Aerosol Dynamics Box Model Studies on the Connection of Sulphuric Acid and New Particle Formation

2007 ◽  
pp. 1013-1017
Author(s):  
Sanna-Liisa Sihto ◽  
Henri Vuollekoski ◽  
J. Leppä ◽  
Ilona Riipinen ◽  
Veli-Matti Kerminen ◽  
...  
Keyword(s):  
Sulphuric Acid ◽  
Particle Formation ◽  
Box Model ◽  
New Particle Formation ◽  
Aerosol Dynamics ◽  
Model Studies

scholarly journals New insights into nocturnal nucleation

2012 ◽  
Vol 12 (9) ◽  
pp. 4297-4312 ◽  
Author(s):  
I. K. Ortega ◽  
T. Suni ◽  
M. Boy ◽  
T. Grönholm ◽  
H. E. Manninen ◽  
...  
Keyword(s):  
Quantum Chemical ◽  
Aerosol Particles ◽  
Particle Formation ◽  
Nucleation And Growth ◽  
Oxidation Products ◽  
New Particle Formation ◽  
Aerosol Dynamics ◽  
Different Types ◽  
Consistent Manner ◽  
Dynamics Models

Abstract. Formation of new aerosol particles by nucleation and growth is a significant source of aerosols in the atmosphere. New particle formation events usually take place during daytime, but in some locations they have been observed also at night. In the present study we have combined chamber experiments, quantum chemical calculations and aerosol dynamics models to study nocturnal new particle formation. All our approaches demonstrate, in a consistent manner, that the oxidation products of monoterpenes play an important role in nocturnal nucleation events. By varying the conditions in our chamber experiments, we were able to reproduce the very different types of nocturnal events observed earlier in the atmosphere. The exact strength, duration and shape of the events appears to be sensitive to the type and concentration of reacting monoterpenes, as well as the extent to which the monoterpenes are exposed to ozone and potentially other atmospheric oxidants.

New Particle Formation and Sulphuric Acid Concentrations During 26 Months in Hyytiälä

2007 ◽  
pp. 226-229
Author(s):  
T. Nieminen ◽  
Markku Kulmala ◽  
Ilona Riipinen ◽  
Anne Hirsikko ◽  
Michael Boy ◽  
...  
Keyword(s):  
Sulphuric Acid ◽  
Particle Formation ◽  
New Particle Formation

Connections Between Ambient Sulphuric Acid and New Particle Formation in Hyytiälä and Heideleberg

2007 ◽  
pp. 1033-1037
Author(s):  
Ilona Riipinen ◽  
Sanna-Liisa Sihto ◽  
Markku Kulmala ◽  
Frank Arnold ◽  
Miikka Dal Maso ◽  
...  
Keyword(s):  
Sulphuric Acid ◽  
Particle Formation ◽  
New Particle Formation

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 Kinetic nucleation and ions in boreal particle formation events

2004 ◽  
Vol 4 (4) ◽  
pp. 3911-3945 ◽  
Author(s):  
L. Laakso ◽  
T. Anttila ◽  
K. E. J. Lehtinen ◽  
P. P. Aalto ◽  
M. Kulmala ◽  
...  
Keyword(s):  
Sulphuric Acid ◽  
Negative Ions ◽  
Particle Formation ◽  
Model Simulations ◽  
Aerosol Dynamics ◽  
Atmospheric Particle ◽  
Relative Contribution ◽  
Charged Aerosol ◽  
Charged Clusters ◽  
Basic Features

Abstract. In order to gain a more comprehensive picture on different mechanisms behind atmospheric particle formation, measurement results from QUEST 2-campaign are analyzed with an aid of an aerosol dynamic model. A special emphasis is laid on air ion and charged aerosol dynamics. Conducted model simulations indicate that kinetic nucleation of ammonia and sulphuric acid together with condensation of sulphuric acid and low-volatile organic vapours onto clusters and particles explain basic features of particle formation events as well as ion characteristics. However, observed excess of negative ions in the diameter range 1.5–3 nm and overcharge of 3–5 nm particles demonstrate that ions are also involved in particle formation. These observations can be explained by preferential condensation of sulphuric acid onto negatively charged clusters and particles. According to model simulations, the relative contribution of ion-based particle formation seem to be smaller than kinetic nucleation of neutral clusters. Conducted model simulations also corroborate the recently-presented hypothesis according to which a large number of so-called thermodynamically stable clusters (TSCs) having a diameter between 1–3 nm exist in the atmosphere. TSCs were found to grow to the observable sizes only under favorable conditions, e.g. when the pre-existing particle concentration was low.

