Organic aerosol formation via sulphate cluster activation

Kulmala, Markku; Kerminen, Veli‐Matti; Anttila, T.; Laaksonen, A.; O’Dowd, Colin

doi:10.1029/2003jd003961

Cited by 203 publications

(211 citation statements)

References 37 publications

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“…As a consequence, such results may help to revisit nucleation schemes implemented in all past simulations of the impact of volcanic eruptions on climate. Schemes involving a third species such as ammonium [ternary nucleation theory (24)] or the nano-Köhler theory of cluster activation (25) are examples of paths to explore to improve the representation of nucleation and particles growth to climate relevant sizes in global models.…”

Section: Discussionmentioning

confidence: 99%

Observations of nucleation of new particles in a volcanic plume

Boulon

Sellegri

Hervo

et al. 2011

Proc. Natl. Acad. Sci. U.S.A.

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Volcanic eruptions caused major weather and climatic changes on timescales ranging from hours to centuries in the past. Volcanic particles are injected in the atmosphere both as primary particles rapidly deposited due to their large sizes on time scales of minutes to a few weeks in the troposphere, and secondary particles mainly derived from the oxidation of sulfur dioxide. These particles are responsible for the atmospheric cooling observed at both regional and global scales following large volcanic eruptions. However, large condensational sinks due to preexisting particles within the plume, and unknown nucleation mechanisms under these circumstances make the assumption of new secondary particle formation still uncertain because the phenomenon has never been observed in a volcanic plume. In this work, we report the first observation of nucleation and new secondary particle formation events in a volcanic plume. These measurements were performed at the puy de Dôme atmospheric research station in central France during the Eyjafjallajokull volcano eruption in Spring 2010. We show that the nucleation is indeed linked to exceptionally high concentrations of sulfuric acid and present an unusual high particle formation rate. In addition we demonstrate that the binary H 2 SO 4 − H 2 O nucleation scheme, as it is usually considered in modeling studies, underestimates by 7 to 8 orders of magnitude the observed particle formation rate and, therefore, should not be applied in tropospheric conditions. These results may help to revisit all past simulations of the impact of volcanic eruptions on climate.secondary aerosols | volcanic sulfur | nanoparticles V olcanic eruptions and their impact on climate have been extensively investigated in geological archives such as sediments (1), ice cores (2-5), and through modeling studies (6, 7) but processes taking place in the volcanic plume have rarely been directly observed. The sulfur dioxide emitted in large amounts during explosive volcanic eruptions (8) can be oxidized to sulfuric acid, thus many authors suspect that the formed sulfuric acid gives rise to the formation of new secondary particle from binary homogeneous nucleation mechanism (1, 9-12). Those new particles can then affect the atmospheric radiative balance both directly and indirectly because they can act as cloud condensation nuclei (CCN) (13). This leads to a cooling effect, which is on a time scale from months to years, depending on the location of the eruption and the height at which volcanic gases were emitted.The Eyjafjallajokull volcano located in the south of Iceland [63°38′ N, 19°36′ W, summit 1,660 m above sea level (asl)] erupted on March 20, 2010. A major outbreak of the central crater under the covering ice cap followed on April 14, 2010 (Institute of Earth Sciences, 2010). A large volcanic plume composed of ashes and gases rose up to the tropopause level (approximately 10 km) for days and were observed by satellite and ground-based remote sensing instruments. The volcanic plume reached European altitude s...

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Section: Discussionmentioning

confidence: 99%

Observations of nucleation of new particles in a volcanic plume

Boulon

Sellegri

Hervo

et al. 2011

Proc. Natl. Acad. Sci. U.S.A.

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“…The onset of low or semi-volatile organic vapour condensation onto the nano-sized inorganic clusters is determined by Nano-Köhler theory, which describes the thermodynamic equilibrium between an inorganic cluster, water, and a water soluble organic compound. For further details of the thermodynamic model, we refer the reader to Kulmala et al (2004b). The particle water and ammonia content, on the other hand, is determined at every time step by equilibration of gaseous water and ammonia with the particulate sulphate and water-soluble organic fraction.…”

Section: Aerosol Dynamicsmentioning

confidence: 99%

MALTE – model to predict new aerosol formation in the lower troposphere

et al. 2006

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Abstract. The manuscript presents a detailed description of the meteorological and chemical code of Malte -a model to predict new aerosol formation in the lower troposphere. The aerosol dynamics are achieved by the new developed UHMA (University of Helsinki Multicomponent Aerosol Model) code with kinetic limited nucleation as responsible mechanism to form new clusters. First results indicate that the model is able to predict the on-and offset of new particle formation as well as the total aerosol number concentrations that were in good agreement with the observations. Further, comparison of predicted and measured H 2 SO 4 concentrations showed a satisfactory agreement. The simulation results indicated that at a certain transitional particle diameter (2-7 nm), organic molecules can begin to contribute significantly to the growth rate compared to sulphuric acid. At even larger particle sizes, organic molecules can dominate the growth rate on days with significant monoterpene concentrations. The intraday vertical evolution of newly formed clusters and particles in two different size ranges resulted in two maxima at the ground. These particles grow around noon to the detectable size range and agree well with measured vertical profiles.

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“…[2] Nucleation events are widespread in the atmospheric boundary layer [Kulmala et al, 2004]. Ambient measurements and modeling studies suggest that nucleated particles can grow into the size range of cloud condensation nuclei (CCN) in various environments ranging from remote continental to highly polluted [Kerminen et al, 2005;Laaksonen et al, 2005;Pirjola et al, 2002;Wang and Penner, 2009;Kuang et al, 2009;Wiedensohler et al, 2009].…”

Section: Introductionmentioning

confidence: 99%

Enhanced organic mass fraction and decreased hygroscopicity of cloud condensation nuclei (CCN) during new particle formation events

Dusek

Frank

Curtius

et al. 2010

Geophysical Research Letters

158

130

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[1] In a forested near-urban location in central Germany, the CCN efficiency of particles smaller than 100 nm decreases significantly during periods of new particle formation. This results in an increase of average activation diameters, ranging from 5 to 8% at supersaturations of 0.33% and 0.74%, respectively. At the same time, the organic mass fraction in the sub-100-nm size range increases from approximately 2/3 to 3/4. This provides evidence that secondary organic aerosol (SOA) components are involved in the growth of new particles to larger sizes, and that the reduced CCN efficiency of small particles is caused by the low hygroscopicity of the condensing material. The observed dependence of particle hygroscopicity (k) on chemical composition can be parameterized as a function of organic and inorganic mass fractions (f org , f inorg ) determined by aerosol mass spectrometry: k = k org f org + k inorg f inorg . The obtained value of k org % 0.1 is characteristic for SOA, and k inorg % 0.7 is consistent with the observed mix of ammonium, sulfate and nitrate ions. Citation: Dusek, U., G. P. Frank, J. Curtius, F. Drewnick, J. Schneider, A. Kürten, D. Rose, M. O. Andreae, S. Borrmann, and U. Pö schl (2010), Enhanced organic mass fraction and decreased hygroscopicity of cloud condensation nuclei (CCN) during new particle formation events, Geophys.

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Organic aerosol formation via sulphate cluster activation

Cited by 203 publications

References 37 publications

Observations of nucleation of new particles in a volcanic plume

Observations of nucleation of new particles in a volcanic plume

MALTE – model to predict new aerosol formation in the lower troposphere

Enhanced organic mass fraction and decreased hygroscopicity of cloud condensation nuclei (CCN) during new particle formation events

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