ALBERT

Description: About half of present-day cloud condensation nuclei originate from atmospheric nucleation, frequently appearing as a burst of new particles near midday. Atmospheric observations show that the growth rate of new particles often accelerates when the diameter of the particles is between one and ten nanometres. In this critical size range, new particles are most likely to be lost by coagulation with pre-existing particles, thereby failing to form new cloud condensation nuclei that are typically 50 to 100 nanometres across. Sulfuric acid vapour is often involved in nucleation but is too scarce to explain most subsequent growth, leaving organic vapours as the most plausible alternative, at least in the planetary boundary layer. Although recent studies predict that low-volatility organic vapours contribute during initial growth, direct evidence has been lacking. The accelerating growth may result from increased photolytic production of condensable organic species in the afternoon, and the presence of a possible Kelvin (curvature) effect, which inhibits organic vapour condensation on the smallest particles (the nano-Kohler theory), has so far remained ambiguous. Here we present experiments performed in a large chamber under atmospheric conditions that investigate the role of organic vapours in the initial growth of nucleated organic particles in the absence of inorganic acids and bases such as sulfuric acid or ammonia and amines, respectively. Using data from the same set of experiments, it has been shown that organic vapours alone can drive nucleation. We focus on the growth of nucleated particles and find that the organic vapours that drive initial growth have extremely low volatilities (saturation concentration less than 10(-4.5) micrograms per cubic metre). As the particles increase in size and the Kelvin barrier falls, subsequent growth is primarily due to more abundant organic vapours of slightly higher volatility (saturation concentrations of 10(-4.5) to 10(-0.5) micrograms per cubic metre). We present a particle growth model that quantitatively reproduces our measurements. Furthermore, we implement a parameterization of the first steps of growth in a global aerosol model and find that concentrations of atmospheric cloud concentration nuclei can change substantially in response, that is, by up to 50 per cent in comparison with previously assumed growth rate parameterizations.〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Trostl, Jasmin -- Chuang, Wayne K -- Gordon, Hamish -- Heinritzi, Martin -- Yan, Chao -- Molteni, Ugo -- Ahlm, Lars -- Frege, Carla -- Bianchi, Federico -- Wagner, Robert -- Simon, Mario -- Lehtipalo, Katrianne -- Williamson, Christina -- Craven, Jill S -- Duplissy, Jonathan -- Adamov, Alexey -- Almeida, Joao -- Bernhammer, Anne-Kathrin -- Breitenlechner, Martin -- Brilke, Sophia -- Dias, Antonio -- Ehrhart, Sebastian -- Flagan, Richard C -- Franchin, Alessandro -- Fuchs, Claudia -- Guida, Roberto -- Gysel, Martin -- Hansel, Armin -- Hoyle, Christopher R -- Jokinen, Tuija -- Junninen, Heikki -- Kangasluoma, Juha -- Keskinen, Helmi -- Kim, Jaeseok -- Krapf, Manuel -- Kurten, Andreas -- Laaksonen, Ari -- Lawler, Michael -- Leiminger, Markus -- Mathot, Serge -- Mohler, Ottmar -- Nieminen, Tuomo -- Onnela, Antti -- Petaja, Tuukka -- Piel, Felix M -- Miettinen, Pasi -- Rissanen, Matti P -- Rondo, Linda -- Sarnela, Nina -- Schobesberger, Siegfried -- Sengupta, Kamalika -- Sipila, Mikko -- Smith, James N -- Steiner, Gerhard -- Tome, Antonio -- Virtanen, Annele -- Wagner, Andrea C -- Weingartner, Ernest -- Wimmer, Daniela -- Winkler, Paul M -- Ye, Penglin -- Carslaw, Kenneth S -- Curtius, Joachim -- Dommen, Josef -- Kirkby, Jasper -- Kulmala, Markku -- Riipinen, Ilona -- Worsnop, Douglas R -- Donahue, Neil M -- Baltensperger, Urs -- England -- Nature. 2016 May 25;533(7604):527-31. doi: 10.1038/nature18271.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉Paul Scherrer Institute, Laboratory of Atmospheric Chemistry, CH-5232 Villigen, Switzerland. ; Carnegie Mellon University, Center for Atmospheric Particle Studies, Pittsburgh, Pennsylvania 15213, USA. ; CERN, CH-1211 Geneva, Switzerland. ; Goethe University Frankfurt, Institute for Atmospheric and Environmental Sciences, 60438 Frankfurt am Main, Germany. ; Department of Physics, University of Helsinki, PO Box 64, FI-00014 Helsinki, Finland. ; Department of Applied Environmental Science, University of Stockholm, SE-10961 Stockholm, Sweden. ; Institute for Atmospheric and Climate Science, ETH Zurich, 8092 Zurich, Switzerland. ; Chemical Sciences Division, Earth System Research Laboratory, NOAA, Boulder, Colorado, USA. ; Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, California 91125, USA. ; Helsinki Institute of Physics, University of Helsinki, PO Box 64, FI-00014 Helsinki, Finland. ; Institute for Ion and Applied Physics, University of Innsbruck, 6020 Innsbruck, Austria. ; Ionicon Analytik GmbH, 6020 Innsbruck, Austria. ; WSL Institute for Snow and Avalanche Research SLF, 7260 Davos, Switzerland. ; University of Eastern Finland, 70211 Kuopio, Finland. ; Finnish Meteorological Institute, 00101 Helsinki, Finland. ; National Center for Atmospheric Research, Atmospheric Chemistry Observations and Modeling Laboratory, Boulder, Colorado 80301, USA. ; Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, Karlsruhe, Germany. ; School of Earth and Environment, University of Leeds, LS2 9JT Leeds, UK. ; Department of Chemistry, University of California, Irvine, California 92697, USA. ; Faculty of Physics, University of Vienna, 1090 Vienna, Austria. ; SIM, University of Lisbon and University of Beira Interior, 1849-016 Lisbon, Portugal. ; Aerodyne Research, Inc., Billerica, Massachusetts 01821, USA.〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/27225126" target="_blank"〉PubMed〈/a〉

