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

2017 ◽  
Author(s):  
Runlong Cai ◽  
Jingkun Jiang
Keyword(s):  
Large Fraction ◽  
Formation Rate ◽  
Particle Formation ◽  
Size Distributions ◽  
New Particle Formation ◽  
Scavenging Effect ◽  
Sink Term ◽  
Field Campaigns ◽  
New Formula ◽  
Clean Atmosphere

Abstract. A new balance formula to estimate new particle formation rate is proposed. It was derived from aerosol general dynamic equation in the discrete form and then converted into an approximately continuous form for analysing data from new particle formation (NPF) field campaigns. The new formula corrects the underestimation of the coagulation scavenging effect occurred in previously used formulae. It also clarifies the criterions in determining upper size bound in measured aerosol size distributions for estimating new particle formation rate. A NPF field campaign was carried out from March 7th to Apr. 7th, 2016, in urban Beijing, and a diethylene glycol scanning mobility particle spectrometer equipped with a miniature cylindrical differential mobility analyser was used to measure aerosol size distributions down to ~1 nm. 11 typical NPF events were observed during this period. Measured aerosol size distributions from 1 nm to 10 μm was used to test the new formula and those widely used ones. Previously used formulae that perform well in relatively clean atmosphere where 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. 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., formation rates of 1.5 nm particles in Beijing are underestimated by 58.9 % on average if neglecting coagulation among particles in nucleation mode.

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

2017 ◽  
Vol 17 (20) ◽  
pp. 12659-12675 ◽  
Author(s):  
Runlong Cai ◽  
Jingkun Jiang
Keyword(s):  
Large Fraction ◽  
Formation Rate ◽  
Particle Formation ◽  
Size Distributions ◽  
New Particle Formation ◽  
Scavenging Effect ◽  
Sink Term ◽  
Field Campaigns ◽  
New Formula ◽  
Clean Atmosphere

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.

scholarly journals New particle formation events in semi-clean South African savannah

2011 ◽  
Vol 11 (7) ◽  
pp. 3333-3346 ◽  
Author(s):  
V. Vakkari ◽  
H. Laakso ◽  
M. Kulmala ◽  
A. Laaksonen ◽  
D. Mabaso ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Growth Rate ◽  
Particle Size ◽  
Sulphuric Acid ◽  
Growth Rates ◽  
Formation Rate ◽  
Particle Formation ◽  
Size Distributions ◽  
New Particle Formation ◽  
Particle Formation And Growth

Abstract. This study is based on 18 months (20 July 2006–5 February 2008) of continuous measurements of aerosol particle size distributions, air ion size distributions, trace gas concentrations and basic meteorology in a semi-clean savannah environment in Republic of South Africa. New particle formation and growth was observed on 69% of the days and bursts of non-growing ions/sub-10 nm particles on additional 14% of the days. This new particle formation frequency is the highest reported from boundary layer so far. Also the new particle formation and growth rates were among the highest reported in the literature for continental boundary layer locations; median 10 nm formation rate was 2.2 cm−3 s−1 and median 10–30 nm growth rate 8.9 nm h−1. The median 2 nm ion formation rate was 0.5 cm−3 s−1 and the median ion growth rates were 6.2, 8.0 and 8.1 nm h−1 for size ranges 1.5–3 nm, 3–7 nm and 7–20 nm, respectively. The growth rates had a clear seasonal dependency with minimum during winter and maxima in spring and late summer. The relative contribution of estimated sulphuric acid to the growth rate was decreasing with increasing particle size and could explain more than 20% of the observed growth rate only for the 1.5–3 nm size range. Also the air mass history analysis indicated the highest formation and growth rates to be associated with the area of highest VOC (Volatile Organic Compounds) emissions following from biological activity rather than the highest estimated sulphuric acid concentrations. The frequency of new particle formation, however, increased nearly monotonously with the estimated sulphuric acid reaching 100% at H2SO4 concentration of 6 · 107 cm−3, which suggests the formation and growth to be independent of each other.

scholarly journals New particle formation events in semi-clean South African savannah

2010 ◽  
Vol 10 (12) ◽  
pp. 30777-30821 ◽  
Author(s):  
V. Vakkari ◽  
H. Laakso ◽  
M. Kulmala ◽  
A. Laaksonen ◽  
D. Mabaso ◽  
...  
Keyword(s):  
Growth Rate ◽  
Sulphuric Acid ◽  
Growth Rates ◽  
Formation Rate ◽  
Particle Formation ◽  
Size Distributions ◽  
New Particle Formation ◽  
Air Mass ◽  
History Analysis ◽  
Particle Formation And Growth

