On the formation of sulphuric acid – Amine clusters in varying atmospheric conditions and its influence on atmospheric new particle formation. Paasonen, P., Olenius, T., Kupiainen, O., KurtÃn, T., Petäjä, T., Birmili, W., Hamed, A., Hu, M., Huey, L., G., Plass-Duelmer, C., Smith, J., N., Wiedensohler, A., Loukonen, V., McGrath, M., J., Ortega, I., K., Laaksonen, A., Vehkamäki, H., & Kulmala, M. Atmospheric Chemistry and Physics, 12(19):9113-9133, 2012.
On the formation of sulphuric acid – Amine clusters in varying atmospheric conditions and its influence on atmospheric new particle formation [link]Website  doi  abstract   bibtex   
Sulphuric acid is a key component in atmo-spheric new particle formation. However, sulphuric acid alone does not form stable enough clusters to initiate par-ticle 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 (J A2B2) at varying atmo-spherically relevant conditions with respect to concentrations of sulphuric acid ([H 2 SO 4 ]), 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 nucle-ation of organic vapours (other than amines) with higher at-mospheric concentrations than sulphuric acid. The modelled formation rates J A2B2 were functions of sulphuric acid con-centration with close to quadratic dependence, which is in good agreement with atmospheric observations of the con-nection between the particle formation rate and sulphuric acid concentration. The coefficients K A2B2 connecting the cluster formation rate and sulphuric acid concentrations as J A2B2 = K A2B2 [H 2 SO 4 ] 2 turned out to depend also on amine concentrations, temperature and relative humidity. We com-pared the modelled coefficients K A2B2 with the correspond-ing coefficients calculated from the atmospheric observa-tions (K obs) from environments with varying temperatures and levels of anthropogenic influence. By taking into account the modelled behaviour of J A2B2 as a function of [H 2 SO 4 ], 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 composi-tions (DMA or TMA or one of both) had different responses to varying meteorological conditions and concentrations of Published by Copernicus Publications on behalf of the European Geosciences Union. 9114 P. Paasonen et al.: Sulphuric acid-amine clusters in varying atmospheric conditions vapours participating in particle formation. The observed in-verse proportionality of the coefficient K obs with RH and temperature agreed best with the modelled coefficient K A2B2 related to formation of a cluster with two H 2 SO 4 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 forma-tion rate of clusters with at least two of both sulphuric acid and amine molecules might be the rate-limiting step for at-mospheric particle formation. More generally, our analysis elucidates the sensitivity of the atmospheric particle forma-tion rate to meteorological variables and concentrations of vapours participating in particle formation (also other than H 2 SO 4).
@article{
 title = {On the formation of sulphuric acid – Amine clusters in varying atmospheric conditions and its influence on atmospheric new particle formation},
 type = {article},
 year = {2012},
 pages = {9113-9133},
 volume = {12},
 websites = {http://www.atmos-chem-phys.net/12/9113/2012/},
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 last_modified = {2023-01-31T22:46:05.400Z},
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 citation_key = {Paasonen2012},
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 abstract = {Sulphuric acid is a key component in atmo-spheric new particle formation. However, sulphuric acid alone does not form stable enough clusters to initiate par-ticle 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 (J A2B2) at varying atmo-spherically relevant conditions with respect to concentrations of sulphuric acid ([H 2 SO 4 ]), 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 nucle-ation of organic vapours (other than amines) with higher at-mospheric concentrations than sulphuric acid. The modelled formation rates J A2B2 were functions of sulphuric acid con-centration with close to quadratic dependence, which is in good agreement with atmospheric observations of the con-nection between the particle formation rate and sulphuric acid concentration. The coefficients K A2B2 connecting the cluster formation rate and sulphuric acid concentrations as J A2B2 = K A2B2 [H 2 SO 4 ] 2 turned out to depend also on amine concentrations, temperature and relative humidity. We com-pared the modelled coefficients K A2B2 with the correspond-ing coefficients calculated from the atmospheric observa-tions (K obs) from environments with varying temperatures and levels of anthropogenic influence. By taking into account the modelled behaviour of J A2B2 as a function of [H 2 SO 4 ], 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 composi-tions (DMA or TMA or one of both) had different responses to varying meteorological conditions and concentrations of Published by Copernicus Publications on behalf of the European Geosciences Union. 9114 P. Paasonen et al.: Sulphuric acid-amine clusters in varying atmospheric conditions vapours participating in particle formation. The observed in-verse proportionality of the coefficient K obs with RH and temperature agreed best with the modelled coefficient K A2B2 related to formation of a cluster with two H 2 SO 4 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 forma-tion rate of clusters with at least two of both sulphuric acid and amine molecules might be the rate-limiting step for at-mospheric particle formation. More generally, our analysis elucidates the sensitivity of the atmospheric particle forma-tion rate to meteorological variables and concentrations of vapours participating in particle formation (also other than H 2 SO 4).},
 bibtype = {article},
 author = {Paasonen, P. and Olenius, T. and Kupiainen, O. and KurtÃn, T. and Petäjä, T. and Birmili, W. and Hamed, A. and Hu, M. and Huey, L. G. and Plass-Duelmer, C. and Smith, J. N. and Wiedensohler, A. and Loukonen, V. and McGrath, M. J. and Ortega, I. K. and Laaksonen, A. and Vehkamäki, H. and Kulmala, M.},
 doi = {10.5194/acp-12-9113-2012},
 journal = {Atmospheric Chemistry and Physics},
 number = {19}
}
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