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

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 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 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 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).

The influence of volcano activity on aerosol formation over the Andes

2020 ◽  
Author(s):  
Federico Bianchi ◽  
Diego Aliaga ◽  
Qiaozhi Zha ◽  
Liine Heikkinen ◽  
Marcos Andrade ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Sulphuric Acid ◽  
Negative Ions ◽  
Particle Formation ◽  
Amazon Forest ◽  
Particle Nucleation ◽  
New Particle Formation ◽  
Aerosol Formation ◽  
Air Masses ◽  
Particle Sizer

&lt;p&gt;A significant fraction (&gt;50%) of cloud condensation nuclei (CCN) in the atmosphere arises from new particle formation (Dunne et al., 2016). While particle nucleation has been observed almost everywhere in the atmosphere, the mechanisms governing this process are still poorly understood and subject of on-going research. For example, it is still largely unknown which components participate in new-particle formation. Laboratory experiments and quantum chemical calculations have identified potential candidates that may play a role, including sulphuric acid, ions, ammonia, amines and highly oxygenated organic molecules (Kirkby et al., 2011; Almeida et al., 2013; Bianchi et al., 2016; Bianchi et al., 2019).&lt;/p&gt;&lt;p&gt;Here we present observations of the formation and growth of newly formed particles measured during intense volcano activities.&lt;/p&gt;&lt;p&gt;The measurements were conducted at Chacaltaya mountain station (5240 m a.s.l.) in Bolivia. The station is located on top of the Cordillera Real. It has air masses coming from the Amazon forest, La Paz and the Bolivian altiplano.&lt;/p&gt;&lt;p&gt;With the Chemical Ionization Atmospheric Pressure interface Time-Of-Light mass spectrometers (CI-APi-TOF) we measured H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt;, the APi-TOF retrieved the chemical composition of positive and negative ions. Ion and particle size distributions were measured with the NAIS (Neutral cluster and Air Ion Spectrometer) and the SMPS (Scanning Mobility Particle Sizer), respectively. The PSM (Particle Sizer Magnifier) measured particles with a cut off that varied from 1-4 nm. Finally, with the ACSM (Aerosol Chemical Speciation Monitor) and the FIGAERO (Filter Inlet for Gases and AEROsols) we retrieved the aerosol chemical composition. Besides this set of instruments, other parameters were measured at the Chacaltaya GAW station.&lt;/p&gt;&lt;p&gt;During the intensive measurement campaign, air masses coming directly from volcano eruptions were detected by all our instruments. We were therefore able to determine the gas and particle chemical composition of the air mass. In addition to that, we observed several NPF events triggered by air masses coming from volcanic emissions. With this set of instruments, we were able to retrieve the chemical composition of the vapours leading to the formation of new particles. It was found that all the nucleation event observed during the volcano activity were triggered by sulphuric acid and ammonia. In the presentation we will show more details on the chemical and physical mechanism behind this process.&lt;/p&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;&lt;p&gt;Almeida, J., et al., (2013) Nature 502, 359-363.&lt;/p&gt;&lt;p&gt;Bianchi, F., et al., (2016) Science 6289, 1109-1112.&lt;/p&gt;&lt;p&gt;Bianchi, F., et al., (2019) Chemical Review 119, 3472&amp;#8722;3509&lt;/p&gt;&lt;p&gt;Dunne et al., (2016) Science 354, 1119-1124.&lt;/p&gt;&lt;p&gt;Kirkby, J., et al., (2011) Nature 476, (7361), 429-433.&lt;/p&gt;

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 (23) ◽  
pp. 7255-7264 ◽  
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 nucleation rates of H2SO4 produced from a liquid reservoir, and atmospheric H2SO4 concentrations are very well replicated in the SO2 oxidation experiments. We hypothesize these features to be due to 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 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 ◽  
...  
Keyword(s):  
Sulphuric Acid ◽  
Power Law ◽  
Particle Production ◽  
Deciduous Forest ◽  
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 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.

scholarly journals A new parametrization for ambient particle formation over coniferous forests and its potential implications for the future

2009 ◽  
Vol 9 (20) ◽  
pp. 8079-8090 ◽  
Author(s):  
B. Bonn ◽  
M. Boy ◽  
M. Kulmala ◽  
A. Groth ◽  
K. Trawny ◽  
...  
Keyword(s):  
Water Vapour ◽  
Sulphuric Acid ◽  
Field Studies ◽  
Particle Formation ◽  
Oxidation Products ◽  
Coniferous Forests ◽  
New Particle Formation ◽  
General Behaviour ◽  
Nucleation Parameters ◽  
Water Vapour Concentration

Abstract. Atmospheric new particle formation is a general phenomenon observed over coniferous forests. So far nucleation is either parameterised as a function of gaseous sulphuric acid concentration only, which is unable to explain the observed seasonality of nucleation events at different measurement sites, or as a function of sulphuric acid and organic molecules. Here we introduce different nucleation parameters based on the interaction of sulphuric acid and terpene oxidation products and elucidate the individual importance. They include basic trace gas and meteorological measurements such as ozone and water vapour concentrations, temperature (for terpene emission) and UV B radiation as a proxy for OH radical formation. We apply these new parameters to field studies conducted at conducted at Finnish and German measurement sites and compare these to nucleation observations on a daily and annual scale. General agreement was found, although the specific compounds responsible for the nucleation process remain speculative. This can be interpreted as follows: During cooler seasons the emission of biogenic terpenes and the OH availability limits the new particle formation while towards warmer seasons the ratio of ozone and water vapour concentration seems to dominate the general behaviour. Therefore, organics seem to support ambient nucleation besides sulphuric acid or an OH-related compound. Using these nucleation parameters to extrapolate the current conditions to prognosed future concentrations of ozone, water vapour and organic concentrations leads to a significant potential increase in the nucleation event number.

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