scholarly journals Measurements of the aerosol chemical composition and mixing state in the Po Valley using multiple spectroscopic techniques

2014 ◽  
Vol 14 (22) ◽  
pp. 12109-12132 ◽  
Author(s):  
S. Decesari ◽  
J. Allan ◽  
C. Plass-Duelmer ◽  
B. J. Williams ◽  
M. Paglione ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Black Carbon ◽  
Mass Spectrometer ◽  
Organic Aerosol ◽  
Spectroscopic Techniques ◽  
Mixing State ◽  
Mass Spectrometers ◽  
Aerosol Mass Spectrometer ◽  
Po Valley ◽  
Aerosol Mass

Abstract. The use of co-located multiple spectroscopic techniques can provide detailed information on the atmospheric processes regulating aerosol chemical composition and mixing state. So far, field campaigns heavily equipped with aerosol mass spectrometers have been carried out mainly in large conurbations and in areas directly affected by their outflow, whereas lesser efforts have been dedicated to continental areas characterised by a less dense urbanisation. We present here the results obtained at a background site in the Po Valley, Italy, in summer 2009. For the first time in Europe, six state-of-the-art spectrometric techniques were used in parallel: aerosol time-of-flight mass spectrometer (ATOFMS), two aerosol mass spectrometers (high-resolution time-of-flight aerosol mass spectrometer – HR-ToF-AMS and soot particle aerosol mass spectrometer – SP-AMS), thermal desorption aerosol gas chromatography (TAG), chemical ionisation mass spectrometry (CIMS) and (offline) proton nuclear magnetic resonance (1H-NMR) spectroscopy. The results indicate that, under high-pressure conditions, atmospheric stratification at night and early morning hours led to the accumulation of aerosols produced by anthropogenic sources distributed over the Po Valley plain. Such aerosols include primary components such as black carbon (BC), secondary semivolatile compounds such as ammonium nitrate and amines and a class of monocarboxylic acids which correspond to the AMS cooking organic aerosol (COA) already identified in urban areas. In daytime, the entrainment of aged air masses in the mixing layer is responsible for the accumulation of low-volatility oxygenated organic aerosol (LV-OOA) and also for the recycling of non-volatile primary species such as black carbon. According to organic aerosol source apportionment, anthropogenic aerosols accumulating in the lower layers overnight accounted for 38% of organic aerosol mass on average, another 21% was accounted for by aerosols recirculated in residual layers but still originating in northern Italy, while a substantial fraction (41%) was due to the most aged aerosols imported from transalpine areas. The different meteorological regimes also affected the BC mixing state: in periods of enhanced stagnation and recirculation of pollutants, the number fraction of the BC-containing particles determined by ATOFMS was 75% of the total, while in the days of enhanced ventilation of the planetary boundary layer (PBL), such fraction was significantly lower (50%) because of the relative greater influence of non-BC-containing aerosol local sources in the Po Valley. Overall, a full internal mixing between BC and the non-refractory aerosol chemical components was not observed during the experiment in this environment.

scholarly journals Quantitative determination of carbonaceous particle mixing state in Paris using single particle mass spectrometer and aerosol mass spectrometer measurements

2013 ◽  
Vol 13 (4) ◽  
pp. 10345-10393
Author(s):  
R. M. Healy ◽  
J. Sciare ◽  
L. Poulain ◽  
M. Crippa ◽  
A. Wiedensohler ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Mass Spectrometer ◽  
Single Particle ◽  
Organic Aerosol ◽  
Particle Mass ◽  
Mixing State ◽  
Aerosol Mass Spectrometer ◽  
Aerosol Mass ◽  
Particle Mixing ◽  
Mixing States

