Modelling Iodine Particle Formation and Growth from Seaweed in a Chamber

2005 ◽  
Vol 2 (4) ◽  
pp. 271 ◽  
Author(s):  
L. Pirjola ◽  
C. D. O'Dowd ◽  
Y. J. Yoon ◽  
K. Sellegri

Environmental Context.Iodine is an important trace species in the marine atmosphere. It contributes to ozone depletion and new particle formation. In recent years, its importance has been realised, however, there is still a gap in our knowledge, from a theoretical framework, of the dominant mechanisms leading to new particle formation and previous theoretical frameworks have not been adequately developed or well understood. This paper presents a state-of-the-art theoretical framework for evaluating the prediction of iodine oxide nucleation and subsequent aerosol growth. Abstract. A sectional atmospheric chemistry and aerosol dynamics box model (AEROFOR) was further developed and used to simulate ultra-fine particle formation and growth from seaweed in a chamber flushed with particle-free atmospheric air. In the model, thermodynamically stable clusters were formed by dimer nucleation of OIO vapour, whose precursor was assumed to be molecular I2 emitted by seaweed. Fractal geometry of particles was taken into account. For the I2 fluxes of (0.5–1.5) × 109 cm−3 s−1 the model predicted strong particle bursts, the steady state concentrations of I2 vapour and particles larger than 3 nm were as high as 4 × 109–1.2 × 1010 cm−3 and 5.0 × 106–9.2 × 106 cm−3 respectively. The steady state was reached in less than 150 s and the predicted growth rates of 3–6 nm particles varied in the range of 1.2–3.6 nm min−1. Sensitivity of the size distribution against I2O3 cluster formation, an extra condensable vapour, the photolysis rate of the OIO vapour as well as against the density of (OIO)n-clusters was discussed. The modelled results were in good agreement with the chamber measurements performed during the BIOFLUX campaign in September, 2003, in Mace Head, Ireland, confirming that I2 emissions and nucleation of iodine oxides can largely explain the coastal nucleation phenomenon.

2010 ◽  
Vol 2010 ◽  
pp. 1-9 ◽  
Author(s):  
Ciaran Monahan ◽  
Henri Vuollekoski ◽  
Markku Kulmala ◽  
Colin O'Dowd

A modal atmospheric aerosol model (M7) is evaluated in terms of predicting marine new particle formation and growth. Simulations were carried out for three different nucleation schemes involving (1) kinetic self-nucleation of OIO (2) nucleationviaOIO activation by H2SO4and (3) nucleationviaOIO activation by H2SO4plus condensation of a low-volatility organic vapour. Peak OIO and H2SO4vapour concentrations were both limited to6×106molecules cm-3at noontime while the peak organic vapour concentration was limited to12×106molecules cm-3. All simulations produced significant concentrations of new particles in the Aitken mode. From a base case particle concentration of 222 cm-3at radii >15 nm, increases in concentrations to 366 cm-3were predicted from the OIO-OIO case, 722 cm-3for the OIO-H2SO4case, and 1584 cm-3for the OIO-H2SO4case with additional condensing organic vapours. The results indicate that open ocean new particle production is feasible for clean conditions; however, new particle production becomes most significant when an additional condensable organic vapour is available to grow the newly formed particles to larger sizes. Comparison to sectional model for a typical case study demonstrated good agreement and the validity of using the modal model.


2015 ◽  
Vol 103 ◽  
pp. 7-17 ◽  
Author(s):  
Z.B. Wang ◽  
M. Hu ◽  
X.Y. Pei ◽  
R.Y. Zhang ◽  
P. Paasonen ◽  
...  

2012 ◽  
Vol 12 (9) ◽  
pp. 4297-4312 ◽  
Author(s):  
I. K. Ortega ◽  
T. Suni ◽  
M. Boy ◽  
T. Grönholm ◽  
H. E. Manninen ◽  
...  

Abstract. Formation of new aerosol particles by nucleation and growth is a significant source of aerosols in the atmosphere. New particle formation events usually take place during daytime, but in some locations they have been observed also at night. In the present study we have combined chamber experiments, quantum chemical calculations and aerosol dynamics models to study nocturnal new particle formation. All our approaches demonstrate, in a consistent manner, that the oxidation products of monoterpenes play an important role in nocturnal nucleation events. By varying the conditions in our chamber experiments, we were able to reproduce the very different types of nocturnal events observed earlier in the atmosphere. The exact strength, duration and shape of the events appears to be sensitive to the type and concentration of reacting monoterpenes, as well as the extent to which the monoterpenes are exposed to ozone and potentially other atmospheric oxidants.


