scholarly journals Chemical characterization of long-range transport biomass burning emissions to the Himalayas: insights from high-resolution aerosol mass spectrometry

2017 ◽  
Author(s):  
Xinghua Zhang ◽  
Jianzhong Xu ◽  
Shichang Kang ◽  
Yanmei Liu ◽  
Qi Zhang
Keyword(s):  
High Resolution ◽  
Long Range ◽  
Biomass Burning ◽  
Monsoon Season ◽  
Chemical Characterization ◽  
Time Resolved ◽  
Entire Study ◽  
Aerosol Mass ◽  
Remote Sites ◽  
Average Size

Abstract. An intensive measurement was conducted at a remote, background, and high-altitude site (Qomolangma station, QOMS, 4276 m a.s.l.) in the northern Himalayas, using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) along with other collocated instruments. The field measurement was performed from April 12 to May 12, 2016 to chemically characterize the high time-resolved submicron particulate matter (PM1) and obtain the dynamic processes (emissions, transport, and chemical processing) of biomass burning (BB), frequently transported from South Asia to the Himalayas during pre-monsoon season. Overall, the average (±1σ) PM1 mass concentration was 4.44 (±4.54) µg m−3 for the entire study, comparable with those observed at other remote sites worldwide. Organic aerosol (OA) was the dominant PM1 species (accounting for 54.3 % of total PM1 on average) followed by black carbon (BC) (25.0 %), sulfate (9.3 %), ammonium (5.8 %), nitrate (5.1 %), and chloride (0.4 %). The average size distributions of PM1 species all peaked at an overlapping accumulation mode (~ 500 nm), suggesting that aerosol particles were internally well-mixed and aged during long-range transportation. Positive matrix factorization (PMF) analysis on the high-resolution organic mass spectra identified three distinct OA factors, including a BB-related OA (BBOA, 43.7 %), a nitrogen-containing OA (NOA, 13.9 %) and a more-oxidized oxygenated OA (MO-OOA, 42.4 %). Two polluted episodes with enhanced PM1 mass loadings and elevated BBOA contributions from the west and southwest of QOMS during the study were observed. A typical BB plume was investigated in detail to illustrate the chemical evolution of aerosol, air mass origins, meteorological conditions and atmospheric oxidation processes.

scholarly journals Chemical characterization of long-range transport biomass burning emissions to the Himalayas: insights from high-resolution aerosol mass spectrometry

2018 ◽  
Vol 18 (7) ◽  
pp. 4617-4638 ◽  
Author(s):  
Xinghua Zhang ◽  
Jianzhong Xu ◽  
Shichang Kang ◽  
Yanmei Liu ◽  
Qi Zhang
Keyword(s):  
High Resolution ◽  
Long Range ◽  
Chemical Evolution ◽  
Biomass Burning ◽  
Field Measurement ◽  
Monsoon Season ◽  
Long Range Transport ◽  
Entire Study ◽  
Aerosol Mass ◽  
Range Transport

Abstract. An intensive field measurement was conducted at a remote, background, high-altitude site (Qomolangma Station, QOMS, 4276 m a.s.l.) in the northern Himalayas, using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) along with other collocated instruments. The field measurement was performed from 12 April to 12 May 2016 to chemically characterize the high time-resolved submicron particulate matter (PM1) and obtain the dynamic processes (emissions, transport, and chemical evolution) of biomass burning (BB), frequently transported from South Asia to the Himalayas during pre-monsoon season. Overall, the average (±1σ) PM1 mass concentration was 4.44 (±4.54) µg m−3 for the entire study, which is comparable with those observed at other remote sites worldwide. Organic aerosol (OA) was the dominant PM1 species (accounting for 54.3 % of total PM1 on average) followed by black carbon (BC) (25.0 %), sulfate (9.3 %), ammonium (5.8 %), nitrate (5.1 %), and chloride (0.4 %). The average size distributions of PM1 species all peaked at an overlapping accumulation mode (∼ 500 nm), suggesting that aerosol particles were internally well-mixed and aged during long-range transport. Positive matrix factorization (PMF) analysis on the high-resolution organic mass spectra identified three distinct OA factors, including a BB-related OA (BBOA, 43.7 %), a nitrogen-containing OA (NOA, 13.9 %) and a more-oxidized oxygenated OA (MO-OOA, 42.4 %). Two polluted episodes with enhanced PM1 mass loadings and elevated BBOA contributions from the west and southwest of QOMS during the study were observed. A typical BB plume was investigated in detail to illustrate the chemical evolution of aerosol characteristics under distinct air mass origins, meteorological conditions, and atmospheric oxidation processes.

