Development of a versatile source apportionment analysis based on positive matrix factorization: a case study of the seasonal variation of organic aerosol sources in Estonia

<p>Bootstrap analysis is commonly used to capture the uncertainties of a bilinear receptor model such as the positive matrix factorization (PMF) model. This approach can estimate the factor-related uncertainties and partially assess the rotational ambiguity of the model. The selection of the e...

Full description

Bibliographic Details
Main Authors: A. Vlachou, A. Tobler, H. Lamkaddam, F. Canonaco, K. R. Daellenbach, J.-L. Jaffrezo, M. C. Minguillón, M. Maasikmets, E. Teinemaa, U. Baltensperger, I. El Haddad, A. S. H. Prévôt
Format: Article
Language:English
Published: Copernicus Publications 2019-06-01
Series:Atmospheric Chemistry and Physics
Online Access:https://www.atmos-chem-phys.net/19/7279/2019/acp-19-7279-2019.pdf
_version_ 1819060686254243840
author A. Vlachou
A. Tobler
H. Lamkaddam
F. Canonaco
K. R. Daellenbach
K. R. Daellenbach
J.-L. Jaffrezo
M. C. Minguillón
M. Maasikmets
E. Teinemaa
U. Baltensperger
I. El Haddad
A. S. H. Prévôt
author_facet A. Vlachou
A. Tobler
H. Lamkaddam
F. Canonaco
K. R. Daellenbach
K. R. Daellenbach
J.-L. Jaffrezo
M. C. Minguillón
M. Maasikmets
E. Teinemaa
U. Baltensperger
I. El Haddad
A. S. H. Prévôt
author_sort A. Vlachou
collection DOAJ
description <p>Bootstrap analysis is commonly used to capture the uncertainties of a bilinear receptor model such as the positive matrix factorization (PMF) model. This approach can estimate the factor-related uncertainties and partially assess the rotational ambiguity of the model. The selection of the environmentally plausible solutions, though, can be challenging, and a systematic approach to identify and sort the factors is needed. For this, comparison of the factors between each bootstrap run and the initial PMF output, as well as with externally determined markers, is crucial. As a result, certain solutions that exhibit suboptimal factor separation should be discarded. The retained solutions would then be used to test the robustness of the PMF output. Meanwhile, analysis of filter samples with the Aerodyne aerosol mass spectrometer and the application of PMF and bootstrap analysis on the bulk water-soluble organic aerosol mass spectra have provided insight into the source identification and their uncertainties. Here, we investigated a full yearly cycle of the sources of organic aerosol (OA) at three sites in Estonia: Tallinn (urban), Tartu (suburban) and Kohtla-Järve (KJ; industrial). We identified six OA sources and an inorganic dust factor. The primary OA types included biomass burning, dominant in winter in Tartu and accounting for 73&thinsp;%&thinsp;<span class="inline-formula">±</span>&thinsp;21&thinsp;% of the total OA, primary biological OA which was abundant in Tartu and Tallinn in spring (21&thinsp;%&thinsp;<span class="inline-formula">±</span>&thinsp;8&thinsp;% and 11&thinsp;%&thinsp;<span class="inline-formula">±</span>&thinsp;5&thinsp;%, respectively), and two other primary OA types lower in mass. A sulfur-containing OA was related to road dust and tire abrasion which exhibited a rather stable yearly cycle, and an oil OA was connected to the oil shale industries in KJ prevailing at this site that comprises 36&thinsp;%&thinsp;<span class="inline-formula">±</span>&thinsp;14&thinsp;% of the total OA in spring. The secondary OA sources were separated based on their seasonal behavior: a winter oxygenated OA dominated in winter (36&thinsp;%&thinsp;<span class="inline-formula">±</span>&thinsp;14&thinsp;% for KJ, 25&thinsp;%&thinsp;<span class="inline-formula">±</span>&thinsp;9&thinsp;% for Tallinn and 13&thinsp;%&thinsp;<span class="inline-formula">±</span>&thinsp;5&thinsp;% for Tartu) and was correlated with benzoic and phthalic acid, implying an anthropogenic origin. A summer oxygenated OA was the main source of OA in summer at all sites (26&thinsp;%&thinsp;<span class="inline-formula">±</span>&thinsp;5&thinsp;% in KJ, 41&thinsp;%&thinsp;<span class="inline-formula">±</span>&thinsp;7&thinsp;% in Tallinn and 35&thinsp;%&thinsp;<span class="inline-formula">±</span>&thinsp;7&thinsp;% in Tartu) and exhibited high correlations with oxidation products of <span class="inline-formula"><i>a</i></span>-pinene-like pinic acid and 3-methyl-1, 2, 3-butanetricarboxylic acid (MBTCA), suggesting a biogenic origin.</p>