Abstract. Single particle mixing state information can be a powerful tool for assessing the relative impact of local and regional sources of ambient particulate matter in urban environments. However, quantitative mixing state data are challenging to obtain using single particle mass spectrometers. In this study, the quantitative chemical composition of carbonaceous single particles has been estimated using an aerosol time-of-flight mass spectrometer (ATOFMS) as part of the MEGAPOLI 2010 winter campaign in Paris, France. Relative peak areas of marker ions for elemental carbon (EC), organic aerosol (OA), ammonium, nitrate, sulphate and potassium were compared with concurrent measurements from an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), a thermal/optical OCEC analyser and a particle into liquid sampler coupled with ion chromatography (PILS-IC). ATOFMS-derived mass concentrations reproduced the variability of these species well (R2 = 0.67–0.78), and ten discrete mixing states for carbonaceous particles were identified and quantified. Potassium content was used to identify particles associated with biomass combustion. The chemical mixing state of HR-ToF-AMS organic aerosol factors, resolved using positive matrix factorization, was also investigated through comparison with the ATOFMS dataset. The results indicate that hydrocarbon-like OA (HOA) detected in Paris is associated with two EC-rich mixing states which differ in their relative sulphate content, while fresh biomass burning OA (BBOA) is associated with two mixing states which differ significantly in their OA/EC ratios. Aged biomass burning OA (OOA2-BBOA) was found to be significantly internally mixed with nitrate, while secondary, oxidized OA (OOA) was associated with five particle mixing states, each exhibiting different relative secondary inorganic ion content. Externally mixed secondary organic aerosol was not observed. These findings demonstrate the heterogeneity of primary and secondary organic aerosol mixing states in Paris. Examination of the temporal behaviour and chemical composition of the ATOFMS classes also enabled estimation of the relative contribution of transported emissions of each chemical species and total particle mass in the size range investigated. Only 22% of the total ATOFMS-derived particle mass was apportioned to fresh, local emissions, with 78% apportioned to regional/continental scale emissions.

scholarly journals Measurements of the aerosol chemical composition and mixing state in the Po Valley using multiple spectroscopic techniques

2014 ◽  
Vol 14 (7) ◽  
pp. 9275-9343 ◽  
Author(s):  
S. Decesari ◽  
J. Allan ◽  
C. Plass-Duelmer ◽  
B. J. Williams ◽  
M. Paglione ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Mass Spectrometer ◽  
Time Of Flight ◽  
Organic Aerosol ◽  
Anthropogenic Sources ◽  
Spectroscopic Techniques ◽  
Po Valley ◽  
Aerosol Mass ◽  
On Line ◽  
Aerosol Chemical Composition

Abstract. The use of co-located multiple spectroscopic techniques can provide detailed information on the atmospheric processes regulating aerosol chemical composition and mixing state. So far, field campaigns heavily equipped with aerosol mass spectrometers have been carried out mainly in large conurbations and in areas directly affected by their outflow, whereas lesser efforts have been dedicated to continental areas characterized by a less dense urbanization. We present here the results obtained in San Pietro Capofiume, which is located in a sparsely inhabited sector of the Po Valley, Italy. The experiment was carried out in summer 2009 in the framework of the EUCAARI project ("European Integrated Project on Aerosol, Cloud Climate Aerosol Interaction"). For the first time in Europe, six state-of-the-art techniques were used in parallel: (1) on-line TSI aerosol time-of-flight mass spectrometer (ATOFMS), (2) on-line Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS), (3) soot particle aerosol mass spectrometer (SP-AMS), (4) on-line high resolution time-of-flight mass spectrometer-thermal desorption aerosol gas chromatograph (HR-ToFMS-TAG), (5) off-line twelve-hour resolution proton nuclear magnetic resonance (H-NMR) spectroscopy, and (6) chemical ionization mass spectrometry (CIMS) for the analysis of gas-phase precursors of secondary aerosol. Data from each aerosol spectroscopic method were analysed individually following ad-hoc tools (i.e. PMF for AMS, Art-2a for ATOFMS). The results obtained from each techniques are herein presented and compared. This allows us to clearly link the modifications in aerosol chemical composition to transitions in air mass origin and meteorological regimes. Under stagnant conditions, atmospheric stratification at night and early morning hours led to the accumulation of aerosols produced by anthropogenic sources distributed over the Po Valley plain. Such aerosols include primary components such as black carbon (BC), only partly internally mixed with secondary semivolatile compounds such as ammonium nitrate and amines. Other organic components originating from anthropogenic sources at night include monocarboxylic acids which correspond to an AMS factor analogous to the "cooking" organic aerosol (COA) already identified in urban areas. In daytime, enhanced mixing in the planetary boundary layer (PBL) along with increasing temperature determined dramatic changes in aerosol composition caused by the evaporation of semivolatile components and by the entrainment of aged aerosols transported downwards from residual layers. In other words, the entrainment of aged air masses is responsible for the accumulation of low-volatility oxygenated organic aerosol (LV-OOAs) and also for the recycling of primary species such as black carbon. The LV-OOA concentrations were shown to correlate to the simple meteorological tracers of humid PBL air produced by daytime convection over land areas. In particular, both PMF-AMS and PMF-NMR could resolve two components of LV-OOA: one from long-range transport from Central Europe, the second from recirculated PBL air from the Po Valley. According to organic aerosol source apportionment by PMF-AMS, anthropogenic aerosols accumulating in the lower layers overnight accounted for 38% of organic aerosol mass on average, another 21% was accounted for by aerosols recirculated in residual layers but still originating in North Italy, while a substantial fraction (41%) was due to the most aged aerosols imported from transalpine areas. Overall, the deployment of six state-of-the-art spectrometric techniques provided a comprehensive picture of the nature and source contributions of aerosols and aerosol precursors at a European rural site with unprecedented level of details.

