Size Distributions of 3–10 Nm Atmospheric Particles: Implications for Nucleation Mechanisms

McMurry, Peter H.; Woo, Keung Shan; Weber, R. J.; Chen, Da‐Ren; Pui, David Y.H.

doi:10.1142/9781848161221_0005

Cited by 31 publications

(49 citation statements)

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“…Parallel measurements of nanoparticles down to 1 nm were made by two DEG systems (one from Brookhaven National Laboratory and the other from University of Minnesota) (Iida et al, 2009;Jiang et al, 2011a). The particle size distribution (PSD) system measured particles in a size range of 10-500 nm (McMurry et al, 2000;Woo et al, 2001;Iida, 2008;Iida et al, 2008). In order to improve the sensitivity in ambient measurements, the Cluster CIMS only measured selected ions such as deprotonated sulfuric acid clusters, clusters containing both sulfuric acid and various amines, with a typical cycle time of 5 min.…”

Section: Ambient Measurementsmentioning

confidence: 99%

Observation of neutral sulfuric acid-amine containing clusters in laboratory and ambient measurements

et al. 2011

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Abstract. Recent ab initio calculations showed that amines can enhance atmospheric sulfuric acid-water nucleation more effectively than ammonia, and this prediction has been substantiated in laboratory measurements. Laboratory studies have also shown that amines can effectively displace ammonia in several types of ammonium clusters. However, the roles of amines in cluster formation and growth at a microscopic molecular scale (from molecular sizes up to 2 nm)have not yet been well understood. Processes that must be understood include the incorporation of amines into sulfuric acid clusters and the formation of organic salts in freshly nucleated particles, which contributes significantly to particle growth rates. We report the first laboratory and ambient measurements of neutral sulfuric acid-amine clusters using the Cluster CIMS, a recently-developed mass spectrometer designed for measuring neutral clusters formed in the atmosphere during nucleation. An experimental technique, which we refer to as Semi-Ambient Signal Amplification (SASA), was employed. Sulfuric acid was added to ambient air, and the concentrations and composition of clusters in this mixture were analyzed by the Cluster CIMS. This experimental approach led to significantly higher cluster concentrations than are normally found in ambient air, thereby increasing signalto-noise levels and allowing us to study reactions between gas phase species in ambient air and sulfuric acid containing clusters. Mass peaks corresponding to clusters containing four H 2 SO 4 molecules and one amine molecule were clearly observed, with the most abundant sulfuric acid-amine clusters being those containing a C2-or C4-amine (i.e. amines with masses of 45 and 73 amu). Evidence for C3-and C5-amines (i.e. amines with masses of 59 and 87 amu) was also Correspondence to: J. Zhao (jzhao@ucar.edu)found, but their correlation with sulfuric acid tetramer was not as strong as was observed for the C2-and C4-amines. The formation mechanisms for those sulfuric acid-amine clusters were investigated by varying the residence time in the inlet. It was concluded that the amines react directly with neutral clusters and that ion-induced clustering of sulfuric acid cluster ions with amines was not a dominant process. Results from ambient measurements using the Cluster CIMS without addition of sulfuric acid have shown that the sulfuric acid-amine clusters were reasonably well correlated with sulfuric acid tetramer and consistent with the SASA experiments at the same Boulder sampling site. Also, clusters that contain C2-or C4-amines were more abundant and better correlated with sulfuric acid tetramer than other types of amine containing clusters. However, ambient measurements of sulfuric acid-amine clusters remain difficult and highly uncertain because their concentrations are only slightly above background levels, even during nucleation events.

