scholarly journals The 2005 Study of Organic Aerosols at Riverside (SOAR-1): instrumental intercomparisons and fine particle composition

2011 ◽  
Vol 11 (23) ◽  
pp. 12387-12420 ◽  
Author(s):  
K. S. Docherty ◽  
A. C. Aiken ◽  
J. A. Huffman ◽  
I. M. Ulbrich ◽  
P. F. DeCarlo ◽  
...  
Keyword(s):  
Gas Phase ◽  
Fine Particles ◽  
Organic Aerosols ◽  
Diurnal Cycles ◽  
Aerosol Mass ◽  
High Volatility ◽  
Multiple State ◽  
Highly Correlated ◽  
Primary Emissions ◽  
A Minor

Abstract. Multiple state-of-the-art instruments sampled ambient aerosol in Riverside, California during the 2005 Study of Organic Aerosols at Riverside (SOAR) to investigate the chemical composition and potential sources of fine particles (PMf) in the inland region of Southern California. In this paper, we briefly summarize the spatial, meteorological and gas-phase conditions during SOAR-1 (15 July–15 August), provide detailed intercomparisons of high-resolution aerosol mass spectrometer (HR-AMS) measurements against complementary measurements, and report the average composition of PMf including the composition of the organic fraction measured by the HR-AMS. Daily meteorology and gas-phase species concentrations were highly consistent, displaying clear diurnal cycles and weekday/weekend contrast. HR-AMS measurements of non-refractory submicron (NR-PM1) mass are consistent and highly correlated with those from a filter dynamics measurement system tapered-element oscillating microbalance (TEOM), while the correlation between HR-AMS and heated TEOM measurements is lower due to loss of high volatility species including ammonium nitrate from the heated TEOM. Speciated HR-AMS measurements are also consistent with complementary measurements as well as with measurements from a collocated compact AMS while HR-AMS OC is similar to standard semi-continuous Sunset measurements within the combined uncertainties of both instruments. A correction intended to account for the loss of semi-volatile OC from the Sunset, however, yields measurements ~30% higher than either HR-AMS or standard Sunset measurements. On average, organic aerosol (OA) was the single largest component of PMf. OA composition was investigated using both elemental analysis and positive matrix factorization (PMF) of HR-AMS OA spectra. Oxygen is the main heteroatom during SOAR-1, with O/C exhibiting a diurnal minimum of 0.28 during the morning rush hour and maximum of 0.42 during the afternoon. O/C is broadly anti-correlated with H/C, while N/C and S/C (excluding organonitrate (ON) and organosulfate (OS) functionalities) are far lower than O/C at about 0.015 and ~0.001, respectively. When ON and OS estimates are included O/C, N/C, and S/C increase by factors of 1.21, 2, and 30, respectively, while H/C changes are insignificant. The increase in these ratios implies that ON accounts for ~1/2 of the organic nitrogen while OS dominate organic sulfur at this location. Accounting for the estimated ON and OS also improves the agreement between anions and cations measured by HR-AMS by ~8%, while amines have only a very small impact (1%) on this balance. Finally, a number of primary and secondary OA components were resolved by PMF. Among these a hydrocarbon-like OA and two minor, local OA components, one of which was associated with amines, were attributed to primary emissions and contributed a minor fraction (~20%) of OA mass. The remaining OA mass was attributed to a number of secondary oxidized OA (OOA) components including the previously-identified low-volatility and semi-volatile OOA components. In addition, we also report for the first time the presence of two additional OOA components.

scholarly journals The 2005 Study of Organic Aerosols at Riverside (SOAR-1): instrumental intercomparisons and fine particle composition

2011 ◽  
Vol 11 (2) ◽  
pp. 6301-6362 ◽  
Author(s):  
K. S. Docherty ◽  
A. C. Aiken ◽  
J. A. Huffman ◽  
I. M. Ulbrich ◽  
P. F. DeCarlo ◽  
...  
Keyword(s):  
Gas Phase ◽  
Fine Particles ◽  
Organic Aerosols ◽  
Organic Aerosol ◽  
Aerosol Mass Spectrometer ◽  
Diurnal Cycles ◽  
Aerosol Mass ◽  
Multiple State ◽  
Anions And Cations ◽  
Highly Correlated