scholarly journals Quantitative determination of carbonaceous particle mixing state in Paris using single-particle mass spectrometer and aerosol mass spectrometer measurements

2013 ◽  
Vol 13 (18) ◽  
pp. 9479-9496 ◽  
Author(s):  
R. M. Healy ◽  
J. Sciare ◽  
L. Poulain ◽  
M. Crippa ◽  
A. Wiedensohler ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Mass Spectrometer ◽  
Single Particle ◽  
Organic Aerosol ◽  
Particle Mass ◽  
Mixing State ◽  
Aerosol Mass Spectrometer ◽  
Aerosol Mass ◽  
Particle Mixing ◽  
Mixing States

Abstract. Single-particle mixing state information can be a powerful tool for assessing the relative impact of local and regional sources of ambient particulate matter in urban environments. However, quantitative mixing state data are challenging to obtain using single-particle mass spectrometers. In this study, the quantitative chemical composition of carbonaceous single particles has been determined using an aerosol time-of-flight mass spectrometer (ATOFMS) as part of the MEGAPOLI 2010 winter campaign in Paris, France. Relative peak areas of marker ions for elemental carbon (EC), organic aerosol (OA), ammonium, nitrate, sulfate and potassium were compared with concurrent measurements from an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), a thermal–optical OCEC analyser and a particle into liquid sampler coupled with ion chromatography (PILS-IC). ATOFMS-derived estimated mass concentrations reproduced the variability of these species well (R2 = 0.67–0.78), and 10 discrete mixing states for carbonaceous particles were identified and quantified. The chemical mixing state of HR-ToF-AMS organic aerosol factors, resolved using positive matrix factorisation, was also investigated through comparison with the ATOFMS dataset. The results indicate that hydrocarbon-like OA (HOA) detected in Paris is associated with two EC-rich mixing states which differ in their relative sulfate content, while fresh biomass burning OA (BBOA) is associated with two mixing states which differ significantly in their OA / EC ratios. Aged biomass burning OA (OOA2-BBOA) was found to be significantly internally mixed with nitrate, while secondary, oxidised OA (OOA) was associated with five particle mixing states, each exhibiting different relative secondary inorganic ion content. Externally mixed secondary organic aerosol was not observed. These findings demonstrate the range of primary and secondary organic aerosol mixing states in Paris. Examination of the temporal behaviour and chemical composition of the ATOFMS classes also enabled estimation of the relative contribution of transported emissions of each chemical species and total particle mass in the size range investigated. Only 22% of the total ATOFMS-derived particle mass was apportioned to fresh, local emissions, with 78% apportioned to regional/continental-scale emissions.

scholarly journals A Black Carbon‐Tracer Method for Estimating Cooking Organic Aerosol From Aerosol Mass Spectrometer Measurements

2019 ◽  
Vol 46 (14) ◽  
pp. 8474-8483 ◽  
Author(s):  
Yao He ◽  
Yele Sun ◽  
Qingqing Wang ◽  
Wei Zhou ◽  
Weiqi Xu ◽  
...  
Keyword(s):  
Black Carbon ◽  
Mass Spectrometer ◽  
Organic Aerosol ◽  
Tracer Method ◽  
Aerosol Mass Spectrometer ◽  
Aerosol Mass

scholarly journals Formation of secondary organic aerosol coating on black carbon particles near vehicular emissions

2017 ◽  
Author(s):  
Alex K. Y. Lee ◽  
Chia-Li Chen ◽  
Jun Liu ◽  
Derek J. Price ◽  
Raghu Betha ◽  
...  
Keyword(s):  
Black Carbon ◽  
Mass Spectrometer ◽  
Secondary Organic Aerosol ◽  
Spectral Characteristics ◽  
Organic Aerosol ◽  
Vehicular Emissions ◽  
Aerosol Mass Spectrometer ◽  
Diurnal Cycles ◽  
Aerosol Mass ◽  
Inorganic Species

