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

The Role of Binary and Ion Nucleation of Sulfuric Acid and Water Vapor in the Dynamics of Sulfate Aerosol Formation in the Atmosphere

2021 ◽  
pp. 53-60
Author(s):  
A. E. Aloyan ◽  
◽  
A. N. Yermakov ◽  
V. O. Arutyunyan ◽  
◽  
...  
Keyword(s):  
Water Vapor ◽  
Sulfuric Acid ◽  
Three Dimensional ◽  
Ionization Rate ◽  
Sulfate Aerosol ◽  
Aerosol Formation ◽  
Three Dimensional Model ◽  
Aerosol Composition ◽  
Transport And Transformation

The results of one-dimensional calculations of the height profiles of nucleated sulfate aerosol particles for the northern mid-latitudes and tropics in winter are presented. Numerical calculations were performed using a three-dimensional model of the transport and transformation of multicompo- nent gas and aerosol substances in the atmosphere, incorporating photochemistry, nucleation involving neutral molecules and ions, as well as condensation/evaporation and coagulation. It is found that the resulting dynamics of the formation of aerosol particle nuclei is not a simple sum of ion and binary (water vapor/sulfuric acid) nucleation rates. This dynamics is determined by the ratio of critical radii of nucleated particles due to binary and ion nucleation of these substances (rcr_bin and rcr_ion) depending on temperature, relative humidity, and ionization rate. This should be taken into account in modeling the gas and aerosol composition of the atmosphere and comparing calculated and observed data.

scholarly journals A chamber study of the influence of boreal BVOC emissions and sulfuric acid on nanoparticle formation rates at ambient concentrations

2016 ◽  
Vol 16 (4) ◽  
pp. 1955-1970 ◽  
Author(s):  
M. Dal Maso ◽  
L. Liao ◽  
J. Wildt ◽  
A. Kiendler-Scharr ◽  
E. Kleist ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Cloud Condensation Nuclei ◽  
Formation Rate ◽  
Particle Growth ◽  
Oxidation Products ◽  
Aerosol Formation ◽  
Nanoparticle Formation ◽  
Aerosol Nanoparticles ◽  
Chamber Study ◽  
Ambient Concentrations

Abstract. Aerosol formation from biogenic and anthropogenic precursor trace gases in continental background areas affects climate via altering the amount of available cloud condensation nuclei. Significant uncertainty still exists regarding the agents controlling the formation of aerosol nanoparticles. We have performed experiments in the Jülich plant–atmosphere simulation chamber with instrumentation for the detection of sulfuric acid and nanoparticles, and present the first simultaneous chamber observations of nanoparticles, sulfuric acid, and realistic levels and mixtures of biogenic volatile compounds (BVOCs). We present direct laboratory observations of nanoparticle formation from sulfuric acid and realistic BVOC precursor vapour mixtures performed at atmospherically relevant concentration levels. We directly measured particle formation rates separately from particle growth rates. From this, we established that in our experiments, the formation rate was proportional to the product of sulfuric acid and biogenic VOC emission strength. The formation rates were consistent with a mechanism in which nucleating BVOC oxidation products are rapidly formed and activate with sulfuric acid. The growth rate of nanoparticles immediately after birth was best correlated with estimated products resulting from BVOC ozonolysis.

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>

Modelling of sulfuric acid and ammonium sulfate aerosol formation in the aerrea2 reactor

1998 ◽  
Vol 29 ◽  
pp. S87-S88
Author(s):  
Martin Wilck ◽  
Frank Stratmann ◽  
Lars Asbjørn Larsen ◽  
Rita Van Dingenen ◽  
Frank Raes
Keyword(s):  
Sulfuric Acid ◽  
Ammonium Sulfate ◽  
Sulfate Aerosol ◽  
Aerosol Formation

scholarly journals Hydration of the Sulfuric Acid–Methylamine Complex and Implications for Aerosol Formation

2014 ◽  
Vol 118 (35) ◽  
pp. 7430-7441 ◽  
Author(s):  
Danielle J. Bustos ◽  
Berhane Temelso ◽  
George C. Shields
Keyword(s):  
Sulfuric Acid ◽  
Aerosol Formation

Hydration of a sulfuric acid–oxalic acid complex: acid dissociation and its atmospheric implication

RSC Advances ◽  
2015 ◽  
Vol 5 (60) ◽  
pp. 48638-48646 ◽  
Author(s):  
Shou-Kui Miao ◽  
Shuai Jiang ◽  
Jiao Chen ◽  
Yan Ma ◽  
Yu-Peng Zhu ◽  
...  
Keyword(s):  
Density Functional Theory ◽  
Sulfuric Acid ◽  
Oxalic Acid ◽  
Density Functional ◽  
Structural Characteristics ◽  
Acid Dissociation ◽  
Acid Complex ◽  
Functional Theory ◽  
Insight Into

We have investigated structural characteristics and thermodynamics of the hydration of a sulfuric acid–oxalic acid complex using density functional theory to gain insight into the ternary nucleation and its atmospheric implication.

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
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