scholarly journals On the roles of sulphuric acid and low-volatility organic vapours in the initial steps of atmospheric new particle formation

2010 ◽  
Vol 10 (22) ◽  
pp. 11223-11242 ◽  
Author(s):  
P. Paasonen ◽  
T. Nieminen ◽  
E. Asmi ◽  
H. E. Manninen ◽  
T. Petäjä ◽  
...  
Keyword(s):  
Sulphuric Acid ◽  
Acid Concentration ◽  
Nucleation Rate ◽  
Formation Rate ◽  
Particle Formation ◽  
New Particle Formation ◽  
Relative Contribution ◽  
Homogenous Nucleation ◽  
Order Of Magnitude ◽  
Sulphuric Acid Concentration

Abstract. Sulphuric acid and organic vapours have been identified as the key components in the ubiquitous secondary new particle formation in the atmosphere. In order to assess their relative contribution and spatial variability, we analysed altogether 36 new particle formation events observed at four European measurement sites during EUCAARI campaigns in 2007–2009. We tested models of several different nucleation mechanisms coupling the formation rate of neutral particles (J) with the concentration of sulphuric acid ([H2SO4]) or low-volatility organic vapours ([org]) condensing on sub-4 nm particles, or with a combination of both concentrations. Furthermore, we determined the related nucleation coefficients connecting the neutral nucleation rate J with the vapour concentrations in each mechanism. The main goal of the study was to identify the mechanism of new particle formation and subsequent growth that minimizes the difference between the modelled and measured nucleation rates. At three out of four measurement sites – Hyytiälä (Finland), Melpitz (Germany) and San Pietro Capofiume (Italy) – the nucleation rate was closely connected to squared sulphuric acid concentration, whereas in Hohenpeissenberg (Germany) the low-volatility organic vapours were observed to be dominant. However, the nucleation rate at the sulphuric acid dominant sites could not be described with sulphuric acid concentration and a single value of the nucleation coefficient, as K in J=K [H2SO4]2, but the median coefficients for different sites varied over an order of magnitude. This inter-site variation was substantially smaller when the heteromolecular homogenous nucleation between H2SO4 and organic vapours was assumed to take place in addition to homogenous nucleation of H2SO4 alone, i.e., J=KSA1[H2SO4]2+KSA2[H2SO4][org]. By adding in this equation a term describing homomolecular organic vapour nucleation, Ks3[org]2, equally good results were achieved. In general, our results suggest that organic vapours do play a role, not only in the condensational growth of the particles, but also in the nucleation process, with a site-specific degree.

scholarly journals On the roles of sulphuric acid and low-volatility organic vapours in the initial steps of atmospheric new particle formation

2010 ◽  
Vol 10 (5) ◽  
pp. 11795-11850 ◽  
Author(s):  
P. Paasonen ◽  
T. Nieminen ◽  
E. Asmi ◽  
H. E. Manninen ◽  
T. Petäjä ◽  
...  
Keyword(s):  
Sulphuric Acid ◽  
Acid Concentration ◽  
Nucleation Rate ◽  
Formation Rate ◽  
Particle Formation ◽  
New Particle Formation ◽  
Relative Contribution ◽  
Homogenous Nucleation ◽  
Condensational Growth ◽  
Sulphuric Acid Concentration