Abstract. This study is based on 18 months (20 July 2006–5 February 2008) of continuous measurements of aerosol particle size distributions, air ion size distributions, trace gas concentrations and basic meteorology in a semi-clean savannah environment in Republic of South Africa. New particle formation and growth was observed on 69% of the days and bursts of non-growing ions/sub-10 nm particles on additional 14% of the days. The new particle formation and growth rates were among the highest reported in the literature for continental boundary layer locations; median 10 nm formation rate was 2.2 cm−3s−1 and median 10–30 nm growth rate 8.9 nm h−1. The median 2 nm ion formation rate was 0.5 cm−3s−1 and the median ion growth rates were 6.2, 8.0 and 8.1 nm h−1 for size ranges 1.5–3 nm, 3–7 nm and 7–20 nm, respectively. Three different approaches were used to study the origin of the formation and growth rates: seasonal variation, air mass history analysis and estimated sulphuric acid contribution to the growth. The growth rates had a clear seasonal dependency with minimum during winter and maxima in spring and late summer and the air mass history analysis indicated the highest formation and growth rates to be associated with the area of highest VOC (Volatile Organic Compounds) emissions rather than the highest estimated sulphuric acid concentrations. The relative contribution of estimated sulphuric acid to the growth rate was decreasing with increasing particle size and could explain more than 20% of the observed growth rate only for the 1.5–3 nm size range. The implication is that the sulphuric acid alone is not enough to explain the growth, but the highest growth rates seem to originate in VOC emissions following from biological activity. The frequency of new particle formation, however, increased nearly monotonously with the estimated sulphuric acid reaching 100% at H2SO4 concentration of 4×107cm−3, which suggests the formation and growth to be independent of each other.

scholarly journals Long-term analysis of clear-sky new particle formation events and non-events in Hyytiälä

2016 ◽  
Author(s):  
Lubna Dada ◽  
Pauli Paasonen ◽  
Tuomo Nieminen ◽  
Stephany Buenrostro Mazon ◽  
Jenni Kontkanen ◽  
...  
Keyword(s):  
Formation Rate ◽  
Threshold Value ◽  
Particle Formation ◽  
New Particle Formation ◽  
Organic Vapors ◽  
Clear Sky ◽  
Sky Conditions ◽  
Oxidized Products ◽  
Condensation Sink

Abstract. New particle formation (NPF) events have been observed all around the world and are known to be a major source of atmospheric aerosol particles. Here we combine 20 years of observations in a boreal forest at the SMEAR II station (Station for Measuring Ecosystem-Atmosphere Relations) in Hyytiälä, Finland, by utilizing previously accumulated knowledge, and by focusing on clear-sky (non-cloudy) conditions. We first investigated the effect of cloudiness on NPF and then compared the NPF event and non-event days during clear-sky conditions. In this comparison we considered, for example, the effects of calculated particle formation rates, condensation sink, trace gas concentrations and various meteorological quantities. The formation rate of 1.5 nm particles was calculated by using proxies for gaseous sulfuric acid and oxidized products of low volatile organic compounds. As expected, our results indicate an increase in the frequency of NPF events under clear-sky conditions. Also, focusing on clearsky conditions enabled us to find a clear separation of many variables related to NPF. For instance, oxidized organic vapors showed higher concentration during the clear-sky NPF event days, whereas the condensation sink (CS) and some trace gases had higher concentrations during the non-event days. The calculated formation rate of 3 nm particles showed a notable difference between the NPF event and non-event days during clear-sky conditions, especially in winter and spring. For spring time, we are able to find a threshold value for the combined values of ambient temperature and CS, above which practically no clear-sky NPF event could be observed. Finally, we present a probability distribution for the frequency of NPF events at a specific CS and temperature.

scholarly journals Iodine speciation and size distribution in ambient aerosols at a coastal new particle formation hotspot in China

2019 ◽  
Vol 19 (6) ◽  
pp. 4025-4039 ◽  
Author(s):  
Huan Yu ◽  
Lili Ren ◽  
Xiangpeng Huang ◽  
Mingjie Xie ◽  
Jun He ◽  
...  
Keyword(s):  
Particle Formation ◽  
Coastal Areas ◽  
Aerosol Sample ◽  
Size Distributions ◽  
New Particle Formation ◽  
Nucleation Mode ◽  
Iodine Species ◽  
Organic Iodine ◽  
Iodine Compounds ◽  
Iodine Speciation

