Modeling the role of highly oxidized multifunctional organic molecules for the growth of new particles over the boreal forest region

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http://hdl.handle.net/10138/211419

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Ostrom , E , Putian , Z , Schurgers , G , Mishurov , M , Kivekas , N , Lihavainen , H , Ehn , M , Rissanen , M P , Kurten , T , Boy , M , Swietlicki , E & Roldin , P 2017 , ' Modeling the role of highly oxidized multifunctional organic molecules for the growth of new particles over the boreal forest region ' , Atmospheric Chemistry and Physics , vol. 17 , no. 14 , pp. 8887-8901 . https://doi.org/10.5194/acp-17-8887-2017

Title: Modeling the role of highly oxidized multifunctional organic molecules for the growth of new particles over the boreal forest region
Author: Ostrom, Emilie; Putian, Zhou; Schurgers, Guy; Mishurov, Mikhail; Kivekas, Niku; Lihavainen, Heikki; Ehn, Mikael; Rissanen, Matti P.; Kurten, Theo; Boy, Michael; Swietlicki, Erik; Roldin, Pontus
Contributor: University of Helsinki, Department of Physics
University of Helsinki, Department of Physics
University of Helsinki, Department of Physics
University of Helsinki, Department of Chemistry
University of Helsinki, Department of Physics
University of Helsinki, Department of Physics
Date: 2017-07-24
Language: eng
Number of pages: 15
Belongs to series: Atmospheric Chemistry and Physics
ISSN: 1680-7316
URI: http://hdl.handle.net/10138/211419
Abstract: In this study, the processes behind observed new particle formation (NPF) events and subsequent organicdominated particle growth at the Pallas AtmosphereEcosystem Supersite in Northern Finland are explored with the one-dimensional column trajectory model ADCHEM. The modeled sub-micron particle mass is up to similar 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 V C) atomic ratio of the SOA is nearly 1. This unusually high O V 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 V 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.
Subject: VOLATILITY BASIS-SET
MASTER CHEMICAL MECHANISM
DYNAMIC VEGETATION MODEL
SIZE DISTRIBUTION DATA
AEROSOL FORMATION
TROPOSPHERIC DEGRADATION
ACTIVITY-COEFFICIENTS
EVAPORATION KINETICS
THERMODYNAMIC MODEL
NORTHERN FINLAND
114 Physical sciences
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