scholarly journals Chemical characterization and sources of submicron aerosols in the northeastern Qinghai-Tibet Plateau: insights from high-resolution mass spectrometry

2019 ◽  
Author(s):  
Xinghua Zhang ◽  
Jianzhong Xu ◽  
Shichang Kang ◽  
Qi Zhang
Keyword(s):  
High Resolution ◽  
Long Range ◽  
Biomass Burning ◽  
Tibet Plateau ◽  
Source Analysis ◽  
Long Range Transport ◽  
Aerosol Mass ◽  
Range Transport ◽  
Qinghai Tibet Plateau ◽  
Mass Concentrations

Abstract. An Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed along with other online instruments to study the highly time-resolved chemistry and sources of submicron aerosols (PM1) at Waliguan (WLG) Baseline Observatory, a high-altitude (3816 m a.s.l.) background station located at the northeastern edge of Qinghai-Tibet Plateau (QTP), during 1–31 July 2017. The average PM1 mass concentration during this study was 9.1 μg m−3 (ranging from 0.3 to 28.1 μg m−3), which was distinct higher than those (2.0–5.7 μg m−3) measured with Aerodyne AMS at other high-elevation sites in the southern or central QTP. Sulfate showed dominant contribution (38.1 %) to PM1 at WLG following by organics (34.5 %), ammonium (15.2 %), nitrate (8.1 %), BC (3.0 %) and chloride (1.1 %). Accordingly, bulk aerosols appeared to be slightly acidic throughout this study mainly related to the enhanced sulfate contribution. All chemical species peaked at the accumulation mode, indicating the well mixed and highly aged aerosol particles at WLG from long-range transport. Positive matrix factorization (PMF) on the high-resolution organic mass spectra resolved four distinct organic aerosol (OA) components, including a traffic-related hydrocarbon-like OA (HOA), a relatively fresh biomass burning OA (BBOA), an aged biomass burning OA (agBBOA) and a more-oxidized oxygenated OA (OOA). On average, the two relatively oxidized OAs, OOA and agBBOA, contributed 34.4 % and 40.4 % of organics, respectively, while the rest were 18.4 % for BBOA and 6.8 % for HOA. Source analysis for air masses displayed higher mass concentrations of PM1 and enhanced contributions of sulfate and biomass burning related OA components (agBBOA + BBOA) were from northeast of the WLG with shorter transport distance, whereas lower PM1 mass concentrations with enhanced OOA contribution were from west after long-range transport, suggesting their distinct aerosol sources and significant impacts of regional transport to aerosol mass loadings and chemistry at WLG.

scholarly journals Chemical characterization and sources of submicron aerosols in the northeastern Qinghai–Tibet Plateau: insights from high-resolution mass spectrometry

2019 ◽  
Vol 19 (11) ◽  
pp. 7897-7911 ◽  
Author(s):  
Xinghua Zhang ◽  
Jianzhong Xu ◽  
Shichang Kang ◽  
Qi Zhang ◽  
Junying Sun
Keyword(s):  
High Resolution ◽  
Long Range ◽  
Biomass Burning ◽  
Tibet Plateau ◽  
Source Analysis ◽  
Long Range Transport ◽  
Aerosol Mass ◽  
Range Transport ◽  
Qinghai Tibet Plateau ◽  
Mass Concentrations

