites at different altitudes (both in the boundary layer and the free troposphere). New particle formation events were detected at all of the 12 field sites during the year-long measurement period. From the data, nucleation and growth rates of newly formed particles were determined for each environment. In a case of parallel ion and neutral cluster measurements, we could also estimate the relative contribution of ion-induced and neutral nucleation to the total particle formation. The formation rates of charged particles at 2 nm accounted for 1-30% of the corresponding total particle formation rates. As a significant new result, we found out that the total particle formation rate varied much more between the different sites than the formation rate of charged particles. This work presents, so far, the most comprehensive effort to experimentally characterize nucleation and growth of atmospheric molecular clusters and nanoparticles at ground-based observation sites on a continental scale. © Author(s) 2010.

Published
2010

46. Trends in new particle formation in eastern Lapland, Finland : effect of decreasing sulfur emissions from Kola Peninsula

Author

Kyro, E. -M, Vaananen, R., Kerminen, V. -M, Virkkula, A., Petaja, T., Asmi, A., Dal Maso, M., Nieminen, T., Juhola, S., Shcherbinin, A., Riipinen, Ilona, Lehtipalo, K., Keronen, P., Aalto, P. P., Hari, P., Kulmala, M., Kyro, E. -M, Vaananen, R., Kerminen, V. -M, Virkkula, A., Petaja, T., Asmi, A., Dal Maso, M., Nieminen, T., Juhola, S., Shcherbinin, A., Riipinen, Ilona, Lehtipalo, K., Keronen, P., Aalto, P. P., Hari, P., and Kulmala, M.

Abstract

The smelter industry in Kola Peninsula is the largest source of anthropogenic SO2 in the Arctic part of Europe and one of the largest within the Arctic domain. Due to socio-economic changes in Russia, the emissions have been decreasing especially since the late 1990s resulting in decreased SO2 concentrations close to Kola in eastern Lapland, Finland. At the same time, the frequency of new particle formation days has been decreasing distinctively at SMEAR I station in eastern Lapland, especially during spring and autumn. We show that sulfur species, namely sulfur dioxide and sulfuric acid, have an important role in both new particle formation and subsequent growth and that the decrease in new particle formation days is a result of the reduction of sulfur emissions originating from Kola Peninsula. In addition to sulfur species, there are many other quantities, such as formation rate of aerosol particles, condensation sink and nucleation mode particle number concentration, which are related to the number of observed new particle formation (NPF) days and need to be addressed when linking sulfur emissions and NPF. We show that while most of these quantities exhibit statistically significant trends, the reduction in Kola sulfur emissions is the most obvious reason for the rapid decline in NPF days. Sulfuric acid explains approximately 20-50% of the aerosol condensational growth observed at SMEAR I, and there is a large seasonal variation with highest values obtained during spring and autumn. We found that (i) particles form earlier after sunrise during late winter and early spring due to high concentrations of SO2 and H2SO4; (ii) several events occurred during the absence of light, and they were connected to higher than average concentrations of SO2; and (iii) high SO2 concentrations could advance the onset of nucleation by several hours. Moreover, air masses coming over Kola Peninsula seemed to favour new particle formation., AuthorCount:16

Published
2014
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47. A chamber study of the influence of boreal BVOC emissions and sulphuric acid on nanoparticle formation rates at ambient concentrations

Author

Dal Maso, M., primary, Liao, L., additional, Wildt, J., additional, Kiendler-Scharr, A., additional, Kleist, E., additional, Tillmann, R., additional, Sipilä, M., additional, Hakala, J., additional, Lehtipalo, K., additional, Ehn, M., additional, Kerminen, V.-M., additional, Kulmala, M., additional, Worsnop, D., additional, and Mentel, T., additional

Published
2014
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48. Elemental composition and clustering of α-pinene oxidation products for different oxidation conditions

Author

Praplan, A. P., primary, Schobesberger, S., additional, Bianchi, F., additional, Rissanen, M. P., additional, Ehn, M., additional, Jokinen, T., additional, Junninen, H., additional, Adamov, A., additional, Amorim, A., additional, Dommen, J., additional, Duplissy, J., additional, Hakala, J., additional, Hansel, A., additional, Heinritzi, M., additional, Kangasluoma, J., additional, Kirkby, J., additional, Krapf, M., additional, Kürten, A., additional, Lehtipalo, K., additional, Riccobono, F., additional, Rondo, L., additional, Sarnela, N., additional, Simon, M., additional, Tomé, A., additional, Tröstl, J., additional, Winkler, P. M., additional, Williamson, C., additional, Ye, P., additional, Curtius, J., additional, Baltensperger, U., additional, Donahue, N. M., additional, Kulmala, M., additional, and Worsnop, D. R., additional

Published
2014
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50. On the composition of ammonia-sulfuric acid clusters during aerosol particle formation

Author

Schobesberger, S., primary, Franchin, A., additional, Bianchi, F., additional, Rondo, L., additional, Duplissy, J., additional, Kürten, A., additional, Ortega, I. K., additional, Metzger, A., additional, Schnitzhofer, R., additional, Almeida, J., additional, Amorim, A., additional, Dommen, J., additional, Dunne, E. M., additional, Ehn, M., additional, Gagné, S., additional, Ickes, L., additional, Junninen, H., additional, Hansel, A., additional, Kerminen, V.-M., additional, Kirkby, J., additional, Kupc, A., additional, Laaksonen, A., additional, Lehtipalo, K., additional, Mathot, S., additional, Onnela, A., additional, Petäjä, T., additional, Riccobono, F., additional, Santos, F. D., additional, Sipilä, M., additional, Tomé, A., additional, Tsagkogeorgas, G., additional, Viisanen, Y., additional, Wagner, P. E., additional, Wimmer, D., additional, Curtius, J., additional, Donahue, N. M., additional, Baltensperger, U., additional, Kulmala, M., additional, and Worsnop, D. R., additional

Published
2014
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