Abstract. Black carbon (BC) emitted from incomplete combustion can result in significant impacts on air quality and climate. Understanding the mixing state of ambient BC and the chemical characteristics of its associated coatings are particularly important to evaluate BC fate and environmental impacts. In this study, we investigate the formation of organic coatings on BC particles in an urban environment (Fontana, California) under hot and dry conditions using a Soot-Particle Aerosol Mass Spectrometer (SP-AMS). The SP-AMS was operated in a configuration that can detect refractory BC (rBC) particles and their coatings exclusively. Using the −log(NOx/NOy) ratio as a proxy for photochemical age of air masses, substantial formation of secondary organic aerosol (SOA) coatings on rBC particles was observed due to active photochemistry in the afternoon, whereas primary organic aerosol (POA) components were strongly associated with rBC from fresh vehicular missions in the morning rush hours. There is also evidence that cooking related organic aerosols were externally mixed from rBC. Positive matrix factorization and elemental analysis illustrate that most of the observed SOA coatings were freshly formed, providing an opportunity to examine SOA coating formation on rBC near vehicular emissions. Approximately 7–20 wt % of secondary organic and inorganic species were estimated to be internally mixed with rBC on average, implying that rBC is unlikely the major condensation sinks of SOA in this study. Diurnal cycles of oxygenated organic aerosol (OOA) observed by a co-located standard high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-MS) correlated well with that of SOA coatings on rBC, but their mass spectral characteristics were different from each other. Our results suggest that at least a portion of SOA materials condensed on rBC surface were chemically different from OOA particles that were externally mixed with rBC, although they are both generated from local photochemistry.

scholarly journals Mixing state of carbonaceous aerosol in an urban environment: single particle characterization using the soot particle aerosol mass spectrometer (SP-AMS)

2015 ◽  
Vol 15 (4) ◽  
pp. 1823-1841 ◽  
Author(s):  
A. K. Y. Lee ◽  
M. D. Willis ◽  
R. M. Healy ◽  
T. B. Onasch ◽  
J. P. D. Abbatt
Keyword(s):  
Cluster Analysis ◽  
Urban Environment ◽  
Mass Spectrometer ◽  
Single Particle ◽  
Soot Particle ◽  
Organic Aerosol ◽  
Mixing State ◽  
Aerosol Mass Spectrometer ◽  
Mass Spectral ◽  
Aerosol Mass

Abstract. Understanding the impact of atmospheric black carbon (BC)-containing particles on human health and radiative forcing requires knowledge of the mixing state of BC, including the characteristics of the materials with which it is internally mixed. In this study, we examine the mixing state of refractory BC (rBC) and other aerosol components in an urban environment (downtown Toronto) utilizing the Aerodyne soot particle aerosol mass spectrometer equipped with a light scattering module (LS-SP-AMS). k-means cluster analysis was used to classify single particle mass spectra into chemically distinct groups. One resultant particle class is dominated by rBC mass spectral signals (C1+ to C5+) while the organic signals fall into a few major particle classes identified as hydrocarbon-like organic aerosol (HOA), oxygenated organic aerosol (OOA), and cooking emission organic aerosol (COA). A gradual mixing is observed with small rBC particles only thinly coated by HOA (~ 28% by mass on average), while over 90% of the HOA-rich particles did not contain detectable amounts of rBC. Most of the particles classified into other inorganic and organic particle classes were not significantly associated with rBC. The single particle results also suggest that HOA and COA emitted from anthropogenic sources were likely major contributors to organic-rich particles with vacuum aerodynamic diameter (dva) ranging from ~ 200 to 400 nm. The similar temporal profiles and mass spectral features of the organic classes identified by cluster analysis and the factors from a positive matrix factorization (PMF) analysis of the ensemble aerosol data set validate the interpretation of the PMF results.

scholarly journals Formation of secondary organic aerosol coating on black carbon particles near vehicular emissions

2017 ◽  
Vol 17 (24) ◽  
pp. 15055-15067 ◽  
Author(s):  
Alex K. Y. Lee ◽  
Chia-Li Chen ◽  
Jun Liu ◽  
Derek J. Price ◽  
Raghu Betha ◽  
...  
Keyword(s):  
Black Carbon ◽  
Mass Spectrometer ◽  
Secondary Organic Aerosol ◽  
Organic Aerosol ◽  
Vehicular Emissions ◽  
Aerosol Mass Spectrometer ◽  
Carbon Particles ◽  
Aerosol Mass ◽  
Inorganic Species ◽  
Dry Conditions