Abstract. Sulphuric acid and organic vapours have been identified as the key components in the ubiquitous secondary new particle formation in the atmosphere. In order to assess their relative contribution and spatial variability, we analyzed altogether 36 new particle formation events observed at four European measurement sites during EUCAARI campaigns in 2007–2009. We tested models of several different nucleation mechanisms coupling the formation rate of neutral particles (J) with the concentration of sulphuric acid ([H2SO4]) or low-volatility organic vapours ([org]) condensing on sub-4 nm particles, or with a combination of both concentrations. Furthermore, we determined the related nucleation coefficients connecting the neutral nucleation rate J with the vapour concentrations in each mechanism. The main goal of the study was to identify the mechanism of new particle formation and subsequent growth that minimizes the difference between the modeled and measured nucleation rates. At three out of four measurement sites – Hyytiälä (Finland), Melpitz (Germany) and San Pietro Capofiume (Italy) – the nucleation rate was closely connected to squared sulphuric acid concentration, whereas in Hohenpeissenberg (Germany) the low-volatility organic vapours were observed to be dominant. However, the nucleation rate at the sulphuric acid dominant sites could not be described with sulphuric acid concentration and a single value of the nucleation coefficient, as K in J=K [H2SO4]2, but the coefficients seemed to vary between the sites. This inter-site variation was substantially smaller when the heteromolecular homogenous nucleation between H2SO4 and organic vapours was assumed to take place in addition to homogenous nucleation of H2SO4 alone, i.e. J=KSA1 [H2SO4]2+KSA2 [H2SO4][org]. By adding in this equation a term describing homomolecular organic vapour nucleation, Ks3 [org]2, equally good results were achieved. In general, our results suggest that organic vapours do play a role, not only in the condensational growth of the particles, but as well in the nucleation process, with a site specific degree.

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).

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 (19) ◽  
pp. 9113-9133 ◽  
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). We also tested how the model results change if we assume that the clusters with two sulphuric acid and two amine molecules would act as seeds for heterogeneous nucleation of organic vapours (other than amines) with higher atmospheric concentrations than sulphuric acid. 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 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 in 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).

scholarly journals Effect of ions on the measurement of sulphuric acid in the CLOUD experiment at CERN

2014 ◽  
Vol 7 (7) ◽  
pp. 6595-6624
Author(s):  
L. Rondo ◽  
A. Kürten ◽  
S. Ehrhart ◽  
S. Schobesberger ◽  
A. Franchin ◽  
...  
Keyword(s):  
Sulphuric Acid ◽  
Mass Spectrometer ◽  
Acid Concentration ◽  
Particle Formation ◽  
Galactic Cosmic Rays ◽  
Cloud Chamber ◽  
Proton Synchrotron ◽  
Ionization Mass ◽  
New Particle Formation ◽  
Sulphuric Acid Concentration

Abstract. Ternary aerosol nucleation experiments were conducted in the CLOUD chamber at CERN in order to investigate the influence of ions on new particle formation. Neutral and ion-induced nucleation experiments, i.e., with and without the presence of ions, were carried out under precisely controlled conditions. The sulphuric acid concentration was measured with a Chemical Ionization Mass Spectrometer (CIMS) during the new particle formation experiments. The added ternary trace gases were ammonia (NH3), dimethylamine (DMA, C2H7N) or oxidised products of pinanediol (PD, C10H18O2). When pinanediol was introduced into the chamber, an increase in the mass spectrometric signal used to determine the sulphuric acid concentration (m/z 97, i.e., HSO4−) was observed due to ions from the CLOUD chamber. The enhancement was only observed during ion-induced nucleation measurements by using either galactic cosmic rays (GCR) or the proton synchrotron (PS) pion beam for the ion generation, respectively. The ion effect typically involved an increase in the apparent sulphuric acid concentration by a factor of ~2 to 3 and was qualitatively verified by the ion measurements by an Atmospheric Pressure interface-Time Of Flight (APi-TOF) mass spectrometer. By applying a high voltage (HV) clearing field inside the CLOUD chamber the ion effect on the CIMS measurement was completely eliminated since, under these conditions, small ions are swept from the chamber in about one second. In order to exclude the ion effect and to provide corrected sulphuric acid concentrations during the GCR and PS beam nucleation experiments, a parameterisation was derived that utilizes the trace gas concentrations and the UV light intensity as input parameters. Atmospheric sulphuric acid measurements with a CIMS showed an insignificant ion effect.

scholarly journals Atmospheric sulphuric acid and aerosol formation: implications from atmospheric measurements for nucleation and early growth mechanisms