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 SO<sub>2</sub> oxidation products other than H<sub>2</sub>SO<sub>4</sub> as a trigger of new particle formation – Part 2: Comparison of ambient and laboratory measurements, and atmospheric implications

2008 ◽  
Vol 8 (3) ◽  
pp. 9673-9695 ◽  
Author(s):  
A. Laaksonen ◽  
M. Kulmala ◽  
T. Berndt ◽  
F. Stratmann ◽  
S. Mikkonen ◽  
...  
Keyword(s):  
Sulphuric Acid ◽  
Laboratory Data ◽  
Particle Formation ◽  
Oxidation Products ◽  
New Particle Formation ◽  
Laboratory Measurements ◽  
So2 Oxidation ◽  
Atmospheric Nucleation ◽  
Trace Species ◽  
Relative Acidity

Abstract. Atmospheric new particle formation is generally thought to occur due to homogeneous or ion-induced nucleation of sulphuric acid. We compare ambient nucleation rates with laboratory data from nucleation experiments involving either sulphuric acid or oxidized SO2. Atmospheric nucleation occurs at H2SO4 concentrations 2–4 orders of magnitude lower than binary or ternary H2SO4 nucleation. In contrast, the atmospheric nucleation rates and H2SO4 concentrations are very well replicated in the SO2 oxidation experiments. We explain these features by the formation of free HSO5 radicals in pace with H2SO4 during the SO2 oxidation. We suggest that at temperatures above ~250 K these radicals produce nuclei of new aerosols much more efficiently than H2SO4. These nuclei are activated to further growth by H2SO4 and possibly other trace species. However, at lower temperatures the atmospheric relative acidity is high enough for the H2SO4–H2O nucleation to dominate.

scholarly journals New particle formation in air mass transported between two measurement sites in Northern Finland

2005 ◽  
Vol 5 (6) ◽  
pp. 11929-11963 ◽  
Author(s):  
M. Komppula ◽  
S.-L. Sihto ◽  
H. Korhonen ◽  
H. Lihavainen ◽  
V.-M. Kerminen ◽  
...  
Keyword(s):  
Growth Rates ◽  
Particle Growth ◽  
Particle Formation ◽  
Distribution Data ◽  
New Particle Formation ◽  
Air Mass ◽  
Air Masses ◽  
Aerosol Dynamics ◽  
Almost All ◽  
Distinct Features

Abstract. This study covers four years of aerosol number size distribution data from Pallas and Värriö sites 250 km apart from each other in Northern Finland and compares new particle formation events between these sites. In eastern air masses almost all events were observed to start earlier at the eastern station Värriö, whereas in western air masses most of the events were observed to start earlier at the western station Pallas. This demonstrates that particle formation in a certain air mass type depends not only on the diurnal variation of the parameters causing the phenomenon (such as photochemistry) but also on some properties carried by the air mass itself. The correlation in growth rates between the two sites was relatively good, which suggests that the amount of condensable vapour causing the growth must have been at about the same level in both sites. The value of condensation sink was frequently much higher at the downwind station. It seems that secondary particle formation related to biogenic sources dominate in many cases over the particle sinks during the air mass transport between the sites. Two cases of transport from Pallas to Värriö were further analysed with an aerosol dynamics model. The model was able to reproduce the observed nucleation events 250 km down-wind at Värriö but revealed some differences between the two cases. The simulated nucleation rates were in both cases similar but the organic concentration profiles that best reproduced the observations were different in the two cases indicating that divergent formation reactions may dominate under different conditions. The simulations also suggested that organic compounds were the main contributor to new particle growth, which offers a tentative hypothesis to the distinct features of new particles at the two sites: Air masses arriving from Atlantic Ocean typically spent approximately only ten hours over land before arriving at Pallas, and thus the time for the organic vapours to accumulate in the air and to interact with the particles is relatively short. This can lead to low nucleation mode growth rates and even to suppression of detectable particle formation event due to efficient scavenging of newly formed clusters, as was observed in the case studies.

