Computational Study of the Clustering of a Cyclohexene Autoxidation Product C6H8O7 with Itself and Sulfuric Acid

2015 ◽  
Vol 119 (30) ◽  
pp. 8414-8421 ◽  
Author(s):  
Jonas Elm ◽  
Nanna Myllys ◽  
Noora Hyttinen ◽  
Theo Kurtén
Keyword(s):  
Sulfuric Acid ◽  
Computational Study ◽  
Autoxidation Product

scholarly journals Enhancing effect of dimethylamine in sulfuric acid nucleation in the presence of water – a computational study

2010 ◽  
Vol 10 (10) ◽  
pp. 4961-4974 ◽  
Author(s):  
V. Loukonen ◽  
T. Kurtén ◽  
I. K. Ortega ◽  
H. Vehkamäki ◽  
A. A. H. Pádua ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Quantum Chemistry ◽  
Computational Study ◽  
Water Molecules ◽  
Enhancing Effect ◽  
Formation Energies

Abstract. We have studied the hydration of sulfuric acid – ammonia and sulfuric acid – dimethylamine clusters using quantum chemistry. We calculated the formation energies and thermodynamics for clusters of one ammonia or one dimethylamine molecule together with 1–2 sulfuric acid and 0–5 water molecules. The results indicate that dimethylamine enhances the addition of sulfuric acid to the clusters much more efficiently than ammonia when the number of water molecules in the cluster is either zero, or greater than two. Further hydrate distribution calculations reveal that practically all dimethylamine-containing two-acid clusters will remain unhydrated in tropospherically relevant circumstances, thus strongly suggesting that dimethylamine assists atmospheric sulfuric acid nucleation much more effectively than ammonia.

New Particle Formation Involving Charged Sulfuric Acid – Ammonia Clusters

2020 ◽  
Author(s):  
Vitus Besel ◽  
Jakub Kubečka ◽  
Theo Kurtén ◽  
Hanna Vehkamäki
Keyword(s):  
Sulfuric Acid ◽  
Computational Study ◽  
Cluster Formation ◽  
Chem Phys ◽  
Particle Formation ◽  
Empirical Method ◽  
Particle Nucleation ◽  
New Particle Formation ◽  
Charged Clusters ◽  
Ammonia Clusters

<div> <p>The bulk of aerosol particles in the atmosphere are formed by gas-to-particle nucleation (Merikanto et al., 2009). However, the exact process of single molecules forming cluster, which subsequently can grow into particles, remains largely unknown. Recently, sulfuric acid has been identified to play a key role in this new particle formation enhanced by other compounds such as organic acids (Zhang, 2010) or ammonia (Anttila et al., 2005). To identify the characteristics of cluster formation and nucleation involving sulfuric acid and ammonia in neutral, positive and negative modes, we conducted a computational study. We used a layered approach for configurational sampling of the molecular clusters starting from utilizing a genetic algorithm in order to explore the whole potential energy surface (PES) with all plausible geometrical minima, however, with very unreliable energies. The structures were further optimized with a semi-empirical method and, then, at the ωB97X-D DFT level of theory. After each step, the optimized geometries were filtered to obtain the global minimum configuration. Further, a high level of theory (DLPNO-CCSD(T)) was used for obtaining the electronic energies, in addition to performing DFT frequency analysis, to calculate the Gibbs free energies of formation. These were passed to the Atmospheric Cluster Dynamics Code (ACDC) (McGrath et al., 2012) for studying the evolution of cluster populations. We determined the global minima for the following sulfuric acid - ammonia clusters: (H<sub>2</sub>SO<sub>4</sub>)<sub>m</sub>(NH<sub>3</sub>)<sub>n</sub> with m=n, m=n+1 and n=m+1 for neutral clusters, (H<sub>2</sub>SO<sub>4</sub>)<sub>m</sub>(HSO<sub>4</sub>)<sup>−</sup>(NH<sub>3</sub>)<sub>n</sub> with m=n and n=m+1 for positively charged clusters, and (H<sub>2</sub>SO<sub>4</sub>)<sub>m</sub>(NH<sub>4</sub>)<sup>+</sup>(NH<sub>3</sub>)<sub>n</sub> with m=n and m=n+1 for negatively charged clusters. Further, we present the formation rates, steady state concentrations and fluxes of these clusters calculated using ACDC and discuss how a new configurational sampling procedure, more precise quantum chemistry methods and parameters, such as symmetry and a quasiharmonic approach, impact these ACDC results in comparison to previous studies.</p> </div><div> <p><em>References:<br></em><em>J. Merikanto, D. V. Spracklen, G. W. Mann, S. J. Pickering, and K. S. Carslaw (2009). Atmos. Chem.  Phys., 9, 8601-8616. <br>R. Zhang (2010). Science, 328, 1366-1367. <br>T. Anttila, H. Vehkamäki, I. Napari, M. Kulmala (2005). Boreal Env. Res., 10, 523. <br>M.J. McGrath, T. Olenius, I.K. Ortega, V. Loukonen, P.  Paasonen, T. Kurten, M. Kulmala (2012). Atmos. Chem. Phys., 12, 2355. <br></em></p> </div>

