First Measurements of Neutral Atmospheric Cluster and 1–2 nm Particle Number Size Distributions During Nucleation Events

Jiang, Jingkun; Zhao, Jun; Chen, Modi; Eisele, F. L.; Scheckman, Jacob; Williams, Brent J.; Kuang, Chongai; McMurry, Peter H.

doi:10.1080/02786826.2010.546817

Cited by 129 publications

(152 citation statements)

References 17 publications

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“…The model is based on new measurements of neutral molecular clusters, particle number distributions down to about 1 nm geometric diameter (21), and precursor gas concentrations. Information about these studies is provided in Materials and Methods and in SI Text.…”

Section: Resultsmentioning

confidence: 99%

“…Model predictions, which require measurements of concentrations of sulfuric acid vapor and basic gaseous compounds, are compared with independent measurements of nucleation rates from intensive atmospheric campaign studies in Mexico City (2006) and Atlanta (2009). Details of these measurements and campaigns are described in previous publications (21,23,(32)(33)(34)(35)(36)(37)(38)(39). Additional information on Cluster CIMS measurements during the 2009 intensive study in Atlanta are provided in SI Text.…”

Section: Methodsmentioning

confidence: 99%

See 1 more Smart Citation

Acid–base chemical reaction model for nucleation rates in the polluted atmospheric boundary layer

Chen

Titcombe

Jiang

et al. 2012

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

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186

280

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Climate models show that particles formed by nucleation can affect cloud cover and, therefore, the earth's radiation budget. Measurements worldwide show that nucleation rates in the atmospheric boundary layer are positively correlated with concentrations of sulfuric acid vapor. However, current nucleation theories do not correctly predict either the observed nucleation rates or their functional dependence on sulfuric acid concentrations. This paper develops an alternative approach for modeling nucleation rates, based on a sequence of acid-base reactions. The model uses empirical estimates of sulfuric acid evaporation rates obtained from new measurements of neutral molecular clusters. The model predicts that nucleation rates equal the sulfuric acid vapor collision rate times a prefactor that is less than unity and that depends on the concentrations of basic gaseous compounds and preexisting particles. Predicted nucleation rates and their dependence on sulfuric acid vapor concentrations are in reasonable agreement with measurements from Mexico City and Atlanta.amines | atmospheric aerosol | climate forcing | nanoparticle | chamber study N ucleation of atmospheric trace gases occurs regularly throughout the continental boundary layer (1). Nucleated particles grow at typical rates of 1-10 nm/h, and can be a significant source of condensation nuclei (2) and cloud condensation nuclei (CCN) (3). The cloud albedo effect is a major source of uncertainty in estimates of climate radiative forcing (4). Because nucleation may affect CCN concentrations, there is a need for microphysical models that reliably predict atmospheric nucleation rates. Fig. 1 summarizes results for the dependence of boundary layer nucleation rates on the number concentration of sulfuric acid vapor, "[H 2 SO 4 ]," measured by the University of Minnesota-National Center for Atmospheric Research (NCAR) research team over the past two decades (5). Also included are data from the University of Helsinki group (6, 7). The considerable scatter in the measurements of the nucleation rate J at a given value of [H 2 SO 4 ] may be due to factors including dependencies on other nucleation precursor gases, temperature, and relative humidity (RH), as well as uncertainties introduced when J is deduced from measurements. Significantly, Fig. 1 shows that for all of these studies nucleation rates range from 1 × 10 −2 to 5 × 10 −6 times the sulfuric acid vapor collision rate, 0.5k 11 [H 2 SO 4 ] 2 , where k 11 is the hard-sphere collision rate constant for sulfuric acid vapor (8).The literature includes a lively debate about the relative importance of ion-induced and neutral nucleation (9, 10). Our work aims to explain nucleation rates observed in the polluted boundary layer atmospheres of Atlanta and Mexico City, where estimated nucleation rates (∼1-10 3 cm −3 ·s −1 ) were often much greater than typical ion production rates (∼2-30 cm −3 ·s −1 ). Therefore, although ion-induced nucleation could contribute to particle production in these locations it is not the dominant ...

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Section: Resultsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Acid–base chemical reaction model for nucleation rates in the polluted atmospheric boundary layer

Chen

Titcombe

Jiang

et al. 2012

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

Self Cite

186

280

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“…Measuring sub-3 nm electrically neutral particles is challenging, and therefore their growth rates have been indirectly deduced from the time lag between the rise in sulfuric acid concentration and the increase in the concentration of 3 nm particles (Weber et al, 1997;Sihto et al, 2006). However, recent instrumental development has enabled the detection of neutral clusters with mobility diameters of down to ∼ 1 nm by using instruments such as the DEG-SMPS (Jiang et al, 2011) and the PSM (Particle Size Magnifier; Vanhanen et al, 2011). Consequently, the growth rates in the sub-3 nm size range have been assessed, for example, by fitting the size distributions measured with a DEG-SMPS to the GDE (Kuang et al, 2012) or by determining the times at which the onset of new particle formation is detected with condensation particle counters with different cutoff sizes (Riccobono et al, 2012).…”

Section: Introductionmentioning

confidence: 99%

Growth of atmospheric clusters involving cluster–cluster collisions: comparison of different growth rate methods

Kontkanen

Olenius²,

Lehtipalo

et al. 2016

Atmos. Chem. Phys.