Abstract. Intense new particle formation (NPF) events were observed in the coastal atmosphere during algae growth and farming season at Xiangshan gulf of the east China coast. High nucleation-mode iodine concentrations measured by ultra-performance liquid chromatography coupled with quadrupole time-of-flight mass spectrometry (UPLC/Q-TOF-MS) confirmed that the NPF events were induced by iodine species. Our study provides important information on iodine speciation, size distributions, and its role in NPF in the context of heavy air pollution in China's coastal areas. For the first time, we identified 5 inorganic iodine species, 45 organic iodine compounds (35 molecular formulas), and a group of iodide–organic adducts in aerosols. The concentrations and size distributions of iodine species down to 10 nm were measured during the iodine-induced NPF, continental NPF, and non-NPF days at the coastal site and compared to those at an inland site. The iodine in the above four aerosol sample types were characterized by iodate, aromatic iodine compounds, iodoacetic acid or iodopropenoic acid, and iodide–organic adducts, respectively. Iodide and organic iodine compounds were found in the nucleation-mode particles; however, it is still not clear whether they contributed to nucleation or just new particle growth. Wild algae, as well as farmed algae, could be an important NPF source in China's coastal areas.

scholarly journals Quantifying aerosol size distributions and their temporal variability in the Southern Great Plains, USA

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
Keyword(s):  
Size Distribution ◽  
Great Plains ◽  
Diurnal Cycle ◽  
Particle Formation ◽  
Aerosol Size Distribution ◽  
Size Distributions ◽  
New Particle Formation ◽  
Scanning Mobility Particle Sizer ◽  
Southern Great Plains ◽  
Particle Sizer

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.

scholarly journals Characterization of Urban New Particle Formation in Amman—Jordan

Atmosphere ◽  
2020 ◽  
Vol 11 (1) ◽  
pp. 79 ◽  
Author(s):  
Tareq Hussein ◽  
Nahid Atashi ◽  
Larisa Sogacheva ◽  
Simo Hakala ◽  
Lubna Dada ◽  
...  
Keyword(s):  
Growth Rate ◽  
Eastern Mediterranean ◽  
Seasonal Pattern ◽  
Formation Rate ◽  
Particle Formation ◽  
New Particle Formation ◽  
Vapor Source ◽  
Back Trajectories ◽  
Pattern Maximum ◽  
The Mean

We characterized new particle formation (NPF) events in the urban background of Amman during August 2016–July 2017. The monthly mean of submicron particle number concentration was 1.2 × 104–3.7 × 104 cm−3 (exhibited seasonal, weekly, and diurnal variation). Nucleation mode (10–15 nm) concentration was 0.7 × 103–1.1 × 103 cm−3 during daytime with a sharp peak (1.1 × 103–1.8 × 103 cm−3) around noon. We identified 110 NPF events (≈34% of all days) of which 55 showed a decreasing mode diameter after growth. The NPF event occurrence was higher in summer than in winter, and events were accompanied with air mass back trajectories crossing over the Eastern Mediterranean. The mean nucleation rate (J10) was 1.9 ± 1.1 cm−3 s−1 (monthly mean 1.6–2.7 cm−3 s−1) and the mean growth rate was 6.8 ± 3.1 nm/h (4.1–8.8 nm/h). The formation rate did not have a seasonal pattern, but the growth rate had a seasonal variation (maximum around August and minimum in winter). The mean condensable vapor source rate was 4.1 ± 2.2 × 105 molecules/cm3 s (2.6–6.9 × 105 molecules/cm3 s) with a seasonal pattern (maximum around August). The mean condensation sink was 8.9 ± 3.3 × 10−3 s−1 (6.4–14.8 × 10−3 s−1) with a seasonal pattern (minimum around June and maximum in winter).

scholarly journals Nanoparticles in boreal forest and coastal environment: a comparison of observations and implications of the nucleation mechanism