2006 ◽  
Vol 6 (12) ◽  
pp. 4079-4091 ◽  
Author(s):  
S.-L. Sihto ◽  
M. Kulmala ◽  
V.-M. Kerminen ◽  
M. Dal Maso ◽  
T. Petäjä ◽  
...  
Keyword(s):  
Time Delay ◽  
Sulphuric Acid ◽  
Acid Concentration ◽  
Particle Formation ◽  
Early Growth ◽  
Activation Mechanism ◽  
Aerosol Formation ◽  
Atmospheric Measurements ◽  
Nucleation Mechanisms ◽  
Sulphuric Acid Concentration

Abstract. We have investigated the formation and early growth of atmospheric secondary aerosol particles building on atmospheric measurements. The measurements were part of the QUEST 2 campaign which took place in spring 2003 in Hyytiälä (Finland). During the campaign numerous aerosol particle formation events occurred of which 15 were accompanied by gaseous sulphuric acid measurements. Our detailed analysis of these 15 events is focussed on nucleation and early growth (to a diameter of 3 nm) of fresh particles. It revealed that new particle formation seems to be a function of the gaseous sulphuric acid concentration to the power from one to two when the time delay between the sulphuric acid and particle number concentration is taken into account. From the time delay the growth rates of freshly nucleated particles from 1 nm to 3 nm were determined. The mean growth rate was 1.2 nm/h and it was clearly correlated with the gaseous sulphuric acid concentration. We tested two nucleation mechanisms – recently proposed cluster activation and kinetic type nucleation – as possible candidates to explain the observed dependences, and determined experimental nucleation coefficients. We found that some events are dominated by the activation mechanism and some by the kinetic mechanism. Inferred coefficients for the two nucleation mechanisms are the same order of magnitude as chemical reaction coefficients in the gas phase and they correlate with the product of gaseous sulphuric acid and ammonia concentrations. This indicates that besides gaseous sulphuric acid also ammonia has a role in nucleation.

scholarly journals Aerosol dynamics simulations on the connection of sulphuric acid and new particle formation

2009 ◽  
Vol 9 (9) ◽  
pp. 2933-2947 ◽  
Author(s):  
S.-L. Sihto ◽  
H. Vuollekoski ◽  
J. Leppä ◽  
I. Riipinen ◽  
V.-M. Kerminen ◽  
...  
Keyword(s):  
Sulphuric Acid ◽  
Acid Concentration ◽  
Linear Dependence ◽  
Particle Number ◽  
Particle Formation ◽  
Number Concentration ◽  
Particle Number Concentration ◽  
Aerosol Dynamics ◽  
Sulphuric Acid Concentration ◽  
Acid Dependence

Abstract. We have performed a series of simulations with an aerosol dynamics box model to study the connection between new particle formation and sulphuric acid concentration. For nucleation either activation mechanism with a linear dependence on the sulphuric acid concentration, kinetic mechanism with a squared dependence on the sulphuric acid concentration or ternary H2O-H2SO4-NH3 nucleation was assumed. The aim was to study the factors that affect the sulphuric acid dependence during the early stages of particle growth, and specifically to find conditions which would yield the linear dependence between the particle number concentration at 3–6 nm and sulphuric acid, as observed in field experiments. The simulations showed that the correlation with sulphuric acid may change during the growth from nucleation size to 3–6 nm size range, the main reason being the size dependent growth rate between 1 and 3 nm. In addition, the assumed size for the nucleated clusters had a crucial impact on the sulphuric acid dependence at 3 nm. A linear dependence between the particle number concentration at 3 nm and sulphuric acid was achieved, when activation nucleation mechanism was used with a low saturation vapour pressure for the condensable organic vapour, or with nucleation taking place at ~2 nm instead of ~1 nm. Simulations with activation, kinetic and ternary nucleation showed that ternary nucleation reproduces too steep dependence on sulphuric acid as compared to the linear or square dependence observed in field measurements.

scholarly journals Global analysis of continental boundary layer new particle formation based on long-term measurements