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Abstract. We simulated the time evolution of atmospheric cluster concentrations in a one-component system where not only do clusters grow by condensation of monomers, but cluster-cluster collisions also significantly contribute to the growth of the clusters. Our aim was to investigate the consistency of the growth rates of sub-3 nm clusters determined with different methods and the validity of the common approach to use them to estimate particle formation rates. We compared the growth rate corresponding to particle fluxes (FGR), the growth rate derived from the appearance times of clusters (AGR), and the growth rate calculated based on irreversible vapor condensation (CGR). We found that the relation between the different growth rates depends strongly on the external conditions and the properties of the model substance. The difference between the different growth rates was typically highest at the smallest, sub-2 nm sizes. FGR was generally lower than AGR and CGR; at the smallest sizes the difference was often very large, while at sizes larger than 2 nm the growth rates were closer to each other. AGR and CGR were in most cases close to each other at all sizes. The difference between the growth rates was generally lower in conditions where cluster concentrations were high, and evaporation and other losses were thus less significant. Furthermore, our results show that the conventional method used to determine particle formation rates from growth rates may give estimates far from the true values. Thus, care must be taken not only in how the growth rate is determined but also in how it is applied.

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“…Recent developments in diethylene glycol (DEG) condensation particle counters (CPCs; Iida et al, 2009;Vanhanen et al, 2011) have made it feasible to develop new scanning mobility particle spectrometers (SMPSs) for extending aerosol size distribution measurement from ∼ 3 nm down to ∼ 1 nm (Jiang et al, 2011a;Franchin et al, 2016). These new spectrometers were deployed in atmospheric observations (Jiang et al, 2011b) and in chamber measurements (Franchin et al, 2016) to study NPF. A miniature cylindrical differential mobility analyzer (mini-cyDMA; Cai et al, 2017) was developed to improve the performance of the DEG-SMPS.…”

Section: Introductionmentioning

confidence: 99%

A new balance formula to estimate new particle formation rate: reevaluating the effect of coagulation scavenging

Cai

Jiang

2017

Atmos. Chem. Phys.

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Abstract.A new balance formula to estimate new particle formation rate is proposed. It is derived from the aerosol general dynamic equation in the discrete form and then converted into an approximately continuous form for analyzing data from new particle formation (NPF) field campaigns. The new formula corrects the underestimation of the coagulation scavenging effect that occurred in the previously used formulae. It also clarifies the criteria for determining the upper size bound in measured aerosol size distributions for estimating new particle formation rate. An NPF field campaign was carried out from 7 March to 7 April 2016 in urban Beijing, and a diethylene glycol scanning mobility particle spectrometer equipped with a miniature cylindrical differential mobility analyzer was used to measure aerosol size distributions down to ∼ 1 nm. Eleven typical NPF events were observed during this period. Measured aerosol size distributions from 1 nm to 10 µm were used to test the new formula and the formulae widely used in the literature. The previously used formulae that perform well in a relatively clean atmosphere in which nucleation intensity is not strong were found to underestimate the comparatively high new particle formation rate in urban Beijing because of their underestimation or neglect of the coagulation scavenging effect. The coagulation sink term is the governing component of the estimated formation rate in the observed NPF events in Beijing, and coagulation among newly formed particles contributes a large fraction to the coagulation sink term. Previously reported formation rates in Beijing and in other locations with intense NPF events might be underestimated because the coagulation scavenging effect was not fully considered; e.g., estimated formation rates of 1.5 nm particles in this campaign using the new formula are 1.3-4.3 times those estimated using the formula neglecting coagulation among particles in the nucleation mode.

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First Measurements of Neutral Atmospheric Cluster and 1–2 nm Particle Number Size Distributions During Nucleation Events

Cited by 129 publications

References 17 publications

Acid–base chemical reaction model for nucleation rates in the polluted atmospheric boundary layer

Acid–base chemical reaction model for nucleation rates in the polluted atmospheric boundary layer

Growth of atmospheric clusters involving cluster–cluster collisions: comparison of different growth rate methods

A new balance formula to estimate new particle formation rate: reevaluating the effect of coagulation scavenging

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