modeling the role of highly oxidized multifunctional organic molecules for the growth of new particles over the boreal forest region
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2017
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Abstract
In this study, the processes behind observed new particle formation
(NPF) events and subsequent organic-dominated particle growth at the Pallas
Atmosphere–Ecosystem Supersite in Northern Finland are explored with the
one-dimensional column trajectory model ADCHEM. The modeled sub-micron
particle mass is up to ∼ 75 % composed of SOA formed from highly
oxidized multifunctional organic molecules (HOMs) with low or extremely low
volatility. In the model the newly formed particles with an initial diameter
of 1.5 nm reach a diameter of 7 nm about 2 h earlier
than what is typically observed at the station. This is an indication that
the model tends to overestimate the initial particle growth. In contrast, the modeled particle growth to CCN size ranges ( > 50 nm in
diameter) seems to be underestimated because the increase in the
concentration of particles above 50 nm in diameter typically occurs
several hours later compared to the observations. Due to the high fraction of
HOMs in the modeled particles, the oxygen-to-carbon (O : C)
atomic ratio of the SOA is nearly 1. This unusually high
O : C and the discrepancy between the modeled and observed
particle growth might be explained by the fact that the model does not
consider any particle-phase reactions involving semi-volatile organic
compounds with relatively low O : C. In the model
simulations where condensation of low-volatility and extremely low-volatility
HOMs explain most of the SOA formation, the phase state of the SOA (assumed
either liquid or amorphous solid) has an insignificant impact on the
evolution of the particle number size distributions. However, the modeled
particle growth rates are sensitive to the method used to estimate the vapor
pressures of the HOMs. Future studies should evaluate how heterogeneous
reactions involving semi-volatility HOMs and other less-oxidized organic
compounds can influence the SOA composition- and size-dependent particle
growth.
| Reference Key |
strm2017atmosphericmodeling
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| Authors | ;E. Öström;E. Öström;Z. Putian;G. Schurgers;M. Mishurov;N. Kivekäs;H. Lihavainen;M. Ehn;M. P. Rissanen;T. Kurtén;M. Boy;E. Swietlicki;P. Roldin;P. Roldin |
| Journal | Journal of agricultural and food chemistry |
| Year | 2017 |
| DOI |
10.5194/acp-17-8887-2017
|
| URL | |
| Keywords |
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