Abstract. An Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed along with other online instruments to study the highly time resolved chemistry and sources of submicron aerosols (PM1) at Waliguan (WLG) Baseline Observatory, a high-altitude (3816 m a.s.l.) background station located at the northeast edge of the Qinghai–Tibet Plateau (QTP), during 1–31 July 2017. The average PM1 mass concentration during this study was 9.1 µg m−3 (ranging from 0.3 to 28.1 µg m−3), which was distinctly higher than those (2.0–5.7 µg m−3) measured with the Aerodyne AMS at other high-elevation sites in the southern or central QTP. Sulfate showed a dominant contribution (38.1 %) to PM1 at WLG followed by organics (34.5 %), ammonium (15.2 %), nitrate (8.1 %), BC (3.0 %) and chloride (1.1 %). Accordingly, bulk aerosols appeared to be slightly acidic throughout this study, mainly related to the enhanced sulfate contribution. All chemical species peaked at the accumulation mode, indicating the well-mixed and highly aged aerosol particles at WLG from long-range transport. Positive matrix factorization (PMF) on the high-resolution organic mass spectra resolved four distinct organic aerosol (OA) components, including a traffic-related hydrocarbon-like OA (HOA), a relatively fresh biomass burning OA (BBOA), an aged biomass burning OA (agBBOA) and a more-oxidized oxygenated OA (OOA). On average, the two relatively oxidized OAs, OOA and agBBOA, contributed 34.4 % and 40.4 % of organics, respectively, while the rest were 18.4 % for BBOA and 6.8 % for HOA. Source analysis for air masses showed that higher mass concentrations of PM1 and enhanced contributions of sulfate and biomass-burning-related OA components (agBBOA + BBOA) were from the northeast of the WLG with shorter transport distance, whereas lower PM1 mass concentrations with enhanced OOA contribution were from the west after long-range transport, suggesting their distinct aerosol sources and significant impacts of regional transport on aerosol mass loadings and chemistry at WLG.

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 Size-resolved aerosol chemistry on Whistler Mountain, Canada with a high-resolution aerosol mass spectrometer during INTEX-B

2009 ◽  
Vol 9 (9) ◽  
pp. 3095-3111 ◽  
Author(s):  
Y. Sun ◽  
Q. Zhang ◽  
A. M. Macdonald ◽  
K. Hayden ◽  
S. M. Li ◽  
...  
Keyword(s):  
High Resolution ◽  
Mass Spectrometer ◽  
High Elevation ◽  
Average Concentration ◽  
Size Distributions ◽  
Mineral Contents ◽  
Entire Study ◽  
Aerosol Mass Spectrometer ◽  
Aerosol Mass ◽  
Dust Events

Abstract. An Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed at the peak of Whistler Mountain (2182 m above sea level), British Columbia, from 19 April to 16 May 2006, as part of the Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign. The mass concentrations and size distributions of non-refractory submicron particle (NR-PM1) species (i.e., sulfate, nitrate, ammonium, chloride, and organics) were measured in situ at 10-min time resolution. The HR-ToF-AMS results agreed well with collocated measurements. The average concentration of non-refractory submicron particulate matter (NR-PM1; 1.9 μg m−3) is similar to those observed at other remote, high elevation sites in North America. Episodes of enhanced aerosol loadings were observed, due to influences of regional and trans-Pacific transport of air pollution. Organics and sulfate were the dominant species, on average accounting for 55% and 30%, respectively, of the NR-PM1 mass. The average size distributions of sulfate and ammonium both showed an accumulation mode peaking at ~500 nm in vacuum aerodynamic diameter (Dva) while those of organic aerosol (OA) and nitrate peaked at ~300 nm. The size differences suggested that sulfate and OA were mostly present in external mixtures from different source origins. We also quantitatively determined the elemental composition of OA using the high resolution mass spectra. Overall, OA at Whistler Peak was highly oxygenated, with an average organic-mass-to-organic-carbon ratio (OM/OC) of 2.28±0.23 and an atomic ratio of oxygen-to-carbon (O/C) of 0.83±0.17. The nominal formula for OA was C1H1.66N0.03O0.83 for the entire study. Two significant trans-Pacific dust events originated from Asia were observed at Whistler Peak during this study. While both events were characterized with significant enhancements of coarse mode particles and mineral contents, the composition and characteristics of NR-PM1 were significantly different between them. One trans-Pacific event occurred on 15 May 2006, during which ammonium sulfate contributed >90% of the total NR-PM1 mass. This event was followed by a high OA episode likely associated with regional emissions. In total, three enhanced regional OA events, each of which lasted 2–3 days, were observed during this study. In contrast to the two dust events, the regional OA events were generally characterized with higher OA/sulfate ratio, less oxidized OA, and lower OM/OC ratio.