Abstract. Multiple state-of-the-art instruments sampled ambient aerosol in Riverside, California during the 2005 Study of Organic Aerosols at Riverside (SOAR) to investigate sources and chemical composition of fine particles (PMf) in the inland region of Southern California. This paper briefly summarizes the spatial, meteorological and gas-phase conditions during SOAR-1 (15 July–15 August) and provides detailed intercomparisons of complementary measurements and average PMf composition during this period. Daily meteorology and gas-phase species concentrations were highly repetitive with meteorological and gas-phase species concentrations displaying clear diurnal cycles and weekday/weekend contrast, with organic aerosol (OA) being the single largest component contributing approximately one-third of PMf mass. In contrast with historical characterizations of OA in the region, several independent source apportionment efforts attributed the vast majority (~80%) of OA mass during SOAR-1 to secondary organic aerosol (SOA). Given the collocation of complementary aerosol measurements combined with a dominance of SOA during SOAR-1, this paper presents new results on intercomparisons among several complementary measurements and on PMf composition during this period. Total non-refractory submicron (NR-PM1) measurements from a high-resolution aerosol mass spectrometer (HR-AMS) are compared with measurements by tapered element oscillating microbalances (TEOM) including a filter dynamics measurement system (TEOMFDMS). NR-PM1 is highly correlated with PM2.5 TEOMFDMS measurements and accounts for the bulk of PM2.5 mass with the remainder contributed primarily by refractory material. In contrast, measurements from a heated TEOM show substantial losses of semi-volatile material, including ammonium nitrate and semi-volatile organic material. Speciated HR-AMS measurements are also consistent and highly correlated with several complementary measurements, including those of a collocated compact AMS (C-AMS). Finally, elemental analysis (EA) of HR-AMS OA spectra allows direct comparison of HR-AMS organic carbon (OC) with measurements from two collocated Sunset thermal-optical semi-continuous monitors, and investigation of the elemental composition of OA in Riverside. While HR-AMS and base OC measurements from both Sunset instruments are similar within the combined uncertainties, a correction intended to account for the loss of semivolatile OC from the Sunset yields OC measurements ~30% higher than either HR-AMS or base Sunset measurements. Oxygen is the main heteroatom of ambient OA during SOAR-1 with a minimum atomic O/C of 0.28 during the morning rush hour and maximum of 0.42 during the afternoon. H/C is broadly anti-correlated with O/C, while N/C and S/C (excluding organonitrate (ON) and organosulfate (OS) functionalities) are far lower than O/C at about 0.015 and ~0.001, respectively. O/C, N/C, and S/C increase by 21%, a factor of 2, and a factor of 30, respectively, while H/C changes little when ON and OS estimates are included. This implies that ON account for ~1/2 of the organic nitrogen while OS dominate organic sulfur at this location. Accounting for the estimated ON and OS also improves the agreement between anions and cations measured by HR-AMS by ~8%, while amines have a very small impact (1%) on this balance.

scholarly journals Mexico City aerosol analysis during MILAGRO using high resolution aerosol mass spectrometry at the urban supersite (T0) – Part 1: Fine particle composition and organic source apportionment

2009 ◽  
Vol 9 (2) ◽  
pp. 8377-8427 ◽  
Author(s):  
A. C. Aiken ◽  
D. Salcedo ◽  
M. J. Cubison ◽  
J. A. Huffman ◽  
P. F. DeCarlo ◽  
...  
Keyword(s):  
High Resolution ◽  
Mexico City ◽  
Biomass Burning ◽  
Emissions Inventory ◽  
Secondary Sources ◽  
Diurnal Cycles ◽  
Aerosol Mass ◽  
Aerosol Mass Spectrometry ◽  
Order Of Magnitude ◽  
Primary Emissions

