Toward Direct Measurement of Atmospheric Nucleation

Kulmala, Markku; Riipinen, Ilona; Sipilä, Mikko; Manninen, Hanna E.; Petäj̈ä, Tuukka; Junninen, Heikki; Maso, Miikka Dal; Mordas, Genrik; Mirme, A.; Vana, Marko; Hirsikko, Anne; Laakso, Lauri; Harrison, Roy M.; Hanson, I.; Leung, Carl; Lehtinen, K. E. J.; Kerminen, Veli‐Matti

doi:10.1126/science.1144124

Cited by 508 publications

(523 citation statements)

References 25 publications

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“…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]. Recently, it has been proposed that nucleation of new particles happens by activation of thermodynamically stable clusters that are either charged [Horrak et al, 1998;Kulmala et al, 2000;Yu and Turco, 2008] or neutral [Kulmala et al, 2007], and continually present in the atmosphere. Many proposed nucleation mechanisms involve sulfuric acid and other highly soluble species [Curtius, 2006;Kuang et al, 2008].…”

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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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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“…Recent instrumental development has brought aerosol measurements down to the size of individual molecules and molecular clusters (Gamero-Castoño & Fernandez de la Mora 2000; Kulmala et al 2007b;Mirme et al 2007;Sipilä et al 2008;Winkler et al 2008a;Jiang et al 2011;Vanhanen et al 2011). Instruments that can detect even the smallest particles are needed for studying atmospheric nucleation (Kerminen et al 2010), and they can have various applications also in the fields of nanotechnology, medicine, etc.…”

Section: Introductionmentioning

confidence: 99%

Remarks on Ion Generation for CPC Detection Efficiency Studies in Sub-3-nm Size Range

Kangasluoma

Junninen

Lehtipalo

et al. 2013

Aerosol Science and Technology

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To calibrate a newly developed condensation particle counter, samples of known chemical composition are needed as the chemistry plays a role in the activation process. For that, we have built a calibration setup and produced ammonium sulfate, sodium chloride, tungsten oxide, silver, alkyl halide, and ionic liquid clusters down to 1 nm in mobility diameter in positive and negative mode. The chemical composition of most negatively charged clusters was solved using high-resolution mass spectrometer and we identified about 70% of the total signal of the mass spectrometer. For the Airmodus Particle Size Magnifier, which was the instrument to be calibrated, we measured cutoff diameters of 1.1, 1.3, 1.4, 1.6, and 1.6-1.8 nm for negative sodium chloride, ammonium sulfate, tungsten oxide, silver, and positive organics, respectively. From the alkyl halide and ionic liquid experiments, we concluded that the composition plays a bigger role than the charge state of the cluster in the activation process. We also showed that relative humidity of the sample flow can change the detection efficiency of the Particle Size Magnifier, which adds some uncertainties to the measured number concentrations.

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“…Here, we term such aerosols delayed primary aerosols, because particle precursors exist already in the undiluted exhaust and the amounts and characteristics of the resulting atmospheric particulate matter do not depend significantly on atmospheric processing or atmospheric photochemistry. In the secondary aerosol formation process driven by atmospheric photochemistry, volatile gaseous compounds emitted by traffic are chemically transformed in the atmosphere to less volatile species, enabling and enhancing secondary aerosol particle formation via condensation, as well as new particle formation (20-22) Whereas the primary and delayed primary particle emissions affect mostly the air quality near the emission source, the effects of the secondary processes are more important on a regional scale.Previous research has demonstrated the importance of nanosized clusters in atmospheric processes, especially in the formation of ultrafine particles (23,24). Some studies have also shown that nanosized clusters have a role in engine emission formation (4, 25).…”

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confidence: 99%

“…Previous research has demonstrated the importance of nanosized clusters in atmospheric processes, especially in the formation of ultrafine particles (23,24). Some studies have also shown that nanosized clusters have a role in engine emission formation (4, 25).…”

mentioning

confidence: 99%

Traffic is a major source of atmospheric nanocluster aerosol

Rönkkö

Kuuluvainen

Karjalainen

et al. 2017

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

209

132

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In densely populated areas, traffic is a significant source of atmospheric aerosol particles. Owing to their small size and complicated chemical and physical characteristics, atmospheric particles resulting from traffic emissions pose a significant risk to human health and also contribute to anthropogenic forcing of climate. Previous research has established that vehicles directly emit primary aerosol particles and also contribute to secondary aerosol particle formation by emitting aerosol precursors. Here, we extend the urban atmospheric aerosol characterization to cover nanocluster aerosol (NCA) particles and show that a major fraction of particles emitted by road transportation are in a previously unmeasured size range of 1.3-3.0 nm. For instance, in a semiurban roadside environment, the NCA represented 20-54% of the total particle concentration in ambient air. The observed NCA concentrations varied significantly depending on the traffic rate and wind direction. The emission factors of NCA for traffic were 2.4·10 15 (kg fuel ) −1 in a roadside environment, 2.6·10 15 (kg fuel ) −1 in a street canyon, and 2.9·10 15 (kg fuel ) −1 in an on-road study throughout Europe. Interestingly, these emissions were not associated with all vehicles. In engine laboratory experiments, the emission factor of exhaust NCA varied from a relatively low value of 1.6·10 12 (kg fuel ) −1 to a high value of 4.3·10 15 (kg fuel ) −1 . These NCA emissions directly affect particle concentrations and human exposure to nanosized aerosol in urban areas, and potentially may act as nanosized condensation nuclei for the condensation of atmospheric low-volatile organic compounds.nanocluster aerosol | atmospheric aerosol | combustion-derived nanoparticles | air pollution | traffic emission D etailed characterization of aerosol sources is required to understand climate impacts and health effects of atmospheric aerosols, as well as to develop technologies and policies capable of mitigating air pollution in urbanized areas. In densely populated areas, one of the most significant source of particles is traffic (1, 2). Owing to their small size and complicated chemical and physical characteristics (3-6), atmospheric particles resulting from traffic emissions pose a significant risk to human health (7-12), and also contribute to anthropogenic forcing of climate (13,14). Previous research on vehicular emissions has demonstrated the presence of soot and ash (3, 15) and solid sub-10-nm core particles (4-6) in primary emissions from vehicles and engines and their variation, depending on vehicle technologies (4, 6), the properties of fuels and lubricant oils (15, 16), and driving conditions (15-17). In addition to particles, exhaust typically contains species that reside in the gaseous phase in the undiluted high-temperature exhaust (5, 18, 19) but condense or even nucleate to the particle phase immediately after the exhaust is released to the atmosphere. Here, we term such aerosols delayed primary aerosols, because particle precursors exist already in the u...

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Toward Direct Measurement of Atmospheric Nucleation

Cited by 508 publications

References 25 publications

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

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

Remarks on Ion Generation for CPC Detection Efficiency Studies in Sub-3-nm Size Range

Traffic is a major source of atmospheric nanocluster aerosol

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