scholarly journals Sources and chemical characterization of organic aerosol during the summer in the eastern Mediterranean

2015 ◽  
Vol 15 (3) ◽  
pp. 3455-3491 ◽  
Author(s):  
E. Kostenidou ◽  
K. Florou ◽  
C. Kaltsonoudis ◽  
M. Tsiflikiotou ◽  
S. Vratolis ◽  
...  
Keyword(s):  
High Resolution ◽  
Eastern Mediterranean ◽  
Fine Particulate Matter ◽  
Chemical Characterization ◽  
Organic Aerosol ◽  
Atomic Ratio ◽  
Photochemical Activity ◽  
Average Mass ◽  
Pollution Levels ◽  
Aerosol Mass

Abstract. The concentration and chemical composition of the non-refractory fine particulate matter (NR-PM1) and black carbon (BC) levels were measured during the summer of 2012 in the suburbs of two Greek cities, Patras and Athens, in an effort to better understand the chemical processing of particles in the high photochemical activity environment of the Eastern Mediterranean. The composition of PM1 was surprisingly similar in both areas demonstrating the importance of regional sources for the corresponding pollution levels. The PM1 average mass concentration was 9–14 μg m−3. The contribution of sulphate was around 38%, while organic aerosol (OA) contributed approximately 45% in both cases. PM1 nitrate levels were low (2%). The oxygen to carbon (O : C) atomic ratio was 0.50 ± 0.08 in Patras and 0.47 ± 0.11 in Athens. In both cases the PM1 was acidic. Positive matrix factorization (PMF) was applied to the high resolution organic aerosol mass spectra obtained by an Aerodyne High Resolution Aerosol Mass Spectrometer (HR-AMS). For Patras five OA sources could be identified: 19% very oxygenated OA (V-OOA), 38% moderately oxygenated OA (M-OOA), 21% biogenic oxygenated OA (b-OOA), 7% hydrocarbon-like OA (HOA-1) associated with traffic sources and 15% hydrocarbon-like OA (HOA-2) related to other primary emissions (including cooking OA). For Athens the corresponding source contributions were: V-OOA (35%), M-OOA (30%), HOA-1 (18%) and HOA-2 (17%). In both cities the major component was OOA, suggesting that under high photochemical conditions most of the OA in the Eastern Mediterranean is quite aged. The contribution of the primary sources (HOA-1 and HOA-2) was important (22% in Patras and 33% in Athens) but not dominant.

scholarly journals Online Chemical Characterization and Source Identification of Summer and Winter Aerosols in Măgurele, Romania

Atmosphere ◽  
2020 ◽  
Vol 11 (4) ◽  
pp. 385 ◽  
Author(s):  
Luminiţa Mărmureanu ◽  
Jeni Vasilescu ◽  
Jay Slowik ◽  
André S. H. Prévôt ◽  
Cristina Antonia Marin ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Winter Season ◽  
Organic Aerosols ◽  
Chemical Characterization ◽  
Primary Source ◽  
Total Carbon ◽  
Absorption Data ◽  
Aerosol Mass ◽  
Total Proportion ◽  
Using Data