Abstract. Submicron aerosol was analyzed during the MILAGRO field campaign in March 2006 at the T0 urban supersite in Mexico City with a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and complementary instrumentation. Mass concentrations, diurnal cycles, and size distributions of inorganic and organic species are similar to results from the CENICA supersite in April 2003 with organic aerosol (OA) comprising about half of the fine PM mass. Positive Matrix Factorization (PMF) analysis of the high resolution OA spectra identified three major components: chemically-reduced urban primary emissions (hydrocarbon-like OA, HOA), oxygenated OA (OOA, mostly secondary OA or SOA), and biomass burning OA (BBOA) that correlates with levoglucosan and acetonitrile. BBOA includes several very large plumes from regional fires and likely also some refuse burning. A fourth OA component is a small local nitrogen-containing reduced OA component (LOA) which accounts for 9% of the OA mass but one third of the organic nitrogen, likely as amines. OOA accounts for almost half of the OA on average, consistent with previous observations. OA apportionment results from PMF-AMS are compared to the PM2.5 chemical mass balance of organic molecular markers (CMB-OMM, from GC/MS analysis of filters). Results from both methods are overall consistent. Both assign the major components of OA to primary urban, biomass burning/woodsmoke, and secondary sources at similar magnitudes. The 2006 Mexico City emissions inventory underestimates the urban primary PM2.5 emissions by a factor of ~4, and it is ~16 times lower than afternoon concentrations when secondary species are included. Additionally, the forest fire contribution is underestimated by at least an order-of-magnitude in the inventory.

scholarly journals Secondary organic aerosol formation from photooxidation of naphthalene and alkylnaphthalenes: implications for oxidation of intermediate volatility organic compounds (IVOCs)

2009 ◽  
Vol 9 (9) ◽  
pp. 3049-3060 ◽  
Author(s):  
A. W. H. Chan ◽  
K. E. Kautzman ◽  
P. S. Chhabra ◽  
J. D. Surratt ◽  
M. N. Chan ◽  
...  
Keyword(s):  
Gas Phase ◽  
Secondary Organic Aerosol ◽  
Organic Aerosol ◽  
Diesel Emissions ◽  
Aerosol Formation ◽  
Gas Phase Reactions ◽  
Large Source ◽  
Aerosol Mass ◽  
Polycyclic Aromatic ◽  
Primary Emissions

Abstract. Current atmospheric models do not include secondary organic aerosol (SOA) production from gas-phase reactions of polycyclic aromatic hydrocarbons (PAHs). Recent studies have shown that primary emissions undergo oxidation in the gas phase, leading to SOA formation. This opens the possibility that low-volatility gas-phase precursors are a potentially large source of SOA. In this work, SOA formation from gas-phase photooxidation of naphthalene, 1-methylnaphthalene (1-MN), 2-methylnaphthalene (2-MN), and 1,2-dimethylnaphthalene (1,2-DMN) is studied in the Caltech dual 28-m3 chambers. Under high-NOx conditions and aerosol mass loadings between 10 and 40 μg m−3, the SOA yields (mass of SOA per mass of hydrocarbon reacted) ranged from 0.19 to 0.30 for naphthalene, 0.19 to 0.39 for 1-MN, 0.26 to 0.45 for 2-MN, and constant at 0.31 for 1,2-DMN. Under low-NOx conditions, the SOA yields were measured to be 0.73, 0.68, and 0.58, for naphthalene, 1-MN, and 2-MN, respectively. The SOA was observed to be semivolatile under high-NOx conditions and essentially nonvolatile under low-NOx conditions, owing to the higher fraction of ring-retaining products formed under low-NOx conditions. When applying these measured yields to estimate SOA formation from primary emissions of diesel engines and wood burning, PAHs are estimated to yield 3–5 times more SOA than light aromatic compounds over photooxidation timescales of less than 12 h. PAHs can also account for up to 54% of the total SOA from oxidation of diesel emissions, representing a potentially large source of urban SOA.

scholarly journals Why do organic aerosols exist? Understanding aerosol lifetimes using the two-dimensional volatility basis set

2013 ◽  
Vol 10 (3) ◽  
pp. 151 ◽  
Author(s):  
N. M. Donahue ◽  
W. Chuang ◽  
S. A. Epstein ◽  
J. H. Kroll ◽  
D. R. Worsnop ◽  
...  
Keyword(s):  
Human Health ◽  
Gas Phase ◽  
Fine Particles ◽  
Critical Role ◽  
Organic Aerosols ◽  
Basis Set ◽  
Oh Radicals ◽  
Phase Oxidation ◽  
Gas Phase Oxidation ◽  
Oxidation Chemistry

