scholarly journals Estimating neutral nanoparticle steady-state size distribution and growth according to measurements of intermediate air ions

2013 ◽  
Vol 13 (18) ◽  
pp. 9597-9603 ◽  
Author(s):  
H. Tammet ◽  
K. Komsaare ◽  
U. Hõrrak

Abstract. Continuous measurements of intermediate air ion size distributions were carried out in the small town Tartu, Estonia, from 1 April 2010 through 7 November 2011. The intermediate ions are charged aerosol particles of diameter 1.5–7.5 nm. In this paper we study what information about neutral nanoparticles of atmospheric aerosols can be drawn from the air ion measurements. Rough estimates of the growth rate and the size distribution of neutral nanoparticles were derived for the subset of measurements while the concentration of the intermediate ions was close to the median and remains in the range of 21 ± 2 cm−3. This criterion excludes the specific new particle formation events characterized with high concentration of intermediate ions and includes only most typical quiet periods between the events when the simultaneous growth, depletion and recharging of particles are described with steady-state equations. We estimated the growth rate of nanoparticles to be about 2 nm h−1 while the growth flux or apparent nucleation rate proved to be about 0.5 cm−3 s−1 at 3 nm and about 0.08 cm−3 s−1 at 7 nm. The results suggest that the process of new particle formation is not interrupted during the quiet periods between events of intensive nucleation of atmospheric aerosols.

2013 ◽  
Vol 13 (5) ◽  
pp. 13519-13540
Author(s):  
H. Tammet ◽  
K. Komsaare ◽  
U. Hõrrak

Abstract. The concentration of nanometer aerosol particles in atmospheric air during quiet periods of new particle formation is low and direct measuring is difficult. We study what information about neutral particles can be drawn from measurements of intermediate ions, which are the electrically charged particles between 1.5–7.5 nm in diameter. If the coagulation sink of nanoparticles and the growth rate of charged particles are known, then the steady state equations allow us to calculate the size distribution of neutral nanoparticles. Variations in the trial value of the growth rate have a minor effect on the estimates of the concentrations and size distributions. There exists a value of the constant growth rate of charged nanoparticles that leads to a minimum deviation of the estimated growth rate of neutral nanoparticles from the growth rate of charged nanoparticles. Rough estimates of the growth rate and size distribution of neutral nanoparticles are derived despite the fact that the sample data of intermediate ion measurements is not accompanied by simultaneous measurements of the background aerosol and ionization rate. In the case of a near-median intermediate ion concentration of 21 ± 2 cm−3 in the urban air of a small town, the growth rate of nanoparticles is estimated to be about 2 nm h−1, while the growth flux or apparent nucleation rate is about 0.5 cm−3 s−1 at 3 nm and about 0.08 cm−3 s−1 at 7 nm. The results suggest that the process of new particle formation is not interrupted during the quiet periods between events of intensive nucleation of atmospheric aerosols.


2010 ◽  
Vol 10 (4) ◽  
pp. 11361-11399 ◽  
Author(s):  
J. Boulon ◽  
K. Sellegri ◽  
H. Venzac ◽  
D. Picard ◽  
E. Weingartner ◽  
...  

Abstract. Aerosol nucleation is an important source of atmospheric particles which have an effect both on the climatic system and on human health. The new particle formation (NPF) process is an ubiquitous phenomenon, yet poorly understood despite the many studies performed on this topic using various approaches (observation, experimentation in smog chambers and modeling). In this work, we investigate the formation of secondary charged aerosols and its climatology at Jungfraujoch, a high altitude site in Swiss Alps (3580 m a.s.l.). Charged particles and clusters (0.5–1.8 nm) were measured within the EUCAARI program from April 2008 to April 2009 and allowed the detection of nucleation events. We found that the aerosol concentration, which is dominated by cluster size class, shows a strong diurnal pattern and that the aerosol size distribution and concentration are strongly influenced by the presence of clouds either during daytime or nighttime conditions. New particle formation events have been investigated and it appears that new particle formation occurs 17.5% of measured days and that the nucleation frequency is strongly linked to air mass origin and path and negatively influenced by cloud presence. In fact, we show that NPF events depend on the occurrence of high concentration VOCs air masses which allowed clusters growing by condensation of organic vapors rather than nucleation of new clusters. Furthermore, the contribution of ions to nucleation process was studied and we found that ion-mediated nucleation (IMN) contribute to 26% of the total nucleation so that ions play an important role in the new particle formation and growth at Jungfraujoch.


2012 ◽  
Vol 12 (20) ◽  
pp. 9923-9939 ◽  
Author(s):  
H. Guo ◽  
D. W. Wang ◽  
K. Cheung ◽  
Z. H. Ling ◽  
C. K. Chan ◽  
...  