Aerosols and organic source apportionment were characterized using data collected during two measurement campaigns. These campaigns were conducted during the summer and winter seasons at Măgurele, a site located southwest of Bucharest, the capital of Romania and one of the largest cities in southeastern Europe (raking seven in Europe based on population). The summer campaign was conducted between 7 June–18 July 2012, and the winter campaign from 14 January–6 February 2013. Approximately 50% of the organic fraction contribution to the total submicron particulate matter sampled by aerosol mass spectrometer was evidenced during both seasons. Submicronic organic aerosol sources were quantified using the positive matrix factorization approach. For warm (summer) and cold (winter) seasons, more than 50% from total organics was represented by oxidized factors. For the summer season, separate analyses were conducted on data influenced by urban and non-urban sources. The influence of pollution from Bucharest on the measurement site was observed in aerosol concentration and composition. The primary organic aerosols have different contribution percentage during summer, depending on their main origin. The influence of Bucharest, during summer, included cooking contribution of 13%. The periods with more regional influence were characterized by lower contribution from traffic and biomass burning in a total proportion of 28%. In winter, the influence of local non-traffic sources was dominant. For more than 99% of the measurements, the biomass burning indicator, f 60 , exceeded the background value, with residential heating being an important source in this area. Fossil fuel contribution was confirmed for one week during the winter campaign, when 14 C analysis of total and elemental carbon revealed the presence of 17% fossil contributions to total carbon. Mass spectrometry, 14 C and absorption data suggest biomass burning as the predominant primary source of organic aerosols for the winter season.

scholarly journals Long-term chemical characterization of tropical and marine aerosols at the Cape Verde Atmospheric Observatory (CVAO) from 2007 to 2011

2014 ◽  
Vol 14 (17) ◽  
pp. 8883-8904 ◽  
Author(s):  
K. W. Fomba ◽  
K. Müller ◽  
D. van Pinxteren ◽  
L. Poulain ◽  
M. van Pinxteren ◽  
...  
Keyword(s):  
Long Range ◽  
Mineral Dust ◽  
Chemical Characterization ◽  
Sea Salt ◽  
Saharan Dust ◽  
Long Range Transport ◽  
Air Mass ◽  
Aerosol Mass ◽  
Range Transport

Abstract. The first long-term aerosol sampling and chemical characterization results from measurements at the Cape Verde Atmospheric Observatory (CVAO) on the island of São Vicente are presented and are discussed with respect to air mass origin and seasonal trends. In total 671 samples were collected using a high-volume PM10 sampler on quartz fiber filters from January 2007 to December 2011. The samples were analyzed for their aerosol chemical composition, including their ionic and organic constituents. Back trajectory analyses showed that the aerosol at CVAO was strongly influenced by emissions from Europe and Africa, with the latter often responsible for high mineral dust loading. Sea salt and mineral dust dominated the aerosol mass and made up in total about 80% of the aerosol mass. The 5-year PM10 mean was 47.1 ± 55.5 μg m−2, while the mineral dust and sea salt means were 27.9 ± 48.7 and 11.1 ± 5.5 μg m−2, respectively. Non-sea-salt (nss) sulfate made up 62% of the total sulfate and originated from both long-range transport from Africa or Europe and marine sources. Strong seasonal variation was observed for the aerosol components. While nitrate showed no clear seasonal variation with an annual mean of 1.1 ± 0.6 μg m−3, the aerosol mass, OC (organic carbon) and EC (elemental carbon), showed strong winter maxima due to strong influence of African air mass inflow. Additionally during summer, elevated concentrations of OM were observed originating from marine emissions. A summer maximum was observed for non-sea-salt sulfate and was connected to periods when air mass inflow was predominantly of marine origin, indicating that marine biogenic emissions were a significant source. Ammonium showed a distinct maximum in spring and coincided with ocean surface water chlorophyll a concentrations. Good correlations were also observed between nss-sulfate and oxalate during the summer and winter seasons, indicating a likely photochemical in-cloud processing of the marine and anthropogenic precursors of these species. High temporal variability was observed in both chloride and bromide depletion, differing significantly within the seasons, air mass history and Saharan dust concentration. Chloride (bromide) depletion varied from 8.8 ± 8.5% (62 ± 42%) in Saharan-dust-dominated air mass to 30 \\textpm 12% (87 ± 11%) in polluted Europe air masses. During summer, bromide depletion often reached 100% in marine as well as in polluted continental samples. In addition to the influence of the aerosol acidic components, photochemistry was one of the main drivers of halogenide depletion during the summer; while during dust events, displacement reaction with nitric acid was found to be the dominant mechanism. Positive matrix factorization (PMF) analysis identified three major aerosol sources: sea salt, aged sea salt and long-range transport. The ionic budget was dominated by the first two of these factors, while the long-range transport factor could only account for about 14% of the total observed ionic mass.