Environmental context Fine particles (aerosols) containing organic compounds are central players in two important environmental issues: aerosol-climate effects and human health effects (including mortality). Although organics constitute half or more of the total fine-particle mass, their chemistry is extremely complex; of critical importance is ongoing oxidation chemistry in both the gas phase and the particle phase. Here we present a method for representing that oxidation chemistry when the actual composition of the organics is not known and show that relatively slow oxidant uptake to particles plays a key role in the very existence of organic aerosols. Abstract Organic aerosols play a critical role in atmospheric chemistry, human health and climate. Their behaviour is complex. They consist of thousands of organic molecules in a rich, possibly highly viscous mixture that may or may not be in phase equilibrium with organic vapours. Because the aerosol is a mixture, compounds from all sources interact and thus influence each other. Finally, most ambient organic aerosols are highly oxidised, so the molecules are secondary products formed from primary emissions by oxidation chemistry and possibly non-oxidative association reactions in multiple phases, including gas-phase oxidation, aqueous oxidation, condensed (organic) phase reactions and heterogeneous interactions of all these phases. In spite of this complexity, we can make a strong existential statement about organic aerosol: They exist throughout the troposphere because heterogeneous oxidation by OH radicals is more than an order of magnitude slower than comparable gas-phase oxidation.

scholarly journals Mexico City aerosol analysis during MILAGRO using high resolution aerosol mass spectrometry at the urban supersite (T0) – Part 1: Fine particle composition and organic source apportionment

2009 ◽  
Vol 9 (17) ◽  
pp. 6633-6653 ◽  
Author(s):  
A. C. Aiken ◽  
D. Salcedo ◽  
M. J. Cubison ◽  
J. A. Huffman ◽  
P. F. DeCarlo ◽  
...  
Keyword(s):  
High Resolution ◽  
Mexico City ◽  
Biomass Burning ◽  
Emissions Inventory ◽  
Secondary Sources ◽  
Diurnal Cycles ◽  
Aerosol Mass ◽  
Aerosol Mass Spectrometry ◽  
Order Of Magnitude ◽  
Primary Emissions

Abstract. Submicron aerosol was analyzed during the MILAGRO field campaign in March 2006 at the T0 urban supersite in Mexico City with a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and complementary instrumentation. Mass concentrations, diurnal cycles, and size distributions of inorganic and organic species are similar to results from the CENICA supersite in April 2003 with organic aerosol (OA) comprising about half of the fine PM mass. Positive Matrix Factorization (PMF) analysis of the high resolution OA spectra identified three major components: chemically-reduced urban primary emissions (hydrocarbon-like OA, HOA), oxygenated OA (OOA, mostly secondary OA or SOA), and biomass burning OA (BBOA) that correlates with levoglucosan and acetonitrile. BBOA includes several very large plumes from regional fires and likely also some refuse burning. A fourth OA component is a small local nitrogen-containing reduced OA component (LOA) which accounts for 9% of the OA mass but one third of the organic nitrogen, likely as amines. OOA accounts for almost half of the OA on average, consistent with previous observations. OA apportionment results from PMF-AMS are compared to the PM2.5 chemical mass balance of organic molecular markers (CMB-OMM, from GC/MS analysis of filters). Results from both methods are overall consistent. Both assign the major components of OA to primary urban, biomass burning/woodsmoke, and secondary sources at similar magnitudes. The 2006 Mexico City emissions inventory underestimates the urban primary PM2.5 emissions by a factor of ~4, and it is ~16 times lower than afternoon concentrations when secondary species are included. Additionally, the forest fire contribution is at least an order-of-magnitude larger than in the inventory.

scholarly journals Aerosol chemical and optical properties over the Paris area within ESQUIF project

2006 ◽  
Vol 6 (11) ◽  
pp. 3257-3280 ◽  
Author(s):  
A. Hodzic ◽  
R. Vautard ◽  
P. Chazette ◽  
L. Menut ◽  
B. Bessagnet
Keyword(s):  
Optical Properties ◽  
Secondary Organic Aerosols ◽  
Organic Aerosols ◽  
Dust Particles ◽  
Aerosol Size Distribution ◽  
Aerosol Composition ◽  
Aerosol Mass ◽  
Coarse Mode ◽  
Paris Area ◽  
Flight Trajectories