2018 ◽  
Author(s):  
Tuomo Nieminen ◽  
Veli-Matti Kerminen ◽  
Tuukka Petäjä ◽  
Pasi P. Aalto ◽  
Mikhail Arshinov ◽  
...  
Keyword(s):  
Growth Rate ◽  
Growth Rates ◽  
Urban Areas ◽  
Global Analysis ◽  
Formation Rate ◽  
Particle Formation ◽  
Urban Environments ◽  
New Particle Formation ◽  
The World ◽  
Order Of Magnitude

Abstract. Atmospheric new particle formation (NPF) is an important phenomenon in terms of the global particle number concentrations. Here we investigated the frequency of NPF, formation rates of 10 nm particles and growth rates in the size range of 10–25 nm using at least one year of aerosol number size-distribution observations at 36 different locations around the world. The majority of these measurement sites are in the Northern Hemisphere. We found that the NPF frequency has a strong seasonal variability, taking place on about 30 % of the days in March–May and on about 10 % of the days in December–February. The median formation rate of 10 nm particles varies by about three orders of magnitude (0.01–10 cm−3 s−1) and the growth rate by about an order of magnitude (1–10 nm h−1). The smallest values of both formation and growth rates were observed at polar sites and the largest ones in urban environments or anthropogenically influenced rural sites. The correlation between the NPF event frequency and the particle formation and growth rate was at best moderate between the different measurement sites, as well as between the sites belonging to a certain environmental regime. For a better understanding of atmospheric NPF and its regional importance, we would need more observational data from different urban areas in practically all parts of the world, from additional remote and rural locations in Northern America, Asia and most of the Southern Hemisphere (especially Australia), from polar areas, and from at least a few locations over the oceans.

scholarly journals Evaluation of the accuracy of analysis tools for atmospheric new particle formation

2011 ◽  
Vol 11 (7) ◽  
pp. 3051-3066 ◽  
Author(s):  
H. Korhonen ◽  
S.-L. Sihto ◽  
V.-M. Kerminen ◽  
K. E. J. Lehtinen
Keyword(s):  
Nucleation Rate ◽  
Formation Rate ◽  
Regression Line ◽  
Particle Formation ◽  
Nucleation Mechanism ◽  
New Particle Formation ◽  
Critical Cluster ◽  
Theoretical Understanding ◽  
Analysis Tools ◽  
Combining Data

Abstract. Several mathematical tools have been developed in recent years to analyze new particle formation rates and to estimate nucleation rates and mechanisms at sub-3 nm sizes from atmospheric aerosol data. Here we evaluate these analysis tools using 1239 numerical nucleation events for which the nucleation mechanism and formation rates were known exactly. The accuracy of the estimates of particle formation rate at 3 nm (J3) showed significant sensitivity to the details of the analysis, i.e. form of equations used and assumptions made about the initial size of nucleating clusters, with the fraction of events within a factor-of-two accuracy ranging from 43–97%. In general, the estimates of the actual nucleation rate at 1.5 nm (J1.5) were less accurate, and even the most accurate analysis set-up estimated only 59% of the events within a factor of two of the simulated mean nucleation rate. The J1.5 estimates were deteriorated mainly by the size dependence of the cluster growth rate below 3 nm, which the analysis tools do not take into account, but also by possible erroneous assumptions about the initial cluster size. The poor estimates of J1.5 can lead to large uncertainties in the nucleation prefactors (i.e. constant P in nucleation equation J1.5 = P × [H2SO4]k). Large uncertainties were found also in the procedures that are used to determine the nucleation mechanism. When applied to individual events, the analysis tools clearly overestimated the number of H2SO4 molecules in a critical cluster for most events, and thus associated them with a wrong nucleation mechanism. However, in some conditions the number of H2SO4 molecules in a critical cluster was underestimated. This indicates that analysis of field data that implies a maximum of 2 H2SO4 molecules in a cluster does not automatically rule out a higher number of molecules in the actual nucleating cluster. Our analysis also suggests that combining data from several new particle formation events to scatter plots of H2SO4 vs formation rates (J1.5 or J3) and determining the slope of the regression line may not give reliable information about the nucleation mechanism. Overall, while the analysis tools for new particle formation are useful for getting order-of-magnitude estimates of parameters related to atmospheric nucleation, one should be very cautious in interpreting the results. It is, for example, possible that the tools may have misdirected our theoretical understanding of the nucleation mechanism.