scholarly journals Mexico city aerosol analysis during MILAGRO using high resolution aerosol mass spectrometry at the urban supersite (T0) – Part 2: Analysis of the biomass burning contribution and the non-fossil carbon fraction

2010 ◽  
Vol 10 (12) ◽  
pp. 5315-5341 ◽  
Author(s):  
A. C. Aiken ◽  
B. de Foy ◽  
C. Wiedinmyer ◽  
P. F. DeCarlo ◽  
I. M. Ulbrich ◽  
...  
Keyword(s):  
High Resolution ◽  
Mexico City ◽  
Biomass Burning ◽  
Forest Fires ◽  
Organic Aerosol ◽  
Total Carbon ◽  
Fire Emissions ◽  
Fossil Carbon ◽  
Aerosol Mass ◽  
The Impact

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 Aerosol Mass Spectrometer (AMS) and complementary instrumentation. Positive Matrix Factorization (PMF) of high resolution AMS spectra identified a biomass burning organic aerosol (BBOA) component, which includes several large plumes that appear to be from forest fires within the region. Here, we show that the AMS BBOA concentration at T0 correlates with fire counts in the vicinity of Mexico City and that most of the BBOA variability is captured when the FLEXPART model is used for the dispersion of fire emissions as estimated from satellite fire counts. The resulting FLEXPART fire impact factor (FIF) correlates well with the observed BBOA, acetonitrile (CH3CN), levoglucosan, and potassium, indicating that wildfires in the region surrounding Mexico City are the dominant source of BBOA at T0 during MILAGRO. The impact of distant BB sources such as the Yucatan is small during this period. All fire tracers are correlated, with BBOA and levoglucosan showing little background, acetonitrile having a well-known tropospheric background of ~100–150 pptv, and PM2.5 potassium having a background of ~160 ng m−3 (two-thirds of its average concentration), which does not appear to be related to BB sources. We define two high fire periods based on satellite fire counts and FLEXPART-predicted FIFs. We then compare these periods with a low fire period when the impact of regional fires is about a factor of 5 smaller. Fire tracers are very elevated in the high fire periods whereas tracers of urban pollution do not change between these periods. Dust is also elevated during the high BB period but this appears to be coincidental due to the drier conditions and not driven by direct dust emission from the fires. The AMS oxygenated organic aerosol (OA) factor (OOA, mostly secondary OA or SOA) does not show an increase during the fire periods or a correlation with fire counts, FLEXPART-predicted FIFs or fire tracers, indicating that it is dominated by urban and/or regional sources and not by the fires near the MCMA. A new 14C aerosol dataset is presented. Both this new and a previously published dataset of 14C analysis suggest a similar BBOA contribution as the AMS and chemical mass balance (CMB), resulting in 13% higher non-fossil carbon during the high vs. low regional fire periods. The new dataset has ~15% more fossil carbon on average than the previously published one, and possible reasons for this discrepancy are discussed. During the low regional fire period, 38% of organic carbon (OC) and 28% total carbon (TC) are from non-fossil sources, suggesting the importance of urban and regional non-fossil carbon sources other than the fires, such as food cooking and regional biogenic SOA. The ambient BBOA/ΔCH3CN ratio is much higher in the afternoon when the wildfires are most intense than during the rest of the day. Also, there are large differences in the contributions of the different OA components to the surface concentrations vs. the integrated column amounts. Both facts may explain some apparent disagreements between BB impacts estimated from afternoon aircraft flights vs. those from 24-h ground measurements. We show that by properly accounting for the non-BB sources of K, all of the BB PM estimates from MILAGRO can be reconciled. Overall, the fires from the region near the MCMA are estimated to contribute 15–23% of the OA and 7–9% of the fine PM at T0 during MILAGRO, and 2–3% of the fine PM as an annual average. The 2006 MCMA emissions inventory contains a substantially lower impact of the forest fire emissions, although a fraction of these emissions occur just outside of the MCMA inventory area.

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