Abstract. Aerosol chemical and optical properties are extensively investigated for the first time over the Paris Basin in July 2000 within the ESQUIF project. The measurement campaign offers an exceptional framework to evaluate the performances of the chemistry-transport model CHIMERE in simulating concentrations of gaseous and aerosol pollutants, as well as the aerosol-size distribution and composition in polluted urban environments against ground-based and airborne measurements. A detailed comparison of measured and simulated variables during the second half of July with particular focus on 19 and 31 pollution episodes reveals an overall good agreement for gas-species and aerosol components both at the ground level and along flight trajectories, and the absence of systematic biases in simulated meteorological variables such as wind speed, relative humidity and boundary layer height as computed by the MM5 model. A good consistency in ozone and NO concentrations demonstrates the ability of the model to reproduce the plume structure and location fairly well both on 19 and 31 July, despite an underestimation of the amplitude of ozone concentrations on 31 July. The spatial and vertical aerosol distributions are also examined by comparing simulated and observed lidar vertical profiles along flight trajectories on 31 July and confirm the model capacity to simulate the plume characteristics. The comparison of observed and modeled aerosol components in the southwest suburb of Paris during the second half of July indicates that the aerosol composition is rather correctly reproduced, although the total aerosol mass is underestimated by about 20%. The simulated Parisian aerosol is dominated by primary particulate matter that accounts for anthropogenic and biogenic primary particles (40%), and inorganic aerosol fraction (40%) including nitrate (8%), sulfate (22%) and ammonium (10%). The secondary organic aerosols (SOA) represent 12% of the total aerosol mass, while the mineral dust accounts for 8%. The comparison demonstrates the absence of systematic errors in the simulated sulfate, ammonium and nitrates total concentrations. However, for nitrates the observed partition between fine and coarse mode is not reproduced. In CHIMERE there is a clear lack of coarse-mode nitrates. This calls for additional parameterizations in order to account for the heterogeneous formation of nitrate onto dust particles. Larger discrepancies are obtained for the secondary organic aerosols due to both inconsistencies in the SOA formation processes in the model leading to an underestimation of their mass and large uncertainties in the determination of the measured aerosol organic fraction. The observed mass distribution of aerosols is not well reproduced, although no clear explanation can be given.

Synthesis of Sic Fine Particles by Gas-Phase Reaction Under Short-Time Microgravity

1992 ◽  
Vol 286 ◽  
Author(s):  
Takeshi Okutani ◽  
Yoshinori Nakata ◽  
Masaakt Suzuki ◽  
Yves Maniette ◽  
Nobuyoshi Goto ◽  
...  
Keyword(s):  
Thermal Decomposition ◽  
Heat Source ◽  
Size Distribution ◽  
Gas Phase ◽  
Fine Particles ◽  
Rapid Heating ◽  
Exothermic Reaction ◽  
Phase Reaction ◽  
Gas Phase Reaction ◽  
Short Time

ABSTRACTSiC fine particles were synthesized by the gas-phase thermal decomposition of tetramethylsilane (Si(CH3)4) in hydrogen under microgravity of 10−4G for 10 sec. Rapid heating to the temperature over 800°C which is required for thermal decomposition of Si(CH3)4) under short-time microgravity was attained using a chemical oven where the heat of exothermic reaction of combustion synthesis of Ti-A1-4B composites was used as the heat source. Monodisperse and spherical SiC fine particles were synthesized under microgravity, whereas aggregates of SiC fine particles were synthesized under 1 G gravity. The SiC particles synthesized under microgravity (150-200 nm) were bigger in size and narrower in size distribution than those under 1 G gravity (100-150 nm).

scholarly journals Seasonal characteristics of fine particulate matter (PM) based on high-resolution time-of-flight aerosol mass spectrometric (HR-ToF-AMS) measurements at the HKUST Supersite in Hong Kong

2015 ◽  
Vol 15 (1) ◽  
pp. 37-53 ◽  
Author(s):  
Y. J. Li ◽  
B. P. Lee ◽  
L. Su ◽  
J. C. H. Fung ◽  
C.K. Chan
Keyword(s):  
Hong Kong ◽  
Organic Aerosols ◽  
Organic Aerosol ◽  
Resolution Time ◽  
Time Resolved ◽  
Air Mass ◽  
Aerosol Mass ◽  
Seasonal Characteristics ◽  
Autumn And Winter ◽  
Air Mass Origin

