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  • 1. Dall'Osto, M.
    et al.
    Beddows, D. C. S.
    Asmi, A.
    Poulain, L.
    Hao, L.
    Freney, E.
    Allan, J. D.
    Canagaratna, M.
    Crippa, M.
    Bianchi, F.
    de Leeuw, G.
    Eriksson, A.
    Swietlicki, E.
    Hansson, Hans Christen
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Henzing, J. S.
    Granier, C.
    Zemankova, K.
    Laj, P.
    Onasch, T.
    Prevot, A.
    Putaud, J. P.
    Sellegri, K.
    Vidal, M.
    Virtanen, A.
    Simo, R.
    Worsnop, D.
    O'Dowd, C.
    Kulmala, M.
    Harrison, Roy M.
    Novel insights on new particle formation derived from a pan-european observing system2018In: Scientific Reports, ISSN 2045-2322, E-ISSN 2045-2322, Vol. 8, article id 1482Article in journal (Refereed)
    Abstract [en]

    The formation of new atmospheric particles involves an initial step forming stable clusters less than a nanometre in size (<similar to 1 nm), followed by growth into quasi-stable aerosol particles a few nanometres (similar to 1-10 nm) and larger (>similar to 10 nm). Although at times, the same species can be responsible for both processes, it is thought that more generally each step comprises differing chemical contributors. Here, we present a novel analysis of measurements from a unique multi-station ground-based observing system which reveals new insights into continental-scale patterns associated with new particle formation. Statistical cluster analysis of this unique 2-year multi-station dataset comprising size distribution and chemical composition reveals that across Europe, there are different major seasonal trends depending on geographical location, concomitant with diversity in nucleating species while it seems that the growth phase is dominated by organic aerosol formation. The diversity and seasonality of these events requires an advanced observing system to elucidate the key processes and species driving particle formation, along with detecting continental scale changes in aerosol formation into the future.

  • 2. Huang, Wei
    et al.
    Saathoff, Harald
    Pajunoja, Aki
    Shen, Xiaoli
    Naumann, Karl-Heinz
    Wagner, Robert
    Virtanen, Annele
    Leisner, Thomas
    Mohr, Claudia
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. Karlsruhe Institute of Technology, Germany.
    alpha-Pinene secondary organic aerosol at low temperature: chemical composition and implications for particle viscosity2018In: Atmospheric Chemistry And Physics, ISSN 1680-7316, E-ISSN 1680-7324, Vol. 18, no 4, p. 2883-2898Article in journal (Refereed)
    Abstract [en]

    Chemical composition, size distributions, and degree of oligomerization of secondary organic aerosol (SOA) from alpha-pinene (C10H16) ozonolysis were investigated for low-temperature conditions (223 K). Two types of experiments were performed using two simulation chambers at the Karlsruhe Institute of Technology: the Aerosol Preparation and Characterization (APC) chamber, and the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) chamber. Experiment type 1 simulated SOA formation at upper tropospheric conditions: SOA was generated in the AIDA chamber directly at 223K at 61% relative humidity (RH; experiment termed cold humid, CH) and for comparison at 6% RH (experiment termed cold dry, CD) conditions. Experiment type 2 simulated SOA uplifting: SOA was formed in the APC chamber at room temperature (296 K) and < 1% RH (experiment termed warm dry, WD) or 21% RH (experiment termed warm humid, WH) conditions, and then partially transferred to the AIDA chamber kept at 223 K, and 61% RH (WDtoCH) or 30% RH (WHtoCH), respectively. Precursor concentrations varied between 0.7 and 2.2 ppm alpha-pinene, and between 2.3 and 1.8 ppm ozone for type 1 and type 2 experiments, respectively. Among other instrumentation, a chemical ionization mass spectrometer (CIMS) coupled to a filter inlet for gases and aerosols (FIGAERO), deploying I as reagent ion, was used for SOA chemical composition analysis.

    For type 1 experiments with lower alpha-pinene concentrations and cold SOA formation temperature (223 K), smaller particles of 100-300 nm vacuum aerodynamic diameter (d(va)/and higher mass fractions (> 40 %) of adducts (molecules with more than 10 carbon atoms) of alpha-pinene oxidation products were observed. For type 2 experiments with higher alpha-pinene concentrations and warm SOA formation temperature (296 K), larger particles (similar to 500 nm d(va)/with smaller mass fractions of adducts (< 35 %) were produced.

