Browsing by Subject "HOM"
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(2020)This thesis presents the Atmospherically Relevant Chemistry and Aerosol Box Model (ARCA box), which is used for simulating atmospheric chemistry and the time evolution of aerosol particles and the formation of stable molecular clusters. The model can be used for example in solving of the concentrations of atmospheric trace gases formed from some predefined precursors, simulation and design of smog chamber experiments or indoor air quality estimation. The backbone of ARCAs chemical library comes from Master Chemical Mechanism (MCM), extended with Peroxy Radical Autoxidation Mechanism (PRAM), and is further extendable with any new reactions. Molecular clustering is simulated with the Atmospheric Cluster Dynamics Code (ACDC). The particle size distribution is represented with two alternative methods whose size and grid density are fully configurable. The evolution of the particle size distribution due to the condensation of low volatile organic vapours and the Brownian coagulation is simulated using established kinetic and thermodynamic theories. The user interface of ARCA differs considerably from the previous comparable models. The model has a graphical user interface which improves its usability and repeatability of the simulations. The user interface increases the potential of ARCA being used also outside the modelling community, for example in the experimental atmospheric sciences or by authorities.
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(2022)The effects of atmospheric aerosol particles on Earth’s radiative balance are mainly cooling, which is mostly due their indirect effects with clouds. In the Arctic more than half of the cloud condensation nuclei (CCN) production is originated from secondary aerosols, and to further the understanding of Arctic climate and its changes due to the global warming, it is necessary to better understand the secondary aerosol processes there. Highly oxygenated organic molecules (HOM) are known to be important for the formation and especially for the growth of newly formed secondary aerosols to climate relevant sizes. Because of the low volatilities of HOM, they can condense onto the smallest particles, which is crucial for the growth of the new particles. Volatile organic compounds (VOC), especially monoterpenes, are known to be sources of HOM in boreal forest, but in the Arctic where the vegetation is scarce the sources of HOM have not yet been identified. The processes related to secondary aerosol formation in the Arctic are still not fully understood. Especially the observations of HOM and their sources are lacking. Recent studies in Ny-Ålesund, Svalbard showed that multiple aerosol precursors are found to be present in the Arctic atmosphere, as well as contributing to the early stages of the formation of secondary particles. However, more molecular scale observations of aerosol precursors are still needed to form a full picture of the Arctic climate processes. In this thesis, the different aerosol precursors and their contributions to the new particle formations in high Arctic location Ny-Ålesund, Svalbard were analysed. Chemical compositions of HOM were identified for the first time from Arctic atmosphere, and their contributions to new particle formation in high Arctic location were investigated. Because of the high concentrations of HOM during the observed NPF events, it can be suggested that they were contributing to the nucleation of aerosol particles. Particle growth rate calculation shows that the HOM present in the study site were responsible for up to 50% of the total growth of the newly formed particles. VOC flux measurements done in same location were also analysed, and Arctic tundra in Svalbard was found out to be a source of at least four different VOC. Furthermore, the identified HOM were linked to the VOC flux measurements, suggesting a possible link between Arctic VOC and HOM.
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(2020)Atmospheric aerosol particles affect Earth’s radiation balance, human health and visibility. Secondary organic aerosol (SOA) contributes a significant fraction to the total atmospheric organic aerosol, and thus plays an important role in climate change. SOA is formed through oxidation of volatile organic compounds (VOCs) and it consists of many individual organic compounds with varying properties. The oxidation products of VOCs include highly oxygenated organic molecules (HOM) that are estimated to explain a large fraction of SOA formation. To estimate the climate impacts of SOA it is essential to understand its properties in the atmosphere. In this thesis, a method to investigate thermally induced evaporation of organic aerosol was developed. SOA particles were generated in a flow tube from alpha-pinene ozonolysis and then directed into a heated tube to initiate particle evaporation. The size distribution of the particles was measured with parallel identification of the evaporated HOM. This method was capable of providing information of SOA evaporation behaviour and the particle-phase composition at different temperatures. Mass spectra of the evaporated HOM and particle size distribution data were analyzed. The obtained results suggest that SOA contains compounds with a wide range of volatilities, including HOM monomers, dimers and trimers. The volatility behaviour of the particulate HOM and their contribution to SOA particle mass was studied. Furthermore, indications of particle-phase reactions occurring in SOA were found.
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