Abstract. Black carbon (BC) emitted from incomplete combustion can result in significant impacts on air quality and climate. Understanding the mixing state of ambient BC and the chemical characteristics of its associated coatings is particularly important to evaluate BC fate and environmental impacts. In this study, we investigate the formation of organic coatings on BC particles in an urban environment (Fontana, California) under hot and dry conditions using a soot-particle aerosol mass spectrometer (SP-AMS). The SP-AMS was operated in a configuration that can exclusively detect refractory BC (rBC) particles and their coatings. Using the −log(NOx ∕ NOy) ratio as a proxy for photochemical age of air masses, substantial formation of secondary organic aerosol (SOA) coatings on rBC particles was observed due to active photochemistry in the afternoon, whereas primary organic aerosol (POA) components were strongly associated with rBC from fresh vehicular emissions in the morning rush hours. There is also evidence that cooking-related organic aerosols were externally mixed from rBC. Positive matrix factorization and elemental analysis illustrate that most of the observed SOA coatings were freshly formed, providing an opportunity to examine SOA coating formation on rBCs near vehicular emissions. Approximately 7–20 wt % of secondary organic and inorganic species were estimated to be internally mixed with rBC on average, implying that rBC is unlikely the major condensation sink of SOA in this study. Comparison of our results to a co-located standard high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) measurement suggests that at least a portion of SOA materials condensed on rBC surfaces were chemically different from oxygenated organic aerosol (OOA) particles that were externally mixed with rBC, although they could both be generated from local photochemistry.

scholarly journals Spatial variation of chemical composition and sources of submicron aerosol in Zurich: factor analysis of mobile aerosol mass spectrometer data

2011 ◽  
Vol 11 (4) ◽  
pp. 12323-12365 ◽  
Author(s):  
C. Mohr ◽  
R. Richter ◽  
P. F. DeCarlo ◽  
A. S. H. Prévôt ◽  
U. Baltensperger
Keyword(s):  
Air Pollution ◽  
Chemical Composition ◽  
Spatial Variation ◽  
Mass Spectrometer ◽  
Organic Aerosol ◽  
Aerosol Mass Spectrometer ◽  
Aerosol Mass ◽  
Regional Background ◽  
Mobile Measurements ◽  
The City

Abstract. Mobile measurements of PM1 (PM with an aerodynamic diameter D<1 μm) chemical composition using a quadrupole aerosol mass spectrometer and a multi-angle absorption photometer were performed using the PSI mobile laboratory during winter 2007/2008 and December 2008 in the metropolitan area of Zurich, Switzerland. Positive matrix factorization (PMF) applied to the organic fraction of PM1 yielded 3 factors: Hydrocarbon-like organic aerosol (HOA) related to traffic emissions; organic aerosol from wood burning for domestic heating purposes (WBOA); and oxygenated organic aerosol (OOA), assigned to secondary organic aerosol formed by oxidation of volatile precursors. The spatial variation of the chemical composition of PM1 shows a uniform distribution throughout the city: for primary emissions, road traffic is important along major roads (varying between 7 and 14% of PM1 for different sites within the city), but overall, domestic wood burning is more important for the organic aerosol concentrations in Zurich during winter time (varying between 8–15% of PM1 for different sites within the city). OOA makes up the largest fraction of organic aerosol (44% on average). A new method, based on simultaneous on-road mobile and stationary background measurements and using the ratio of on-road sulfate to stationary sulfate to correct for small-scale dynamic effects, allows for the separation of PM1 emitted or produced locally and the PM1 from the regional background. It could be shown that especially during thermal inversions over the Swiss plateau, regional background concentrations contribute substantially to particulate number concentrations (60% on average) as well as to the concentrations of PM1 components (on average 60% for black carbon and HOA, over 97% for WBOA and OOA, and more than 94% for the measured inorganic components) in downtown Zurich. The results emphasize, on a scientific level, the advantage of mobile measurements for distinguishing local from regional air pollution, and on a political level, the importance of regional collaboration for mitigating air pollution issues.

scholarly journals Single particle characterization using the soot particle aerosol mass spectrometer (SP-AMS)

2014 ◽  
Vol 14 (10) ◽  
pp. 15323-15361 ◽  
Author(s):  
A. K. Y. Lee ◽  
M. D. Willis ◽  
R. M. Healy ◽  
T. B. Onasch ◽  
J. P. D. Abbatt
Keyword(s):  
Mass Spectrometer ◽  
Single Particle ◽  
Soot Particle ◽  
Organic Aerosol ◽  
Anthropogenic Sources ◽  
Mixing State ◽  
Aerosol Mass Spectrometer ◽  
Mass Spectral ◽  
Aerosol Mass ◽  
The Impact

