Sources, sinks and transformation of BVOCs and aerosols in boreal forest boundary layer

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http://urn.fi/URN:ISBN:978-952-7276-02-0
Julkaisun nimi: Sources, sinks and transformation of BVOCs and aerosols in boreal forest boundary layer
Tekijä: Zhou, Putian
Muu tekijä: Helsingin yliopisto, matemaattis-luonnontieteellinen tiedekunta, fysiikan laitos
Opinnäytteen taso: Väitöskirja (artikkeli)
Tiivistelmä: A large amount of biogenic volatile organic compounds (BVOCs) are emitted from boreal forests. Once emitted, BVOCs can be oxidized in the air, participate in particle formation and growth and thus indirectly affect local, regional and global climate. BVOCs act as a bridge between the biosphere and the atmosphere including atmospheric chemistry in both gas and particle phases. In this thesis we studied the in-canopy sources and sinks of BVOCs, the roles of BVOCs in gas and particle phases, as well as the impact of aerosol dynamics on the vertical aerosol fluxes in the planetary boundary layer. Several findings in this thesis are shown below: (1) By using a newly implemented gas dry deposition model in a one-dimensional chemical transport model SOSAA (model to Simulate the concentrations of Organic vapours, Sulphuric Acid and Aerosols) we simulated the in-canopy source and sink terms of 12 featured BVOCs. According to the strength of individual terms, BVOCs were classified into five categories: Cemis in which most of the emitted gases are transported out of the canopy, Cemis-chem in which most of the emitted gases are quickly oxidized inside the canopy, Cemis-depo in which emissions are comparable to deposition, Cdepo in which the dominant deposition sink leads to downward fluxes and Cchem-depo in which the chemical production compensates a part of deposition. (2) High upward fluxes of formic acid over a boreal forest were observed. The required unknown precursors and emission sources were quantified to explain the missing sources inside the canopy. (3) The simulated O3 concentration change due to chemical reactions related to BVOCs was in average less than 10% of the deposition sink. (4) The highly oxidized multifunctional organic molecules (HOMs) play a dominant role in the growth of new particles over the sub-Arctic forest region at the Pallas Atmosphere-Ecosystem Supersite and account for ∼ 75% of total SOA mass during new particle formation events. (5) The modelled vertical aerosol fluxes above the canopy caused by aerosol dynamics were comparable or sometimes exceeded that caused by particle dry deposition. This introduced large biases between measured flux and the particle dry deposition flux. The findings (1), (2), (3), (5) were obtained over the boreal forest at SMEAR (Station for Measuring ecosystem-Atmosphere Relations) II. This thesis provides a new numerical tool to analyse detailed sources and sinks of BVOCs, which can be applied in other ecosystems and further implemented in large-scale models.A large amount of biogenic volatile organic compounds (BVOCs) are emitted from boreal forests. Once emitted, BVOCs can be oxidized in the air, participate in particle formation and growth and thus indirectly affect local, regional and global climate. BVOCs act as a bridge between the biosphere and the atmosphere including atmospheric chemistry in both gas and particle phases. In this thesis we studied the in-canopy sources and sinks of BVOCs, the roles of BVOCs in gas and particle phases, as well as the impact of aerosol dynamics on the vertical aerosol fluxes in the planetary boundary layer. Several findings in this thesis are shown below: (1) By using a newly implemented gas dry deposition model in a one-dimensional chemical transport model SOSAA (model to Simulate the concentrations of Organic vapours, Sulphuric Acid and Aerosols) we simulated the in-canopy source and sink terms of 12 featured BVOCs. According to the strength of individual terms, BVOCs were classified into five categories: Cemis in which most of the emitted gases are transported out of the canopy, Cemis-chem in which most of the emitted gases are quickly oxidized inside the canopy, Cemis-depo in which emissions are comparable to deposition, Cdepo in which the dominant deposition sink leads to downward fluxes and Cchem-depo in which the chemical production compensates a part of deposition. (2) High upward fluxes of formic acid over a boreal forest were observed. The required unknown precursors and emission sources were quantified to explain the missing sources inside the canopy. (3) The simulated O3 concentration change due to chemical reactions related to BVOCs was in average less than 10% of the deposition sink. (4) The highly oxidized multifunctional organic molecules (HOMs) play a dominant role in the growth of new particles over the sub-Arctic forest region at the Pallas Atmosphere-Ecosystem Supersite and account for ∼ 75% of total SOA mass during new particle formation events. (5) The modelled vertical aerosol fluxes above the canopy caused by aerosol dynamics were comparable or sometimes exceeded that caused by particle dry deposition. This introduced large biases between measured flux and the particle dry deposition flux. The findings (1), (2), (3), (5) were obtained over the boreal forest at SMEAR (Station for Measuring ecosystem-Atmosphere Relations) II. This thesis provides a new numerical tool to analyse detailed sources and sinks of BVOCs, which can be applied in other ecosystems and further implemented in large-scale models.
URI: URN:ISBN:978-952-7276-02-0
http://hdl.handle.net/10138/234205
Päiväys: 2018-04-20
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