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

  • Emilie Ostrom
  • , Zhou Putian
  • , Guy Schurgers
  • , Mikhail Mishurov
  • , Niku Kivekas
  • , Heikki Lihavainen
  • , Mikael Ehn
  • , Matti P. Rissanen
  • , Theo Kurten
  • , Michael Boy
  • , Erik Swietlicki
  • , Pontus Roldin

Research output: Contribution to journalArticleScientificpeer-review

28 Citations (Scopus)

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 75HOMs) 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 (textgreater 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.
Original languageEnglish
Pages (from-to)8887-8901
Number of pages15
JournalAtmospheric Chemistry and Physics
Volume17
Issue number14
DOIs
Publication statusPublished - 1 Jul 2017
Externally publishedYes
Publication typeA1 Journal article-refereed

Keywords

  • 114 Physical sciences
  • TROPOSPHERIC DEGRADATION
  • EVAPORATION KINETICS
  • AEROSOL FORMATION
  • MASTER CHEMICAL MECHANISM
  • ACTIVITY-COEFFICIENTS
  • DYNAMIC VEGETATION MODEL
  • NORTHERN FINLAND
  • SIZE DISTRIBUTION DATA
  • THERMODYNAMIC MODEL
  • VOLATILITY BASIS-SET

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