Description: Experiments were conducted to investigate light absorption of organic aerosol (OA) in fresh and photo-chemically aged biomass-burning emissions. The experiments considered residential hardwood fuel (oak) and fuels commonly consumed in wild-land and prescribed fires in the United States (pocosin pine and gallberry). Photo-chemical aging was performed in an environmental chamber. We constrained the effective light-absorption properties of the OA using conservative limiting assumptions, and found that both primary organic aerosol (POA) in the fresh emissions and secondary organic aerosol (SOA) produced by photo-chemical aging contain brown carbon, and absorb light to a significant extent. This work presents the first direct evidence that SOA produced in aged biomass-burning emissions is absorptive. For the investigated fuels, SOA is less absorptive than POA in the long visible, but exhibits stronger wavelength-dependence and is more absorptive in the short visible and near-UV. Light absorption by SOA in biomass-burning emissions might be an important contributor to the global radiative forcing budget.

Description: When NOx is introduced to organic emissions, aerosol production is sometimes, but not always, reduced. Under certain conditions, these interactions will instead increase aerosol concentrations. We expanded the two-dimensional volatility basis set (2-D-VBS) to include the effects of NOx on aerosol formation. This includes the formation of organonitrates, where the addition of a nitrate group contributes to a decrease of 2.5 orders of magnitude in volatility. With this refinement, we model outputs from experimental results, such as the atomic N : C ratio, organonitrate mass, and nitrate fragments in AMS measurements. We also discuss the mathematical methods underlying the implementation of the 2-D-VBS and provide the complete code in the Supplemental material. A developer version is available on Bitbucket, an online community repository.

Description: Experiments were conducted to investigate light absorption of organic aerosol (OA) in fresh and photo-chemically aged biomass-burning emissions. The experiments considered residential hardwood fuel (oak) and fuels commonly consumed in wild-land and prescribed fires in the United States (pocosin pine and gallberry). Photo-chemical aging was performed in an environmental chamber. We constrained the light-absorption properties of the OA using conservative limiting assumptions, and found that both primary organic aerosol (POA) in the fresh emissions and secondary organic aerosol (SOA) produced by photo-chemical aging absorb light to a significant extent, and are categorized as brown carbon. This work presents the first direct evidence that SOA produced in aged biomass-burning emissions is absorptive. For the investigated fuels, SOA is less absorptive than POA in the long visible, but exhibits steeper wavelength-dependence (larger Absorption Ångström Exponent) and is more absorptive in the short visible and near-UV. Light absorption by SOA in biomass-burning emissions might be an important contributor to the global radiative forcing budget.

Description: When NOx is introduced to organic emissions, aerosol production is sometimes, but not always, reduced. Under certain conditions, these interactions will instead increase aerosol concentrations. We expanded the two-dimensional volatility basis set (2D-VBS) to include the effects of NOx on aerosol formation. This includes the formation of organonitrates, where the addition of a nitrate group contributes to a decrease of 2.5 orders of magnitude in volatility. With this refinement, we model outputs from experimental results, such as the atomic N : C ratio, organonitrate mass, and nitrate fragments in Aerosol Mass Spectrometer (AMS) measurements. We also discuss the mathematical methods underlying the implementation of the 2D-VBS and provide the complete code in the Supplement. A developer version is available on Bitbucket, an online community repository.