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

2007 ◽  
Vol 7 (8) ◽  
pp. 1899-1914 ◽  
Author(s):  
I. Riipinen ◽  
S.-L. Sihto ◽  
M. Kulmala ◽  
F. Arnold ◽  
M. Dal Maso ◽  
...  

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 nucleation coefficients were 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.

2006 ◽  
Vol 6 (5) ◽  
pp. 10837-10882 ◽  
Author(s):  
I. Riipinen ◽  
S.-L. Sihto ◽  
M. Kulmala ◽  
F. Arnold ◽  
M. Dal Maso ◽  
...  

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.


2011 ◽  
Vol 11 (7) ◽  
pp. 3333-3346 ◽  
Author(s):  
V. Vakkari ◽  
H. Laakso ◽  
M. Kulmala ◽  
A. Laaksonen ◽  
D. Mabaso ◽  
...  

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.


2010 ◽  
Vol 2010 ◽  
pp. 1-9 ◽  
Author(s):  
Ciaran Monahan ◽  
Henri Vuollekoski ◽  
Markku Kulmala ◽  
Colin O'Dowd

A modal atmospheric aerosol model (M7) is evaluated in terms of predicting marine new particle formation and growth. Simulations were carried out for three different nucleation schemes involving (1) kinetic self-nucleation of OIO (2) nucleationviaOIO activation by H2SO4and (3) nucleationviaOIO activation by H2SO4plus condensation of a low-volatility organic vapour. Peak OIO and H2SO4vapour concentrations were both limited to6×106molecules cm-3at noontime while the peak organic vapour concentration was limited to12×106molecules cm-3. All simulations produced significant concentrations of new particles in the Aitken mode. From a base case particle concentration of 222 cm-3at radii >15 nm, increases in concentrations to 366 cm-3were predicted from the OIO-OIO case, 722 cm-3for the OIO-H2SO4case, and 1584 cm-3for the OIO-H2SO4case with additional condensing organic vapours. The results indicate that open ocean new particle production is feasible for clean conditions; however, new particle production becomes most significant when an additional condensable organic vapour is available to grow the newly formed particles to larger sizes. Comparison to sectional model for a typical case study demonstrated good agreement and the validity of using the modal model.


2010 ◽  
Vol 10 (12) ◽  
pp. 30777-30821 ◽  
Author(s):  
V. Vakkari ◽  
H. Laakso ◽  
M. Kulmala ◽  
A. Laaksonen ◽  
D. Mabaso ◽  
...  

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.


2015 ◽  
Vol 103 ◽  
pp. 7-17 ◽  
Author(s):  
Z.B. Wang ◽  
M. Hu ◽  
X.Y. Pei ◽  
R.Y. Zhang ◽  
P. Paasonen ◽  
...  

2019 ◽  
Vol 19 (16) ◽  
pp. 10537-10555 ◽  
Author(s):  
Simo Hakala ◽  
Mansour A. Alghamdi ◽  
Pauli Paasonen ◽  
Ville Vakkari ◽  
Mamdouh I. Khoder ◽  
...  

Abstract. Atmospheric aerosols have significant effects on human health and the climate. A large fraction of these aerosols originates from secondary new particle formation (NPF), where atmospheric vapors form small particles that subsequently grow into larger sizes. In this study, we characterize NPF events observed at a rural background site of Hada Al Sham (21.802∘ N, 39.729∘ E), located in western Saudi Arabia, during the years 2013–2015. Our analysis shows that NPF events occur very frequently at the site, as 73 % of all the 454 classified days were NPF days. The high NPF frequency is likely explained by the typically prevailing conditions of clear skies and high solar radiation, in combination with sufficient amounts of precursor vapors for particle formation and growth. Several factors suggest that in Hada Al Sham these precursor vapors are related to the transport of anthropogenic emissions from the coastal urban and industrial areas. The median particle formation and growth rates for the NPF days were 8.7 cm−3 s−1 (J7 nm) and 7.4 nm h−1 (GR7−12 nm), respectively, both showing highest values during late summer. Interestingly, the formation and growth rates increase as a function of the condensation sink, likely reflecting the common anthropogenic sources of NPF precursor vapors and primary particles affecting the condensation sink. A total of 76 % of the NPF days showed an unusual progression, where the observed diameter of the newly formed particle mode started to decrease after the growth phase. In comparison to most long-term measurements, the NPF events in Hada Al Sham are exceptionally frequent and strong both in terms of formation and growth rates. In addition, the frequency of the decreasing mode diameter events is higher than anywhere else in the world.


Author(s):  
T. Nieminen ◽  
Markku Kulmala ◽  
Ilona Riipinen ◽  
Anne Hirsikko ◽  
Michael Boy ◽  
...  

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

2007 ◽  
pp. 1013-1017
Author(s):  
Sanna-Liisa Sihto ◽  
Henri Vuollekoski ◽  
J. Leppä ◽  
Ilona Riipinen ◽  
Veli-Matti Kerminen ◽  
...  

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