scholarly journals Effect of ions on sulfuric acid-water binary particle formation: 1. Theory for kinetic- and nucleation-type particle formation and atmospheric implications

2016 ◽  
Vol 121 (4) ◽  
pp. 1736-1751 ◽  
Author(s):  
Joonas Merikanto ◽  
Jonathan Duplissy ◽  
Anni Määttänen ◽  
Henning Henschel ◽  
Neil M. Donahue ◽  
...  
2018 ◽  
Vol 123 (2) ◽  
pp. 1269-1296 ◽  
Author(s):  
Anni Määttänen ◽  
Joonas Merikanto ◽  
Henning Henschel ◽  
Jonathan Duplissy ◽  
Risto Makkonen ◽  
...  

2015 ◽  
Vol 15 (2) ◽  
pp. 2905-2956 ◽  
Author(s):  
M. Olin ◽  
T. Rönkkö ◽  
M. Dal Maso

Abstract. A new exhaust aerosol model CFD-TUTEAM (Tampere University of Technology Exhaust Aerosol Model for Computational Fluid Dynamics) was developed. The model can be used to simulate particle formation and evolution in diesel exhaust. The model has an Eulerian sub-model that provides spatial information within the computational domain, and a computationally less expensive Lagrangian sub-model that can be used to examine particle formation in a high temporal resolution. Particle formation in a laboratory sampling system that includes a porous tube type diluter and an aging chamber was modeled with CFD-TUTEAM. The simulation results imply that over 99% of new particles are formed in the aging chamber region, because nucleation rate remains at high level in the aging chamber due to low dilution ratio and low nucleation exponents. The nucleation exponents for sulfuric acid in sulfuric acid-water nucleation ranging from 0.25 to 1 appeared to fit best with measurement data, which are the same values as the slopes of volatile nucleation mode number concentration vs. raw exhaust sulfuric acid concentration obtained from the measurement data. These nucleation exponents are very low compared to the nucleation exponents obtained from the classical nucleation theory of binary sulfuric acid-water nucleation. The values of nucleation exponent lower than unity suggest that other compounds, such as hydrocarbons, might have a significant role in the nucleation process.


2021 ◽  
Author(s):  
James Brean ◽  
Manuel Dall’Osto ◽  
Rafel Simó ◽  
Zongbo Shi ◽  
David C. S. Beddows ◽  
...  

2018 ◽  
Vol 18 (16) ◽  
pp. 11779-11791 ◽  
Author(s):  
Ximeng Qi ◽  
Aijun Ding ◽  
Pontus Roldin ◽  
Zhengning Xu ◽  
Putian Zhou ◽  
...  

Abstract. Highly oxygenated multifunctional compounds (HOMs) play a key role in new particle formation (NPF), but their quantitative roles in different environments of the globe have not been well studied yet. Frequent NPF events were observed at two “flagship” stations under different environmental conditions, i.e. a remote boreal forest site (SMEAR II) in Finland and a suburban site (SORPES) in polluted eastern China. The averaged formation rate of 6 nm particles and the growth rate of 6–30 nm particles were 0.3 cm−3 s−1 and 4.5 nm h−1 at SMEAR II compared to 2.3 cm−3 s−1 and 8.7 nm h−1 at SORPES, respectively. To explore the differences of NPF at the two stations, the HOM concentrations and NPF events at two sites were simulated with the MALTE-BOX model, and their roles in NPF and particle growth in the two distinctly different environments are discussed. The model provides an acceptable agreement between the simulated and measured concentrations of sulfuric acid and HOMs at SMEAR II. The sulfuric acid and HOM organonitrate concentrations are significantly higher but other HOM monomers and dimers from monoterpene oxidation are lower at SORPES compared to SMEAR II. The model simulates the NPF events at SMEAR II with a good agreement but underestimates the growth of new particles at SORPES, indicating a dominant role of anthropogenic processes in the polluted environment. HOMs from monoterpene oxidation dominate the growth of ultrafine particles at SMEAR II while sulfuric acid and HOMs from aromatics oxidation play a more important role in particle growth. This study highlights the distinct roles of sulfuric acid and HOMs in NPF and particle growth in different environmental conditions and suggests the need for molecular-scale measurements in improving the understanding of NPF mechanisms in polluted areas like eastern China.


2007 ◽  
Vol 7 (1) ◽  
pp. 211-222 ◽  
Author(s):  
M. Ehn ◽  
T. Petäjä ◽  
H. Aufmhoff ◽  
P. Aalto ◽  
K. Hämeri ◽  
...  

Abstract. The hygroscopic growth of aerosol particles present in a boreal forest was measured at a relative humidity of 88%. Simultaneously the gas phase concentration of sulfuric acid, a very hygroscopic compound, was monitored. The focus was mainly on days with new particle formation by nucleation. The measured hygroscopic growth factors (GF) correlated positively with the gaseous phase sulfuric acid concentrations. The smaller the particles, the stronger the correlation, with r=0.20 for 50 nm and r=0.50 for 10 nm particles. The increase in GF due to condensing sulfuric acid is expected to be larger for particles with initially smaller masses. During new particle formation, the changes in solubility of the new particles were calculated during their growth to Aitken mode sizes. As the modal diameter increased, the solubility of the particles decreased. This indicated that the initial particle growth was due to more hygroscopic compounds, whereas the later growth during the evening and night was mainly caused by less hygroscopic or even hydrophobic compounds. For all the measured sizes, a diurnal variation in GF was observed both during days with and without particle formation. The GF was lowest at around midnight, with a mean value of 1.12–1.24 depending on particle size and if new particle formation occurred during the day, and increased to 1.25–1.34 around noon. This can be tentatively explained by day- and nighttime gas-phase chemistry; different vapors will be present depending on the time of day, and through condensation these compounds will alter the hygroscopic properties of the particles in different ways.


2018 ◽  
Vol 18 (3) ◽  
pp. 1835-1861 ◽  
Author(s):  
Johannes Größ ◽  
Amar Hamed ◽  
André Sonntag ◽  
Gerald Spindler ◽  
Hanna Elina Manninen ◽  
...  

Abstract. This paper revisits the atmospheric new particle formation (NPF) process in the polluted Central European troposphere, focusing on the connection with gas-phase precursors and meteorological parameters. Observations were made at the research station Melpitz (former East Germany) between 2008 and 2011 involving a neutral cluster and air ion spectrometer (NAIS). Particle formation events were classified by a new automated method based on the convolution integral of particle number concentration in the diameter interval 2–20 nm. To study the relevance of gaseous sulfuric acid as a precursor for nucleation, a proxy was derived on the basis of direct measurements during a 1-month campaign in May 2008. As a major result, the number concentration of freshly produced particles correlated significantly with the concentration of sulfur dioxide as the main precursor of sulfuric acid. The condensation sink, a factor potentially inhibiting NPF events, played a subordinate role only. The same held for experimentally determined ammonia concentrations. The analysis of meteorological parameters confirmed the absolute need for solar radiation to induce NPF events and demonstrated the presence of significant turbulence during those events. Due to its tight correlation with solar radiation, however, an independent effect of turbulence for NPF could not be established. Based on the diurnal evolution of aerosol, gas-phase, and meteorological parameters near the ground, we further conclude that the particle formation process is likely to start in elevated parts of the boundary layer rather than near ground level.


Sign in / Sign up

Export Citation Format

Share Document