Abstract. In order to investigate the formation and growth processes of nucleation mode particles, and to quantify the particle number (PN) concentration and size distributions in Hong Kong, an intensive field measurement was conducted from 25 October to 29 November in 2010 near the mountain summit of Tai Mo Shan, a suburban site approximately the geographical centre of the New Territories in Hong Kong. Based on observations of the particle size distribution, new particle formation (NPF) events were found on 12 out of 35 days with the estimated formation rate J5.5 from 0.97 to 10.2 cm−3 s−1, and the average growth rates from 1.5 to 8.4 nm h−1. The events usually began at 10:00–11:00 LT characterized by the occurrence of a nucleation mode with a peak diameter of 6–10 nm. Solar radiation, wind speed, sulfur dioxide (SO2) and ozone (O3) concentrations were on average higher, whereas temperature, relative humidity and daytime nitrogen dioxide (NO2) concentration were lower on NPF days than on non-NPF days. Back trajectory analysis suggested that in majority of the NPF event days, the air masses originated from the northwest to northeast directions. The concentrations of gaseous sulfuric acid (SA) showed good power-law relationship with formation rates, with exponents ranging from 1 to 2. The result suggests that the cluster activation theory and kinetic nucleation could potentially explain the observed NPF events in this mountainous atmosphere of Hong Kong. Meanwhile, in these NPF events, the contribution of sulfuric acid vapor to particle growth rate (GR5.5–25) ranged from 9.2 to 52.5% with an average of 26%. Measurement-based calculated oxidation rates of monoterpenes (i.e. α-pinene, β-pinene, myrcene and limonene) by O3 positively correlated with the GR5.5–25 (R = 0.80, p < 0.05). The observed associations of the estimated formation rate J5.5 and the growth rate GR5.5–25 with gaseous sulfuric acid and volatile organic compounds (VOCs) suggested the critical roles of sulfuric acid and biogenic VOCs (e.g. α-pinene and β-pinene) in these NPF events.


2019 ◽  
Author(s):  
Sophia Brilke ◽  
Nikolaus Fölker ◽  
Thomas Müller ◽  
Konrad Kandler ◽  
Xianda Gong ◽  
...  

Abstract. Atmospheric particle size distributions were measured in Paphos, Cyprus, during the A-LIFE (Absorbing aerosol layers in a changing climate: aging, lifetime and dynamics) field experiment from April 3–30, 2017. The newly developed DMA-train is deployed for the first time in an atmospheric environment for the direct measurement of the nucleation mode size range between 1.8–10 nm diameter. The DMA-train setup consists of seven size channels, of which five are set to fixed particle mobility diameters and two additional diameters are obtained by alternating voltage settings in one DMA every 10 s. In combination with a conventional Mobility Particle Size Spectrometer (MPSS) and an Aerodynamic Particle Sizer (APS) the complete atmospheric aerosol size distribution from 1.8 nm–10 µm is covered. The focus of the A-LIFE study is to characterize new particle formation (NPF) in the Eastern Mediterranean region at a measurement site with strong local pollution sources. The nearby Paphos airport was found to be a large emission source for nucleation mode particles and we analysed the size distribution of the airport emission plumes at approximately 500 m from the main runway. The analysis yielded 9 NPF events in 27 measurement days from the combined analysis of the DMA-train, MPSS and trace gas monitors. Growth rate calculations were performed and a size-dependency of the initial growth rate (


2020 ◽  
Vol 20 (9) ◽  
pp. 5645-5656 ◽  
Author(s):  
Sophia Brilke ◽  
Nikolaus Fölker ◽  
Thomas Müller ◽  
Konrad Kandler ◽  
Xianda Gong ◽  
...  

Abstract. Atmospheric particle size distributions were measured in Paphos, Cyprus, during the A-LIFE (absorbing aerosol layers in a changing climate: ageing, lifetime and dynamics) field experiment from 3 to 30 April 2017. The newly developed differential mobility analyser train (DMA-train) was deployed for the first time in an atmospheric environment for the direct measurement of the nucleation mode size range between 1.8 and 10 nm diameter. The DMA-train set-up consists of seven size channels, of which five are set to fixed particle mobility diameters and two additional diameters are obtained by alternating voltage settings in one DMA every 10 s. In combination with a conventional mobility particle size spectrometer (MPSS) and an aerodynamic particle sizer (APS) the complete atmospheric aerosol size distribution from 1.8 nm to 10 µm was covered. The focus of the A-LIFE study was to characterize new particle formation (NPF) in the eastern Mediterranean region at a measurement site with strong local pollution sources. The nearby Paphos airport was found to be a large emission source for nucleation mode particles, and we analysed the size distribution of the airport emission plumes at approximately 500 m from the main runway. The analysis yielded nine NPF events in 27 measurement days from the combined analysis of the DMA-train, MPSS and trace gas monitors. Growth rate calculations were performed, and a size dependency of the initial growth rate (<10 nm) was observed for one event case. Fast changes of the sub-10 nm size distribution on a timescale of a few minutes were captured by the DMA-train measurement during early particle growth and are discussed in a second event case. In two cases, particle formation and growth were detected in the nucleation mode size range which did not exceed the 10 nm threshold. This finding implies that NPF likely occurs more frequently than estimated from studies where the lower nanometre size regime is not covered by the size distribution measurements.


