Effect of Molecular Structure and Hydration on the Uptake of Gas-Phase Sulfuric Acid by Charged Clusters/Ultrafine Particles

Nadykto, Alexey B.; Natsheh, Anas Al; Yu, Fangqun; Mikkelsen, Kurt V.; Ruuskanen, Juhani

doi:10.1080/02786820490426084

Cited by 20 publications

(13 citation statements)

References 23 publications

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“…On the other hand, this is not the most stable structure and its dipole moment is almost double that of the NAT-2 dipole moment value. Recently Nadykto et al [27,28] reported that the increment of the dipole moment of the molecular conformation will increase the value of the uptake coefficient of the cluster. This highlights the high reactivity of this molecular complex.…”

Section: Vibrational Frequencies and Ir Spectrum Analysismentioning

confidence: 98%

Theoretical investigation of the coexistence of α and β-nitric acid trihydrates (NAT) molecular conformations

2006

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Section: Vibrational Frequencies and Ir Spectrum Analysismentioning

confidence: 98%

Theoretical investigation of the coexistence of α and β-nitric acid trihydrates (NAT) molecular conformations

2006

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“…Theoretical calculations predict that condensation of vapor molecules, especially of sulfuric acid and its hydrates, is faster for charged particles compared with neutral particles [ Yu and Turco , 2000; Laakso et al , 2003; Nadykto and Yu , 2003; Nadykto et al , 2004]. This means that charged nuclei are expected to grow faster in size than what neutral nuclei do.…”

Section: Applicability Of the Analytical Expressionsmentioning

confidence: 99%

“…Despite these uncertainties, the value of EF is expected to be close to unity for nuclei larger than about 3–5 nm in diameter, which means that the charging state is not significantly affected by this phenomenon in the size range that can be measured using current instrumentation. Below 3 nm, the value of EF increases rapidly with decreasing particle size and may reach values larger than 2 when the nuclei diameter approaches 1 nm [ Laakso et al , 2003; Nadykto and Yu , 2003; Nadykto et al , 2004].…”

Section: Applicability Of the Analytical Expressionsmentioning

confidence: 99%

Charging state of the atmospheric nucleation mode: Implications for separating neutral and ion‐induced nucleation

et al. 2007

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[1] One way of getting information about the relative roles of neutral and ion-induced nucleation in the atmosphere is to measure the charging state of aerosol particles, i.e., the extent by which the charged fraction of aerosol particles differs from the corresponding equilibrium charged fraction. By using a theoretical approach, we investigated how the charging state of a growing nucleation mode behaves under different atmospheric conditions. We found that the time evolution of the nuclei charging state is governed by two parameters: the initial nuclei charging state determined by the nucleation mechanism and the parameter K that is directly proportional to the cluster ion concentration and inversely proportional to the nuclei growth rate. We demonstrated that if the value K is larger than a certain threshold value (2-4 nm À1 ), any information about the initial charging state of the nuclei, and thereby about the nucleation mechanism, will be lost by the time the nuclei grow into the measurement size range (>3 nm). By making a few simplifying assumptions, we derived an analytical expression for the functional dependence of the nuclei charging state as a function of the nuclei size. We demonstrated that the derived expression can usually be fitted into experimental data on nuclei charging states. When the value of K is small enough, the obtained fitting can be extrapolated successfully down to sizes where the nucleation has taken place to obtain information about the relative importance of neutral and ion-induced nucleation.Citation: Kerminen, V.-M., T. Anttila, T. Petäjä, L. Laakso, S. Gagné, K. E. J. Lehtinen, and M. , Charging state of the atmospheric nucleation mode: Implications for separating neutral and ion-induced nucleation,

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“…Any plausible theory, however, must predict sufficiently high growth rates since freshly-nucleated clusters are scavenged away very rapidly by pre-existing particles (Kerminen et al, 2001). In particular, it has been suggested that the presence of electric charges in freshly-formed clusters enhance the uptake of polar molecules such as sulfuric acid, thereby giving a growth advantage to charged clusters over neutral ones (Yu and Turco, 2001;Nadykto and Yu, 2003;Nadykto et al, 2004). Atmospheric ions are thus expected to be involved in both nucleation and growth, but their overall importance to particle formation is an open question at present.…”

Section: Introductionmentioning

confidence: 99%

Kinetic nucleation and ions in boreal forest particle formation events

et al. 2004

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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. 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, an 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 and/or contribution of ion-induced nucleation on particle formation. According to model simulations, which assume that the nucleation rate is equal to the sulfuric acid collision rate, the relative contribution of ion-based particle formation seems 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 observable sizes only under favorable conditions, e.g. when the pre-existing particle concentration was low.

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Effect of Molecular Structure and Hydration on the Uptake of Gas-Phase Sulfuric Acid by Charged Clusters/Ultrafine Particles

Cited by 20 publications

References 23 publications

Theoretical investigation of the coexistence of α and β-nitric acid trihydrates (NAT) molecular conformations

Theoretical investigation of the coexistence of α and β-nitric acid trihydrates (NAT) molecular conformations

Charging state of the atmospheric nucleation mode: Implications for separating neutral and ion‐induced nucleation

Kinetic nucleation and ions in boreal forest particle formation events

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