Abstract. Understanding the impact of atmospheric black carbon (BC) containing particles on human health and radiative forcing requires knowledge of the mixing state of BC, including the characteristics of the materials with which it is internally mixed. In this study, we demonstrate for the first time the capabilities of the Aerodyne Soot-Particle Aerosol Mass Spectrometer equipped with a light scattering module (LS-SP-AMS) to examine the mixing state of refractory BC (rBC) and other aerosol components in an urban environment (downtown Toronto). K-means clustering analysis was used to classify single particle mass spectra into chemically distinct groups. One resultant cluster is dominated by rBC mass spectral signals (C1+ to C5+) while the organic signals fall into a few major clusters, identified as hydrocarbon-like organic aerosol (HOA), oxygenated organic aerosol (OOA), and cooking emission organic aerosol (COA). A nearly external mixing is observed with small BC particles only thinly coated by HOA (∼28% by mass on average), while over 90% of the HOA-rich particles did not contain detectable amounts of rBC. Most of the particles classified into other inorganic and organic clusters were not significantly associated with BC. The single particle results also suggest that HOA and COA emitted from anthropogenic sources were likely major contributors to organic-rich particles with low to mid-range aerodynamic diameter (dva). The similar temporal profiles and mass spectral features of the organic clusters and the factors from a positive matrix factorization (PMF) analysis of the ensemble aerosol dataset validate the conventional interpretation of the PMF results.

scholarly journals Spatial variation of chemical composition and sources of submicron aerosol in Zurich during wintertime using mobile aerosol mass spectrometer data

2011 ◽  
Vol 11 (15) ◽  
pp. 7465-7482 ◽  
Author(s):  
C. Mohr ◽  
R. Richter ◽  
P. F. DeCarlo ◽  
A. S. H. Prévôt ◽  
U. Baltensperger
Keyword(s):  
Air Pollution ◽  
Chemical Composition ◽  
Mass Spectrometer ◽  
Organic Aerosol ◽  
Urban Background ◽  
Aerosol Mass Spectrometer ◽  
Background Site ◽  
Aerosol Mass ◽  
Mobile Measurements ◽  
The City

Abstract. Mobile measurements of PM1 (particulate matter with an aerodynamic diameter <1 μm) chemical composition using a quadrupole aerosol mass spectrometer and a multi-angle absorption photometer were performed using the PSI mobile laboratory during winter 2007/2008 and December 2008 in the metropolitan area of Zurich, Switzerland. Positive matrix factorization (PMF) applied to the organic fraction of PM1 yielded 3 factors: Hydrocarbon-like organic aerosol (HOA) related to traffic emissions; organic aerosol from wood burning for domestic heating purposes (WBOA); and oxygenated organic aerosol (OOA), assigned to secondary organic aerosol formed by oxidation of volatile precursors. The chemical composition of PM1 was assessed for an urban background site and various sites throughout the city. The background site is dominated by secondary inorganic and organic species (57 %), BC, HOA, and WBOA account for 15 %, 6 %, and 12 %, respectively. As for the other sites, HOA is important along major roads (varying between 7 and 14 % of PM1 for different sites within the city, average all sites 8 %), domestic wood burning makes up between 8–15 % of PM1 for different sites within the city (average all sites 10.5 %). OOA makes up the largest fraction of organic aerosol (44 % on average). A new method allows for the separation and quantification of the local fraction of PM1 emitted or rapidly formed in the city, and the fraction of PM1 originating from the urban background. The method is based on simultaneous on-road mobile and stationary background measurements and the correction of small-scale meteorological effects using the ratio of on-road sulfate to stationary sulfate. Especially during thermal inversions over the Swiss plateau, urban background concentrations contribute substantially to particulate number concentrations (between 40 and 80 % depending on meteorological conditions and emissions, 60 % on average) as well as to the mass concentrations of PM1 components measured on road in downtown Zurich (between 30 and 90 %, on average 60 % for black carbon and HOA, and between 90 and 100 % for WBOA, OOA, and the measured inorganic components). The results emphasize, on a scientific level, the advantage of mobile measurements for distinguishing local from regional air pollution research, and on a political level, the importance of regional collaboration for mitigating air pollution issues.

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