CIMS Sulfuric Acid Detection Efficiency Enhanced by Amines Due to Higher Dipole Moments: A Computational Study

2013 ◽  
Vol 117 (51) ◽  
pp. 14109-14119 ◽  
Author(s):  
Oona Kupiainen-Määttä ◽  
Tinja Olenius ◽  
Theo Kurtén ◽  
Hanna Vehkamäki
Keyword(s):  
Sulfuric Acid ◽  
Detection Efficiency ◽  
Computational Study ◽  
Dipole Moments

Computational Study of the Reaction between Biogenic Stabilized Criegee Intermediates and Sulfuric Acid

2007 ◽  
Vol 111 (17) ◽  
pp. 3394-3401 ◽  
Author(s):  
Theo Kurtén ◽  
Boris Bonn ◽  
Hanna Vehkamäki ◽  
Markku Kulmala
Keyword(s):  
Sulfuric Acid ◽  
Computational Study ◽  
Criegee Intermediates ◽  
Stabilized Criegee Intermediates

Hydrogen Bonding in the Sulfuric Acid–Methanol–Water System: A Matrix Isolation and Computational Study

2014 ◽  
Vol 119 (11) ◽  
pp. 2271-2280 ◽  
Author(s):  
Mark Rozenberg ◽  
Aharon Loewenschuss ◽  
Claus J. Nielsen
Keyword(s):  
Hydrogen Bonding ◽  
Sulfuric Acid ◽  
Computational Study ◽  
Matrix Isolation ◽  
Water System ◽  
System A

scholarly journals Effect of Hydration and Base Contaminants on Sulfuric Acid Diffusion Measurement: A Computational Study

2014 ◽  
Vol 48 (6) ◽  
pp. 593-603 ◽  
Author(s):  
Tinja Olenius ◽  
Theo Kurtén ◽  
Oona Kupiainen-Määttä ◽  
Henning Henschel ◽  
Ismael K. Ortega ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Computational Study ◽  
Diffusion Measurement ◽  
Acid Diffusion

Vibrational analysis of aqueous sulfuric acid: A computational study

2009 ◽  
Vol 109 (9) ◽  
pp. 1984-1990 ◽  
Author(s):  
Yoong-Kee Choe ◽  
Eiji Tsuchida ◽  
Tamio Ikeshoji
Keyword(s):  
Sulfuric Acid ◽  
Computational Study ◽  
Vibrational Analysis ◽  
Aqueous Sulfuric Acid

H-Bonding of Sulfuric Acid with Its Decomposition Products: An Infrared Matrix Isolation and Computational Study of the H2SO4·H2O·SO3 Complex

2016 ◽  
Vol 120 (20) ◽  
pp. 3450-3455 ◽  
Author(s):  
Mark Rozenberg ◽  
Aharon Loewenschuss ◽  
Claus J. Nielsen
Keyword(s):  
Sulfuric Acid ◽  
Computational Study ◽  
Matrix Isolation ◽  
Decomposition Products

scholarly journals Computational Study of the Hydration of Sulfuric Acid Dimers: Implications for Acid Dissociation and Aerosol Formation

2012 ◽  
Vol 116 (39) ◽  
pp. 9745-9758 ◽  
Author(s):  
Berhane Temelso ◽  
Thuong Ngoc Phan ◽  
George C. Shields
Keyword(s):  
Sulfuric Acid ◽  
Computational Study ◽  
Acid Dissociation ◽  
Aerosol Formation
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