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- Title
Source characterization of Highly Oxidized Multifunctional Compounds in a Boreal Forest Environment using Positive Matrix Factorization.
- Authors
Chao Yan; Wei Nie; Äijälä, Mikko; Rissanen, Matti P.; Canagaratna, Manjula R.; Massoli, Paola; Junninen, Heikki; Jokinen, Tuija; Sarnela, Nina; Häme, Silja; Schobesberger, Siegfried; Canonaco, Francesco; Prevot, Andre S. H.; Petäjä, Tuukka; Kulmala, Markku; Sipilä, Mikko; Worsnop, Douglas R.; Ehn, Mikael
- Abstract
Highly oxidized multifunctional compounds (HOMs) have been demonstrated to be important for atmospheric secondary organic aerosols (SOA) and new particle formation (NPF), yet it remains unclear which the main atmospheric HOM formation pathways are. In this study, a nitrate ion based Chemical Ionization Atmospheric-Pressure-interface Time-of-flight mass spectrometer (CI-APi-TOF) was deployed to measure HOMs in the boreal forest in Hyytiälä, southern Finland. Positive matrix factorization (PMF) was applied to separate the detected HOM species into several factors, relating these “factors” to plausible formation pathways. PMF was performed with a revised error estimation derived from laboratory data, and this approach was validated by mathematical diagnostics of the PMF solutions. Three factors explained the majority (>95%) of the data variation, but the optimal solution found six factors, including two nighttime factors, three daytime factors, and a transport factor. One nighttime factor is almost identical to laboratory spectra generated from monoterpene ozonolysis, while the second likely represents monoterpene oxidation initiated by NO3. The exact chemical processes forming the different daytime factors remain unclear, but they all have clearly distinct diurnal profiles, very likely related to monoterpene oxidation with a strong influence from NO, presumably through its effect on peroxy radical (RO2) chemistry. Apart from these five “local” factors, the sixth factor is interpreted as a transport related factor. These findings improve our understanding of HOM production by confirming current knowledge and inspiring future research directions, and provide new perspectives on using factorization methods to understand short-lived atmospheric species.
- Subjects
TAIGAS; ATMOSPHERIC aerosols; OXIDATION; NITRATES; CHEMICAL ionization mass spectrometry; FACTORIZATION
- Publication
Atmospheric Chemistry & Physics Discussions, 2016, p1
- ISSN
1680-7367
- Publication type
Article
- DOI
10.5194/acp-2016-367