Abstract. Atmospheric particulate matter (PM) remains poorly understood due to the lack of comprehensive measurements at high time resolution for tracking its dynamic features and the lack of long-term observation for tracking its seasonal variability. Here, we present highly time-resolved and seasonal compositions and characteristics of non-refractory components in PM with a diameter less than 1 μm (NR-PM1) at a suburban site in Hong Kong. The measurements were made with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) at the Hong Kong University of Science and Technology (HKUST) Air Quality Research Supersite for 4 months, with one in each season of the year. The average NR-PM1 concentration of ~ 15 μg m−3 is higher than those AMS measurements made in South Korea and Japan, but lower than those in North China, the Yangtze River Delta and the nearby Pearl River Delta. The seasonal dependence of the total NR-PM1 monthly averaged concentrations was small, but that of the fractions of the species in NR-PM1 was significant. Site characteristic plays an important role in the relative fractions of species in NR-PM1 and our results are generally consistent with measurements at other non-urban sites in this regard. Detailed analyses were conducted on the AMS data in the aspects of (1) species concentrations, (2) size distributions, (3) degree of oxygenation of organics, and (4) positive matrix factorization (PMF)-resolved organic factors in a seasonal context, as well as with air mass origin from back-trajectory analysis. Sulfate had the highest fraction in NR-PM1 (> 40%), and the surrogates of secondary organic species – semi-volatile oxygenated organic aerosol (SVOOA) and low-volatility oxygenated organic aerosol (LVOOA) – prevailed (~ 80%) in the organic portion of NR-PM1. Local contributions to the organic portion of NR-PM1 at this suburban site was strongly dependent on season. The hydrocarbon-like organic aerosol (HOA) factor related to local traffic emissions contributed > 10% to organic aerosols in spring and summer but only 6–7% in autumn and winter. The cooking organic aerosol (COA) factor contributed > 10% to organic aerosols in winter. With the aid of highly time-resolved data, diurnal patterns of the degree of oxygenation of organic aerosols were used to determine the sources and formation processes of the least understood organic portion of PM. The oxygen-to-carbon atomic ratio (O : C) and average carbon oxidation state OS C) showed little variation in autumn and winter, when the long-range transport of oxidized organics dominated, whereas they peaked in the afternoon in spring and summer, when locally produced secondary organic aerosol prevailed. Air mass origin, in contrast, had a strong influence on both NR-PM1 concentrations and the fractions of species in NR-PM1. The findings of the current study provide a better understanding of the role of air mass origin in the seasonal characteristics of the PM composition and the relative importance of local vs. transported organic aerosols in this region.

scholarly journals Towards a better understanding of the origins, chemical composition and aging of oxygenated organic aerosols: case study of a Mediterranean industrialized environment, Marseille

2013 ◽  
Vol 13 (15) ◽  
pp. 7875-7894 ◽  
Author(s):  
I. El Haddad ◽  
B. D'Anna ◽  
B. Temime-Roussel ◽  
M. Nicolas ◽  
A. Boreave ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Organic Aerosols ◽  
Industrial Emissions ◽  
Aerosol Mass Spectrometer ◽  
Statistical Confidence ◽  
Aerosol Mass ◽  
Novel Approach ◽  
Organic Markers ◽  
The Impact ◽  
First Time

Abstract. As part of the FORMES summer 2008 experiment, an Aerodyne compact time-of-flight aerosol mass spectrometer (cToF-AMS) was deployed at an urban background site in Marseille to investigate the sources and aging of organic aerosols (OA). France's second largest city and the largest port in the Mediterranean, Marseille, provides a locale that is influenced by significant urban industrialized emissions and an active photochemistry with very high ozone concentrations. Particle mass spectra were analyzed by positive matrix factorization (PMF2) and the results were in very good agreement with previous apportionments obtained using a chemical mass balance (CMB) approach coupled to organic markers and metals (El Haddad et al., 2011a). AMS/PMF2 was able to identify for the first time, to the best of our knowledge, the organic aerosol emitted by industrial processes. Even with significant industries in the region, industrial OA was estimated to contribute only ~ 5% of the total OA mass. Both source apportionment techniques suggest that oxygenated OA (OOA) constitutes the major fraction, contributing ~ 80% of OA mass. A novel approach combining AMS/PMF2 data with 14C measurements was applied to identify and quantify the fossil and non-fossil precursors of this fraction and to explicitly assess the related uncertainties. Results show with high statistical confidence that, despite extensive urban and industrial emissions, OOA is overwhelmingly non-fossil, formed via the oxidation of biogenic precursors, including monoterpenes. AMS/PMF2 results strongly suggest that the variability observed in the OOA chemical composition is mainly driven in our case by the aerosol photochemical age. This paper presents the impact of photochemistry on the increase of OOA oxygenation levels, formation of humic-like substances (HULIS) and the evolution of α-pinene SOA (secondary OA) components.

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