    We also observed differences (up to 20 degrees C) in maximum desorption temperature (T-max/of individual compounds desorbing from the particles deposited on the FIGAERO Teflon filter for different experiments, indicating that T-max is not purely a function of a compound's vapor pressure or volatility, but is also influenced by diffusion limitations within the particles (particle viscosity), interactions between particles deposited on the filter (particle matrix), and/or particle mass on the filter. Highest T max were observed for SOA under dry conditions and with higher adduct mass fraction; lowest T-max were observed for SOA under humid conditions and with lower adduct mass fraction. The observations indicate that particle viscosity may be influenced by intra-and inter-molecular hydrogen bonding between oligomers, and particle water uptake, even under such low-temperature conditions.

    Our results suggest that particle physicochemical properties such as viscosity and oligomer content mutually influence each other, and that variation in T-max of particle desorptions may have implications for particle viscosity and particle matrix effects. The differences in particle physicochemical properties observed between our different experiments demonstrate the importance of taking experimental conditions into consideration when interpreting data from laboratory studies or using them as input in climate models.

  • 3. Lehtipalo, Katrianne
    et al.
    Yan, Chao
    Dada, Lubna
    Bianchi, Federico
    Xiao, Mao
    Wagner, Robert
    Stolzenburg, Dominik
    Ahonen, Lauri R.
    Amorim, Antonio
    Baccarini, Andrea
    Bauer, Paulus S.
    Baumgartner, Bernhard
    Bergen, Anton
    Bernhammer, Anne-Kathrin
    Breitenlechner, Martin
    Brilke, Sophia
    Buchholz, Angela
    Mazon, Stephany Buenrostro
    Chen, Dexian
    Chen, Xuemeng
    Dias, Antonio
    Dommen, Josef
    Draper, Danielle C.
    Duplissy, Jonathan
    Ehn, Mikael
    Finkenzeller, Henning
    Fischer, Lukas
    Frege, Carla
    Fuchs, Claudia
    Garmash, Olga
    Gordon, Hamish
    Hakala, Jani
    He, Xucheng
    Heikkinen, Liine
    Heinritzi, Martin
    Helm, Johanna C.
    Hofbauer, Victoria
    Hoyle, Christopher R.
    Jokinen, Tuija
    Kangasluoma, Juha
    Kerminen, Veli-Matti
    Kim, Changhyuk
    Kirkby, Jasper
    Kontkanen, Jenni
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. University of Helsinki, Finland.
    Kuerten, Andreas
    Lawler, Michael J.
    Mai, Huajun
    Mathot, Serge
    Mauldin, Roy L.
    Molteni, Ugo
    Nichman, Leonid
    Nie, Wei
    Nieminen, Tuomo
    Ojdanic, Andrea
    Onnela, Antti
    Passananti, Monica
    Petaja, Tuukka
    Piel, Felix
    Pospisilova, Veronika
    Quelever, Lauriane L. J.
    Rissanen, Matti P.
    Rose, Clemence
    Sarnela, Nina
    Schallhart, Simon
    Schuchmann, Simone
    Sengupta, Kamalika
    Simon, Mario
    Sipila, Mikko
    Tauber, Christian
    Tome, Antonio
    Trostl, Jasmin
    Vaisanen, Olli
    Vogel, Alexander L.
    Volkamer, Rainer
    Wagner, Andrea C.
    Wang, Mingyi
    Weitz, Lena
    Wimmer, Daniela
    Ye, Penglin
    Ylisirnio, Arttu
    Zha, Qiaozhi
    Carslaw, Kenneth S.
    Curtius, Joachim
    Donahue, Neil M.
    Flagan, Richard C.
    Hansel, Armin
    Riipinen, Ilona
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. Tampere University of Technology, Finland.
    Virtanen, Annele
    Winkler, Paul M.
    Baltensperger, Urs
    Kulmala, Markku
    Worsnop, Douglas R.
    Multicomponent new particle formation from sulfuric acid, ammonia, and biogenic vapors2018In: Science Advances, E-ISSN 2375-2548, Vol. 4, no 12, article id eaau5363Article in journal (Refereed)
    Abstract [en]

    A major fraction of atmospheric aerosol particles, which affect both air quality and climate, form from gaseous precursors in the atmosphere. Highly oxygenated organic molecules (HOMs), formed by oxidation of biogenic volatile organic compounds, are known to participate in particle formation and growth. However, it is not well understood how they interact with atmospheric pollutants, such as nitrogen oxides (NOx) and sulfur oxides (SOx) from fossil fuel combustion, as well as ammonia (NH3) from livestock and fertilizers. Here, we show how NOx suppresses particle formation, while HOMs, sulfuric acid, and NH3 have a synergistic enhancing effect on particle formation. We postulate a novel mechanism, involving HOMs, sulfuric acid, and ammonia, which is able to closely reproduce observations of particle formation and growth in daytime boreal forest and similar environments. The findings elucidate the complex interactions between biogenic and anthropogenic vapors in the atmospheric aerosol system.

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