2009 ◽  
Vol 9 (6) ◽  
pp. 26627-26651 ◽  
Author(s):  
K. Lehtipalo ◽  
M. Kulmala ◽  
M. Sipilä ◽  
T. Petäjä ◽  
M. Vana ◽  
...  
Keyword(s):  
Boreal Forest ◽  
Pulse Height ◽  
Particle Formation ◽  
Coastal Environment ◽  
Nucleation Mechanism ◽  
Limiting Factor ◽  
Size Distributions ◽  
New Particle Formation ◽  
Particle Size Distributions ◽  
Large Molecules

Abstract. The detailed mechanism of secondary new particle formation in the atmosphere is still under debate. It is proposed that particle formation happens via activation of 1–2 nm atmospheric neutral molecular clusters and/or large molecules. Since traditional instrumentation does not reach these sizes, the hypothesis has not yet been verified. By directly measuring particle size distributions down to mobility diameters of about 1.3 nm with a pulse-height CPC we provide evidence of the nucleation mechanism in coastal environment (Mace Head, Ireland) and in boreal forest (Hyytiälä, Finland). In both places neutral sub-3 nm condensation nuclei (nano-CN) were continuously present, even when no new particle formation was detected. In Mace Head, however, the concentration of the nano-CN was far too low to account for the particle formation rates during particle bursts. Thus the results imply that on coastal sites new particle formation initiates, as proposed earlier, via homogenous nucleation from biogenic iodine vapors. In contrary, activation of pre-existing nano-CN remains a possible explanation in the boreal forest, but the observed concentrations are not the limiting factor for the particle formation events.

scholarly journals On the formation of sulphuric acid-amine clusters in varying atmospheric conditions and its influence on atmospheric new particle formation

2012 ◽  
Vol 12 (5) ◽  
pp. 11485-11537 ◽  
Author(s):  
P. Paasonen ◽  
T. Olenius ◽  
O. Kupiainen ◽  
T. Kurtén ◽  
T. Petäjä ◽  
...  
Keyword(s):  
Relative Humidity ◽  
Sulphuric Acid ◽  
Acid Concentration ◽  
Formation Rate ◽  
Particle Formation ◽  
Atmospheric Conditions ◽  
New Particle Formation ◽  
Atmospheric Particle ◽  
Atmospheric Observations ◽  
Sulphuric Acid Concentration

Abstract. Sulphuric acid is a key component in atmospheric new particle formation. However, sulphuric acid alone does not form stable enough clusters to initiate particle formation in atmospheric conditions. Strong bases, such as amines, have been suggested to stabilize sulphuric acid clusters and thus participate in particle formation. We modelled the formation rate of clusters with two sulphuric acid and two amine molecules (JA2B2) at varying atmospherically relevant conditions with respect to concentrations of sulphuric acid ([H2SO4]), dimethylamine ([DMA]) and trimethylamine ([TMA]), temperature and relative humidity (RH). The modelled formation rates JA2B2 were functions of sulphuric acid concentration with close to quadratic dependence, which is in good agreement with atmospheric observations of the connection between the particle formation rate and sulphuric acid concentration. The coefficients KA2B2 connecting the cluster formation rate and sulphuric acid concentrations as JA2B2 = KA2B2[H2SO4]2 turned out to depend also on amine concentrations, temperature and relative humidity. We tested how the model results change if the clusters with two sulphuric acid and two amine molecules are assumed to act as seeds for heterogeneous nucleation of organic vapours (other than amines) with higher atmospheric concentrations than sulphuric acid. We also compared the modelled coefficients KA2B2 with the corresponding coefficients calculated from the atmospheric observations (Kobs) from environments with varying temperatures and levels of anthropogenic influence. By taking into account the modelled behaviour of JA2B2 as a function of [H2SO4], temperature and RH, the atmospheric particle formation rate was reproduced more closely than with the traditional semi-empirical formulae based on sulphuric acid concentration only. The formation rates of clusters with two sulphuric acid and two amine molecules with different amine compositions (DMA or TMA or one of both) had different responses to varying meteorological conditions and concentrations of vapours participating to particle formation. The observed inverse proportionality of the coefficient Kobs with RH and temperature agreed best with the modelled coefficient KA2B2 related to formation of a~cluster with two H2SO4 and one or two TMA molecules, assuming that these clusters can grow in collisions with abundant organic vapour molecules. In case this assumption is valid, our results suggest that the formation rate of clusters with at least two of both sulphuric acid and amine molecules might be the rate-limiting step for atmospheric particle formation. More generally, our analysis elucidates the sensitivity of the atmospheric particle formation rate to meteorological variables and concentrations of vapours participating in particle formation (also other than H2SO4).

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