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Section: Ambient Measurementsmentioning

confidence: 99%

Observation of neutral sulfuric acid-amine containing clusters in laboratory and ambient measurements

et al. 2011

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“…Identification of NPF and growth processes within urban atmosphere is more difficult than within rural or remote atmosphere (Kulmala et al, 2004a;Holmes, 2007). Numerous studies have focused on and devoted considerable efforts to NPF and growth over worldwide urban areas (Harrison et al, 2000;McMurry et al, 2000;Shi et al, 2001;Woo et al, 2001;Alam et al, 2003;Dunn et al, 2004;Zhang et al, 2004a;Shi et al, 2007;Hussein et al, 2008;Olofson et al, 2009). To date, only a few measurements on NPF events have been performed in the urban or suburban areas of China (Wehner et al, 2004;Wu et al, 2007;Liu et al, 2008;Gao et al, 2009;Yue et al, 2009;Yao et al, 2010;Shen et al, 2011;Zhang et al, 2011), which leads to an unclear outline of urban NPF and growth in this region.…”

Section: Introductionmentioning

confidence: 99%

Aerosol Size Spectra and Particle Formation Events at Urban Shanghai in Eastern China

Cheng

Zhang

et al. 2012

Aerosol Air Qual. Res.

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Aerosol number size distributions between 10 nm and 10 µm were measured from October 2008 to February 2009 in Shanghai, China. The average particle number, surface and volume concentrations were 1.3 × 10 4 1/cm 3 , 6.4 × 10 2 µm 2 /cm 3 and 64 µm 3 /cm 3 , respectively. Aitken particles dominated the total number of particles, and accumulated particles were the greatest contributor to particle surface area. Particle number size distributions could be characterized by multi-lognormal functions. The average number size distributions of aerosols revealed a clear diurnal pattern of two peaks within 30-60 nm corresponding to the morning and afternoon traffic rush hours. All size particles had two peaks in mean number concentrations during the rush hours, and 10-20 nm and 20-50 nm particles had one additional peak in late morning. The new particle formation events were found on four days out of 73. The apparent formation rates varied from 0.2 to 0.5 cm 3 /s, and the growth rates of newly formed particles were 3.3-5.5 nm/h. Overall, the new particle formation events had a significant impact on particle size spectra in the nucleation and Atiken modes, but insignificant effects on particle surface and volume concentrations.

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“…Correspondence to: F. Stratmann (straddi@tropos.de) Nucleation, usually detected as enhanced number concentration of particles in the size range below 10 nm, has been observed in Arctic areas (Wiedensohler et al, 1996;Pirjola et al, 1998), in marine locations (e.g., Hoppel et al, 1994;O'Dowd et al, 1999) and in continental locations, such as boreal forests (Mäkelä et al, 1997;Nilsson et al, 2001), remote (e.g., Weber et al, 1997), polluted sites (e.g., Birmili and Wiedensohler, 2000;McMurry et al, 2000), the free troposphere (Clarke, 1992;Schröder and Ström, 1997), and in the vicinity of evaporating clouds (Hegg et al, 1990;Wiedensohler et al, 1997;Keil and Wendisch, 2001).…”

Section: Introductionmentioning

confidence: 99%

New-particle formation events in a continental boundary layer: first results from the SATURN experiment

et al. 2003

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Abstract. During the SATURN experiment, which took place from 27 May to 14 June 2002, new particle formation in the continental boundary layer was investigated. Simultaneous ground-based and tethered-balloon-borne measurements were performed, including meteorological parameters, particle number concentrations and size distributions, gaseous precursor concentrations and SODAR and LIDAR observations.Newly formed particles were observed inside the residual layer, before the break-up process of the nocturnal inversion, and inside the mixing layer throughout the break-up of the nocturnal inversion and during the evolution of the planetary boundary layer.

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Size Distributions of 3–10 Nm Atmospheric Particles: Implications for Nucleation Mechanisms

Cited by 31 publications

References 0 publications

Observation of neutral sulfuric acid-amine containing clusters in laboratory and ambient measurements

Observation of neutral sulfuric acid-amine containing clusters in laboratory and ambient measurements

Aerosol Size Spectra and Particle Formation Events at Urban Shanghai in Eastern China

New-particle formation events in a continental boundary layer: first results from the SATURN experiment

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