Source characterization of highly oxidized multifunctional compounds in a boreal forest environment using positive matrix factorization
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 ioni...
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| Format: | Article |
| Language: | English |
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Copernicus Publications
2016-10-01
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| Series: | Atmospheric Chemistry and Physics |
| Online Access: | https://www.atmos-chem-phys.net/16/12715/2016/acp-16-12715-2016.pdf |
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doaj-4cf707afd44648fba725cce53271fe53 |
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Article |
| collection |
DOAJ |
| language |
English |
| format |
Article |
| sources |
DOAJ |
| author |
C. Yan W. Nie W. Nie M. Äijälä M. P. Rissanen M. R. Canagaratna P. Massoli H. Junninen T. Jokinen T. Jokinen N. Sarnela S. A. K. Häme S. Schobesberger S. Schobesberger F. Canonaco L. Yao A. S. H. Prévôt T. Petäjä T. Petäjä M. Kulmala M. Sipilä D. R. Worsnop D. R. Worsnop M. Ehn |
| spellingShingle |
C. Yan W. Nie W. Nie M. Äijälä M. P. Rissanen M. R. Canagaratna P. Massoli H. Junninen T. Jokinen T. Jokinen N. Sarnela S. A. K. Häme S. Schobesberger S. Schobesberger F. Canonaco L. Yao A. S. H. Prévôt T. Petäjä T. Petäjä M. Kulmala M. Sipilä D. R. Worsnop D. R. Worsnop M. Ehn Source characterization of highly oxidized multifunctional compounds in a boreal forest environment using positive matrix factorization Atmospheric Chemistry and Physics |
| author_facet |
C. Yan W. Nie W. Nie M. Äijälä M. P. Rissanen M. R. Canagaratna P. Massoli H. Junninen T. Jokinen T. Jokinen N. Sarnela S. A. K. Häme S. Schobesberger S. Schobesberger F. Canonaco L. Yao A. S. H. Prévôt T. Petäjä T. Petäjä M. Kulmala M. Sipilä D. R. Worsnop D. R. Worsnop M. Ehn |
| author_sort |
C. Yan |
| title |
Source characterization of highly oxidized multifunctional compounds in a boreal forest environment using positive matrix factorization |
| title_short |
Source characterization of highly oxidized multifunctional compounds in a boreal forest environment using positive matrix factorization |
| title_full |
Source characterization of highly oxidized multifunctional compounds in a boreal forest environment using positive matrix factorization |
| title_fullStr |
Source characterization of highly oxidized multifunctional compounds in a boreal forest environment using positive matrix factorization |
| title_full_unstemmed |
Source characterization of highly oxidized multifunctional compounds in a boreal forest environment using positive matrix factorization |
| title_sort |
source characterization of highly oxidized multifunctional compounds in a boreal forest environment using positive matrix factorization |
| publisher |
Copernicus Publications |
| series |
Atmospheric Chemistry and Physics |
| issn |
1680-7316 1680-7324 |
| publishDate |
2016-10-01 |
| description |
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, which agrees well
with an estimate based on ambient data. 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 NO<sub>3</sub>. 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 (RO<sub>2</sub>) 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. |
| url |
https://www.atmos-chem-phys.net/16/12715/2016/acp-16-12715-2016.pdf |
| work_keys_str_mv |
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doaj-4cf707afd44648fba725cce53271fe532020-11-24T23:04:23ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242016-10-0116127151273110.5194/acp-16-12715-2016Source characterization of highly oxidized multifunctional compounds in a boreal forest environment using positive matrix factorizationC. Yan0W. Nie1W. Nie2M. Äijälä3M. P. Rissanen4M. R. Canagaratna5P. Massoli6H. Junninen7T. Jokinen8T. Jokinen9N. Sarnela10S. A. K. Häme11S. Schobesberger12S. Schobesberger13F. Canonaco14L. Yao15A. S. H. Prévôt16T. Petäjä17T. Petäjä18M. Kulmala19M. Sipilä20D. R. Worsnop21D. R. Worsnop22M. Ehn23Department of Physics, University of Helsinki, Helsinki, 00140, FinlandDepartment of Physics, University of Helsinki, Helsinki, 00140, FinlandJoint International Research Laboratory of Atmospheric and Earth System Sciences, School of Atmospheric Sciences, Nanjing University, Nanjing, 210046, ChinaDepartment of Physics, University of Helsinki, Helsinki, 00140, FinlandDepartment of Physics, University of Helsinki, Helsinki, 00140, FinlandAerodyne Research, Inc., Billerica, MA 01821, USAAerodyne Research, Inc., Billerica, MA 01821, USADepartment of Physics, University of Helsinki, Helsinki, 00140, FinlandDepartment of Physics, University of Helsinki, Helsinki, 00140, Finlandnow at: Department of Chemistry, University of California, Irvine, CA, 92617, USADepartment of Physics, University of Helsinki, Helsinki, 00140, FinlandDepartment of Physics, University of Helsinki, Helsinki, 00140, FinlandDepartment of Physics, University of Helsinki, Helsinki, 00140, Finlandnow at: Department of Atmospheric Sciences, University of Washington, Seattle, Washington 98195, USALaboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, 5232, SwitzerlandShanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science & Engineering, Fudan University, Shanghai, 200433, ChinaLaboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, 5232, SwitzerlandDepartment of Physics, University of Helsinki, Helsinki, 00140, FinlandJoint International Research Laboratory of Atmospheric and Earth System Sciences, School of Atmospheric Sciences, Nanjing University, Nanjing, 210046, ChinaDepartment of Physics, University of Helsinki, Helsinki, 00140, FinlandDepartment of Physics, University of Helsinki, Helsinki, 00140, FinlandDepartment of Physics, University of Helsinki, Helsinki, 00140, FinlandAerodyne Research, Inc., Billerica, MA 01821, USADepartment of Physics, University of Helsinki, Helsinki, 00140, FinlandHighly 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, which agrees well with an estimate based on ambient data. 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 NO<sub>3</sub>. 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 (RO<sub>2</sub>) 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.https://www.atmos-chem-phys.net/16/12715/2016/acp-16-12715-2016.pdf |