scholarly journals EUCAARI ion spectrometer measurements at 12 European sites – analysis of new particle formation events

2010 ◽  
Vol 10 (16) ◽  
pp. 7907-7927 ◽  
Author(s):  
H. E. Manninen ◽  
T. Nieminen ◽  
E. Asmi ◽  
S. Gagné ◽  
S. Häkkinen ◽  
...  
Keyword(s):  
Formation Rate ◽  
Charged Particles ◽  
Particle Formation ◽  
Nucleation And Growth ◽  
Spatial And Temporal Variation ◽  
New Particle Formation ◽  
Continental Scale ◽  
Relative Contribution ◽  
Total Particle ◽  
Integrated Project

Abstract. We present comprehensive results on continuous atmospheric cluster and particle measurements in the size range ~1–42 nm within the European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) project. We focused on characterizing the spatial and temporal variation of new particle formation events and relevant particle formation parameters across Europe. Different types of air ion and cluster mobility spectrometers were deployed at 12 field sites across Europe from March 2008 to May 2009. The measurements were conducted in a wide variety of environments, including coastal and continental locations as well as sites at different altitudes (both in the boundary layer and the free troposphere). New particle formation events were detected at all of the 12 field sites during the year-long measurement period. From the data, nucleation and growth rates of newly formed particles were determined for each environment. In a case of parallel ion and neutral cluster measurements, we could also estimate the relative contribution of ion-induced and neutral nucleation to the total particle formation. The formation rates of charged particles at 2 nm accounted for 1–30% of the corresponding total particle formation rates. As a significant new result, we found out that the total particle formation rate varied much more between the different sites than the formation rate of charged particles. This work presents, so far, the most comprehensive effort to experimentally characterize nucleation and growth of atmospheric molecular clusters and nanoparticles at ground-based observation sites on a continental scale.

scholarly journals Aerosol dynamics simulations on the connection of sulphuric acid and new particle formation

2008 ◽  
Vol 8 (3) ◽  
pp. 11363-11394 ◽  
Author(s):  
S.-L. Sihto ◽  
H. Vuollekoski ◽  
J. Leppä ◽  
I. Riipinen ◽  
V.-M. Kerminen ◽  
...  
Keyword(s):  
Sulphuric Acid ◽  
Acid Concentration ◽  
Linear Dependence ◽  
Particle Number ◽  
Particle Formation ◽  
Number Concentration ◽  
Particle Number Concentration ◽  
Aerosol Dynamics ◽  
Sulphuric Acid Concentration ◽  
Acid Dependence

Abstract. We have performed a series of simulations with an aerosol dynamics box model to study the connection between new particle formation and sulphuric acid concentration. For nucleation either activation mechanism with a linear dependence on the sulphuric acid concentration or ternary H2O-H2SO4-NH3 nucleation was assumed. We investigated the factors that affect the sulphuric acid dependence during the early stages of particle growth, and tried to find conditions which would yield the linear dependence between the particle number concentration at 3–6 nm and sulphuric acid, as observed in field experiments. The simulations showed that the correlation with sulphuric acid may change during the growth from nucleation size to 3–6 nm size range, the main reason being the size dependent growth rate between 1 and 3 nm. In addition, the assumed size for the nucleated clusters had a crucial impact on the sulphuric acid dependence at 3 nm. The simulations yielded a linear dependence between the particle number concentration at 3 nm and sulphuric acid, when a low saturation vapour pressure for the condensable organic vapour was assumed, or when nucleation took place at ~2 nm instead of ~1 nm. Comparison of results with activation and ternary nucleation showed that ternary nucleation cannot explain the experimentally observed linear or square dependence on sulphuric acid.

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