first_indexed 2024-12-21T14:30:56Z
format Article
id doaj.art-281c9143d36f47099f11ea2125cd4f68
institution Directory Open Access Journal
issn 1680-7316
1680-7324
language English
last_indexed 2024-12-21T14:30:56Z
publishDate 2019-06-01
publisher Copernicus Publications
record_format Article
series Atmospheric Chemistry and Physics
spelling doaj.art-281c9143d36f47099f11ea2125cd4f682022-12-21T19:00:30ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242019-06-01197279729510.5194/acp-19-7279-2019Development of a versatile source apportionment analysis based on positive matrix factorization: a case study of the seasonal variation of organic aerosol sources in EstoniaA. Vlachou0A. Tobler1H. Lamkaddam2F. Canonaco3K. R. Daellenbach4K. R. Daellenbach5J.-L. Jaffrezo6M. C. Minguillón7M. Maasikmets8E. Teinemaa9U. Baltensperger10I. El Haddad11A. S. H. Prévôt12Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen PSI, SwitzerlandLaboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen PSI, SwitzerlandLaboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen PSI, SwitzerlandLaboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen PSI, SwitzerlandLaboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen PSI, Switzerlandnow at: Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, P.O. Box 64, 00014, Helsinki, FinlandUniversité Grenoble Alpes, CNRS, IRD, G-INP, IGE, 38000 Grenoble, FranceInstitute of Environmental Assessment and Water Research (IDAEA), CSIC, 08034 Barcelona, SpainEstonian Environmental Research Centre, 10617, Tallinn, EstoniaEstonian Environmental Research Centre, 10617, Tallinn, EstoniaLaboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen PSI, SwitzerlandLaboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen PSI, SwitzerlandLaboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen PSI, Switzerland<p>Bootstrap analysis is commonly used to capture the uncertainties of a bilinear receptor model such as the positive matrix factorization (PMF) model. This approach can estimate the factor-related uncertainties and partially assess the rotational ambiguity of the model. The selection of the environmentally plausible solutions, though, can be challenging, and a systematic approach to identify and sort the factors is needed. For this, comparison of the factors between each bootstrap run and the initial PMF output, as well as with externally determined markers, is crucial. As a result, certain solutions that exhibit suboptimal factor separation should be discarded. The retained solutions would then be used to test the robustness of the PMF output. Meanwhile, analysis of filter samples with the Aerodyne aerosol mass spectrometer and the application of PMF and bootstrap analysis on the bulk water-soluble organic aerosol mass spectra have provided insight into the source identification and their uncertainties. Here, we investigated a full yearly cycle of the sources of organic aerosol (OA) at three sites in Estonia: Tallinn (urban), Tartu (suburban) and Kohtla-Järve (KJ; industrial). We identified six OA sources and an inorganic dust factor. The primary OA types included biomass burning, dominant in winter in Tartu and accounting for 73&thinsp;%&thinsp;<span class="inline-formula">±</span>&thinsp;21&thinsp;% of the total OA, primary biological OA which was abundant in Tartu and Tallinn in spring (21&thinsp;%&thinsp;<span class="inline-formula">±</span>&thinsp;8&thinsp;% and 11&thinsp;%&thinsp;<span class="inline-formula">±</span>&thinsp;5&thinsp;%, respectively), and two other primary OA types lower in mass. A sulfur-containing OA was related to road dust and tire abrasion which exhibited a rather stable yearly cycle, and an oil OA was connected to the oil shale industries in KJ prevailing at this site that comprises 36&thinsp;%&thinsp;<span class="inline-formula">±</span>&thinsp;14&thinsp;% of the total OA in spring. The secondary OA sources were separated based on their seasonal behavior: a winter oxygenated OA dominated in winter (36&thinsp;%&thinsp;<span class="inline-formula">±</span>&thinsp;14&thinsp;% for KJ, 25&thinsp;%&thinsp;<span class="inline-formula">±</span>&thinsp;9&thinsp;% for Tallinn and 13&thinsp;%&thinsp;<span class="inline-formula">±</span>&thinsp;5&thinsp;% for Tartu) and was correlated with benzoic and phthalic acid, implying an anthropogenic origin. A summer oxygenated OA was the main source of OA in summer at all sites (26&thinsp;%&thinsp;<span class="inline-formula">±</span>&thinsp;5&thinsp;% in KJ, 41&thinsp;%&thinsp;<span class="inline-formula">±</span>&thinsp;7&thinsp;% in Tallinn and 35&thinsp;%&thinsp;<span class="inline-formula">±</span>&thinsp;7&thinsp;% in Tartu) and exhibited high correlations with oxidation products of <span class="inline-formula"><i>a</i></span>-pinene-like pinic acid and 3-methyl-1, 2, 3-butanetricarboxylic acid (MBTCA), suggesting a biogenic origin.</p>https://www.atmos-chem-phys.net/19/7279/2019/acp-19-7279-2019.pdf