Author(s):  
Jiarong Liu ◽  
Ling Liu ◽  
Hui Rong ◽  
Xiuhui Zhang

Amino acids are recognized as significant components of atmospheric aerosols. However, its potential role in the atmospheric new particle formation (NPF) is poorly understood, especially aspartic acid (ASP), one of...


2015 ◽  
Vol 15 (21) ◽  
pp. 12283-12313 ◽  
Author(s):  
A. Lupascu ◽  
R. Easter ◽  
R. Zaveri ◽  
M. Shrivastava ◽  
M. Pekour ◽  
...  

Abstract. Accurate representation of the aerosol lifecycle requires adequate modeling of the particle number concentration and size distribution in addition to their mass, which is often the focus of aerosol modeling studies. This paper compares particle number concentrations and size distributions as predicted by three empirical nucleation parameterizations in the Weather Research and Forecast coupled with chemistry (WRF-Chem) regional model using 20 discrete size bins ranging from 1 nm to 10 μm. Two of the parameterizations are based on H2SO4, while one is based on both H2SO4 and organic vapors. Budget diagnostic terms for transport, dry deposition, emissions, condensational growth, nucleation, and coagulation of aerosol particles have been added to the model and are used to analyze the differences in how the new particle formation parameterizations influence the evolving aerosol size distribution. The simulations are evaluated using measurements collected at surface sites and from a research aircraft during the Carbonaceous Aerosol and Radiative Effects Study (CARES) conducted in the vicinity of Sacramento, California. While all three parameterizations captured the temporal variation of the size distribution during observed nucleation events as well as the spatial variability in aerosol number, all overestimated by up to a factor of 2.5 the total particle number concentration for particle diameters greater than 10 nm. Using the budget diagnostic terms, we demonstrate that the combined H2SO4 and low-volatility organic vapor parameterization leads to a different diurnal variability of new particle formation and growth to larger sizes compared to the parameterizations based on only H2SO4. At the CARES urban ground site, peak nucleation rates are predicted to occur around 12:00 Pacific (local) standard time (PST) for the H2SO4 parameterizations, whereas the highest rates were predicted at 08:00 and 16:00 PST when low-volatility organic gases are included in the parameterization. This can be explained by higher anthropogenic emissions of organic vapors at these times as well as lower boundary-layer heights that reduce vertical mixing. The higher nucleation rates in the H2SO4-organic parameterization at these times were largely offset by losses due to coagulation. Despite the different budget terms for ultrafine particles, the 10–40 nm diameter particle number concentrations from all three parameterizations increased from 10:00 to 14:00 PST and then decreased later in the afternoon, consistent with changes in the observed size and number distribution. We found that newly formed particles could explain up to 20–30 % of predicted cloud condensation nuclei at 0.5 % supersaturation, depending on location and the specific nucleation parameterization. A sensitivity simulation using 12 discrete size bins ranging from 1 nm to 10 μm diameter gave a reasonable estimate of particle number and size distribution compared to the 20 size bin simulation, while reducing the associated computational cost by ~ 36 %.


2019 ◽  
Vol 19 (18) ◽  
pp. 11985-12006 ◽  
Author(s):  
Peter J. Marinescu ◽  
Ezra J. T. Levin ◽  
Don Collins ◽  
Sonia M. Kreidenweis ◽  
Susan C. van den Heever

Abstract. A quality-controlled, 5-year dataset of aerosol number size distributions (particles with diameters (Dp) from 7 nm through 14 µm) was developed using observations from a scanning mobility particle sizer, aerodynamic particle sizer, and a condensation particle counter at the Department of Energy's Southern Great Plains (SGP) site. This dataset was used for two purposes. First, typical characteristics of the aerosol size distribution (number, surface area, and volume) were calculated for the SGP site, both for the entire dataset and on a seasonal basis, and size distribution lognormal fit parameters are provided. While the median size distributions generally had similar shapes (four lognormal modes) in all the seasons, there were some significant differences between seasons. These differences were most significant in the smallest particles (Dp<30 nm) and largest particles (Dp>800 nm). Second, power spectral analysis was conducted on this long-term dataset to determine key temporal cycles of total aerosol concentrations, as well as aerosol concentrations in specified size ranges. The strongest cyclic signal was associated with a diurnal cycle in total aerosol number concentrations that was driven by the number concentrations of the smallest particles (Dp<30 nm). This diurnal cycle in the smallest particles occurred in all seasons in ∼50 % of the observations, suggesting a persistent influence of new particle formation events on the number concentrations observed at the SGP site. This finding is in contrast with earlier studies that suggest new particle formation is observed primarily in the springtime at this site. The timing of peak concentrations associated with this diurnal cycle was shifted by several hours depending on the season, which was consistent with seasonal differences in insolation and boundary layer processes. Significant diurnal cycles in number concentrations were also found for particles with Dp between 140 and 800 nm, with peak concentrations occurring in the overnight hours, which were primarily associated with both nitrate and organic aerosol cycles. Weaker cyclic signals were observed for longer timescales (days to weeks) and are hypothesized to be related to the timescales of synoptic weather variability. The strongest periodic signals (3.5–5 and 7 d cycles) for these longer timescales varied depending on the season, with no cyclic signals and the lowest variability in the summer.


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