2019 ◽  
Vol 19 (16) ◽  
pp. 10537-10555 ◽  
Author(s):  
Simo Hakala ◽  
Mansour A. Alghamdi ◽  
Pauli Paasonen ◽  
Ville Vakkari ◽  
Mamdouh I. Khoder ◽  
...  

Abstract. Atmospheric aerosols have significant effects on human health and the climate. A large fraction of these aerosols originates from secondary new particle formation (NPF), where atmospheric vapors form small particles that subsequently grow into larger sizes. In this study, we characterize NPF events observed at a rural background site of Hada Al Sham (21.802∘ N, 39.729∘ E), located in western Saudi Arabia, during the years 2013–2015. Our analysis shows that NPF events occur very frequently at the site, as 73 % of all the 454 classified days were NPF days. The high NPF frequency is likely explained by the typically prevailing conditions of clear skies and high solar radiation, in combination with sufficient amounts of precursor vapors for particle formation and growth. Several factors suggest that in Hada Al Sham these precursor vapors are related to the transport of anthropogenic emissions from the coastal urban and industrial areas. The median particle formation and growth rates for the NPF days were 8.7 cm−3 s−1 (J7 nm) and 7.4 nm h−1 (GR7−12 nm), respectively, both showing highest values during late summer. Interestingly, the formation and growth rates increase as a function of the condensation sink, likely reflecting the common anthropogenic sources of NPF precursor vapors and primary particles affecting the condensation sink. A total of 76 % of the NPF days showed an unusual progression, where the observed diameter of the newly formed particle mode started to decrease after the growth phase. In comparison to most long-term measurements, the NPF events in Hada Al Sham are exceptionally frequent and strong both in terms of formation and growth rates. In addition, the frequency of the decreasing mode diameter events is higher than anywhere else in the world.


2007 ◽  
pp. 1013-1017
Author(s):  
Sanna-Liisa Sihto ◽  
Henri Vuollekoski ◽  
J. Leppä ◽  
Ilona Riipinen ◽  
Veli-Matti Kerminen ◽  
...  

2020 ◽  
Vol 54 (14) ◽  
pp. 8547-8557 ◽  
Author(s):  
Chenjuan Deng ◽  
Yueyun Fu ◽  
Lubna Dada ◽  
Chao Yan ◽  
Runlong Cai ◽  
...  

2010 ◽  
Vol 10 (14) ◽  
pp. 6721-6735 ◽  
Author(s):  
S. Crumeyrolle ◽  
H. E. Manninen ◽  
K. Sellegri ◽  
G. Roberts ◽  
L. Gomes ◽  
...  

Abstract. Aerosol properties were studied during an intensive airborne measurement campaign that took place at Rotterdam in Netherlands in May 2008 within the framework of the European Aerosol Cloud Climate and Air Quality Interactions project (EUCAARI). The objective of this study is to illustrate seven events of new particle formation (NPF) observed with two Condensation Particle Counters (CPCs) operated on board the ATR-42 research aircraft in airsectors around Rotterdam, and to provide information on the spatial extent of the new particle formation phenomenon based on 1-s resolution measurements of ultra-fine particle (in the size range 3–10 nm diameter, denoted N3-10 hereafter) concentrations. The results show that particle production occurred under the influence of different air mass origins, at different day times and over the North Sea as well as over the continent. The number concentration of freshly nucleated particles (N3-10) varied between 5000 and 100 000 cm−3 within the boundary layer (BL). Furthermore the vertical extension for all nucleation events observed on the ATR-42 never exceeded the upper limit of the BL. The horizontal extent of N3-10 could not be delimited due to inflexible flight plans which could not be modified to accommodate real-time results. However, the NPF events were observed over geographically large areas; typically the horizontal extension was about 100 km and larger.


2020 ◽  
Author(s):  
Vitus Besel ◽  
Jakub Kubečka ◽  
Theo Kurtén ◽  
Hanna Vehkamäki

<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>


2017 ◽  
Vol 44 (6) ◽  
pp. 2958-2966 ◽  
Author(s):  
Claudia Mohr ◽  
Felipe D. Lopez-Hilfiker ◽  
Taina Yli-Juuti ◽  
Arto Heitto ◽  
Anna Lutz ◽  
...  

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