spellingShingle A. Vlachou
A. Tobler
H. Lamkaddam
F. Canonaco
K. R. Daellenbach
K. R. Daellenbach
J.-L. Jaffrezo
M. C. Minguillón
M. Maasikmets
E. Teinemaa
U. Baltensperger
I. El Haddad
A. S. H. Prévôt
Development of a versatile source apportionment analysis based on positive matrix factorization: a case study of the seasonal variation of organic aerosol sources in Estonia
Atmospheric Chemistry and Physics
title Development of a versatile source apportionment analysis based on positive matrix factorization: a case study of the seasonal variation of organic aerosol sources in Estonia
title_full Development of a versatile source apportionment analysis based on positive matrix factorization: a case study of the seasonal variation of organic aerosol sources in Estonia
title_fullStr Development of a versatile source apportionment analysis based on positive matrix factorization: a case study of the seasonal variation of organic aerosol sources in Estonia
title_full_unstemmed Development of a versatile source apportionment analysis based on positive matrix factorization: a case study of the seasonal variation of organic aerosol sources in Estonia
title_short Development of a versatile source apportionment analysis based on positive matrix factorization: a case study of the seasonal variation of organic aerosol sources in Estonia
title_sort development of a versatile source apportionment analysis based on positive matrix factorization a case study of the seasonal variation of organic aerosol sources in estonia
url https://www.atmos-chem-phys.net/19/7279/2019/acp-19-7279-2019.pdf
work_keys_str_mv AT avlachou developmentofaversatilesourceapportionmentanalysisbasedonpositivematrixfactorizationacasestudyoftheseasonalvariationoforganicaerosolsourcesinestonia
AT atobler developmentofaversatilesourceapportionmentanalysisbasedonpositivematrixfactorizationacasestudyoftheseasonalvariationoforganicaerosolsourcesinestonia
AT hlamkaddam developmentofaversatilesourceapportionmentanalysisbasedonpositivematrixfactorizationacasestudyoftheseasonalvariationoforganicaerosolsourcesinestonia
AT fcanonaco developmentofaversatilesourceapportionmentanalysisbasedonpositivematrixfactorizationacasestudyoftheseasonalvariationoforganicaerosolsourcesinestonia
AT krdaellenbach developmentofaversatilesourceapportionmentanalysisbasedonpositivematrixfactorizationacasestudyoftheseasonalvariationoforganicaerosolsourcesinestonia
AT krdaellenbach developmentofaversatilesourceapportionmentanalysisbasedonpositivematrixfactorizationacasestudyoftheseasonalvariationoforganicaerosolsourcesinestonia
AT jljaffrezo developmentofaversatilesourceapportionmentanalysisbasedonpositivematrixfactorizationacasestudyoftheseasonalvariationoforganicaerosolsourcesinestonia
AT mcminguillon developmentofaversatilesourceapportionmentanalysisbasedonpositivematrixfactorizationacasestudyoftheseasonalvariationoforganicaerosolsourcesinestonia
AT mmaasikmets developmentofaversatilesourceapportionmentanalysisbasedonpositivematrixfactorizationacasestudyoftheseasonalvariationoforganicaerosolsourcesinestonia
AT eteinemaa developmentofaversatilesourceapportionmentanalysisbasedonpositivematrixfactorizationacasestudyoftheseasonalvariationoforganicaerosolsourcesinestonia
AT ubaltensperger developmentofaversatilesourceapportionmentanalysisbasedonpositivematrixfactorizationacasestudyoftheseasonalvariationoforganicaerosolsourcesinestonia
AT ielhaddad developmentofaversatilesourceapportionmentanalysisbasedonpositivematrixfactorizationacasestudyoftheseasonalvariationoforganicaerosolsourcesinestonia
AT ashprevot developmentofaversatilesourceapportionmentanalysisbasedonpositivematrixfactorizationacasestudyoftheseasonalvariationoforganicaerosolsourcesinestonia