scholarly journals Connections between atmospheric sulphuric acid and new particle formation during QUEST III–IV campaigns in Heidelberg and Hyytiälä

2006 ◽  
Vol 6 (5) ◽  
pp. 10837-10882 ◽  
Author(s):  
I. Riipinen ◽  
S.-L. Sihto ◽  
M. Kulmala ◽  
F. Arnold ◽  
M. Dal Maso ◽  
...  
Keyword(s):  
Sulphuric Acid ◽  
Power Law ◽  
Growth Rates ◽  
Particle Production ◽  
Particle Formation ◽  
Rural Site ◽  
Main Process ◽  
Time Lags ◽  
New Particle Formation ◽  
Particle Formation And Growth

Abstract. This study investigates the connections between atmospheric sulphuric acid and new particle formation during QUEST III and BACCI/QUEST IV campaigns. The campaigns have been conducted in Heidelberg (2004) and Hyytiälä (2005), the first representing a polluted site surrounded by deciduous forest, and the second a rural site in a boreal forest environment. We have studied the role of sulphuric acid in particle formation and growth by determining 1) the power-law dependencies between sulphuric acid ([H2SO4]), and particle concentrations (N3–6) or formation rates at 1 nm and 3 nm (J1 and J3; 2) the time delays between [H2SO4] and N3–6 or J3, and the growth rates for 1–3 nm particles; 3) the empirical nucleation coefficients A and K in relations J1=A[H2SO4] and J1=K[H2SO4]2, respectively; 4) theoretical predictions for J1 and J3 for the days when no significant particle formation is observed, based on the observed sulphuric acid concentrations and condensation sinks. In both environments, N3–6 or J3 and [H2SO4] were linked via a power-law relation with exponents typically ranging from 1 to 2. The result suggests that the cluster activation theory and kinetic nucleation have the potential to explain the observed particle formation. However, some differences between the sites existed: The 1–3 nm growth rates were slightly higher and the nucleation coefficients about an order of magnitude greater in Heidelberg than in Hyytiälä conditions. The time lags between J3 and [H2SO4] were consistently lower than the corresponding delays between N3–6 and [H2SO4]. The exponents in the J3∝[H2SO4]nJ3-connection were consistently higher than or equal to the exponents in the relation N3–6∝[H2SO4]nN36. In the J1 values, no significant differences were found between the observed rates on particle formation event days and the predictions on non-event days. The J3 values predicted by the cluster activation or kinetic nucleation hypotheses, on the other hand, were considerably lower on non-event days than the rates observed on particle formation event days. This study provides clear evidence implying that the main process limiting the observable particle formation is the competition between the growth of the freshly formed particles and their loss by scavenging, rather than the initial particle production by nucleation of sulphuric acid. In general, it can be concluded that the simple models based on sulphuric acid concentrations and particle formation by cluster activation or kinetic nucleation can predict the occurence of atmospheric particle formation and growth well, if the particle scavenging is accurately accounted for.

scholarly journals Coupling an aerosol box model with one-dimensional flow: a tool for understanding observations of new particle formation events

Tellus B ◽  
2016 ◽  
Vol 68 (1) ◽  
pp. 29706 ◽  
Author(s):  
Niku Kivekäs ◽  
Jimmie Carpman ◽  
Pontus Roldin ◽  
Johannes Leppä ◽  
Ewan O'Connor ◽  
...  
Keyword(s):  
Particle Formation ◽  
Box Model ◽  
New Particle Formation ◽  
One Dimensional ◽  
Dimensional Flow
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