scholarly journals Molecular characterization of free tropospheric aerosol collected at the Pico Mountain Observatory: a case study with a long-range transported biomass burning plume

2015 ◽  
Vol 15 (9) ◽  
pp. 5047-5068 ◽  
Author(s):  
K. Dzepina ◽  
C. Mazzoleni ◽  
P. Fialho ◽  
S. China ◽  
B. Zhang ◽  
...  
Keyword(s):  
North America ◽  
Molecular Characterization ◽  
Long Range ◽  
Biomass Burning ◽  
Elemental Carbon ◽  
Long Range Transport ◽  
Air Masses ◽  
Tropospheric Aerosol ◽  
Range Transport

Abstract. Free tropospheric aerosol was sampled at the Pico Mountain Observatory located at 2225 m above mean sea level on Pico Island of the Azores archipelago in the North Atlantic. The observatory is located ~ 3900 km east and downwind of North America, which enables studies of free tropospheric air transported over long distances. Aerosol samples collected on filters from June to October 2012 were analyzed to characterize organic carbon, elemental carbon, and inorganic ions. The average ambient concentration of aerosol was 0.9 ± 0.7 μg m−3. On average, organic aerosol components represent the largest mass fraction of the total measured aerosol (60 ± 51%), followed by sulfate (23 ± 28%), nitrate (13 ± 10%), chloride (2 ± 3%), and elemental carbon (2 ± 2%). Water-soluble organic matter (WSOM) extracted from two aerosol samples (9/24 and 9/25) collected consecutively during a pollution event were analyzed using ultrahigh-resolution electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry. Approximately 4000 molecular formulas were assigned to each of the mass spectra in the range of m/z 100–1000. The majority of the assigned molecular formulas had unsaturated structures with CHO and CHNO elemental compositions. FLEXPART retroplume analyses showed the sampled air masses were very aged (average plume age > 12 days). These aged aerosol WSOM compounds had an average O/C ratio of ~ 0.45, which is relatively low compared to O/C ratios of other aged aerosol. The increase in aerosol loading during the measurement period of 9/24 was linked to biomass burning emissions from North America by FLEXPART retroplume analysis and Moderate Resolution Imaging Spectroradiometer (MODIS) fire counts. This was confirmed with biomass burning markers detected in the WSOM and with the morphology and mixing state of particles as determined by scanning electron microscopy. The presence of markers characteristic of aqueous-phase reactions of phenolic species suggests that the aerosol collected at the Pico Mountain Observatory had undergone cloud processing before reaching the site. Finally, the air masses of 9/25 were more aged and influenced by marine emissions, as indicated by the presence of organosulfates and other species characteristic of marine aerosol. The change in the air masses for the two samples was corroborated by the changes in ethane, propane, and ozone, morphology of particles, as well as by the FLEXPART retroplume simulations. This paper presents the first detailed molecular characterization of free tropospheric aged aerosol intercepted at a lower free troposphere remote location and provides evidence of low oxygenation after long-range transport. We hypothesize this is a result of the selective removal of highly aged and polar species during long-range transport, because the aerosol underwent a combination of atmospheric processes during transport facilitating aqueous-phase removal (e.g., clouds processing) and fragmentation (e.g., photolysis) of components.

scholarly journals Molecular characterization of free tropospheric aerosol collected at the Pico Mountain Observatory: a case study with long range transported biomass burning plumes

2014 ◽  
Vol 14 (17) ◽  
pp. 24753-24810 ◽  
Author(s):  
K. Dzepina ◽  
C. Mazzoleni ◽  
P. Fialho ◽  
S. China ◽  
B. Zhang ◽  
...  
Keyword(s):  
North America ◽  
Organic Carbon ◽  
Molecular Characterization ◽  
Biomass Burning ◽  
North Atlantic ◽  
Air Masses ◽  
The North ◽  
Tropospheric Aerosol ◽  
The North Atlantic

Abstract. Free tropospheric aerosol was sampled at the Pico Mountain Observatory located at 2225 m a.m.s.l. on Pico Island of the Azores archipelago in the North Atlantic. The observatory (38°28'15'' N; 28°24'14'' W) is located ∼3900 km east and downwind of North America, which enables studies of free tropospheric air transported over long distances, mainly from North America. Aerosol samples collected on filters from June to October 2012 were analyzed to characterize organic carbon, elemental carbon and inorganic ion species. The average ambient concentration of aerosol was 0.9 μg m−3; on average organic aerosol contributes the majority of mass (57%), followed by sulfate (21%) and nitrate (17%). Filter-collected aerosol measurements were positively correlated (with an r2 ≥ 0.80) with continuous aerosol measurements of black carbon, aerosol light scattering and number concentration. Water-soluble organic carbon (WSOC) species extracted from two aerosol samples (9/24 and 9/25) collected consecutively during a pollution event were analyzed using ultrahigh-resolution Fourier transform ion cyclotron resonance mass spectrometry. FLEXPART retroplume analysis shows the sampled air masses were very aged (average plume age > 12 days). Approximately 4000 molecular formulas were assigned to each of the mass spectra in the range of m/z 100–1000. The majority of the assigned molecular formulas have unsaturated structures with CHO and CHNO elemental compositions. These aged WSOC compounds have an average O / C ratio of ∼0.45, which is relatively low compared to O / C ratios of other aged aerosol and might be the result of evaporation and increased fragmentation during long-range transport. The increase in aerosol loading during the measurement period of 9/24 was linked to biomass burning emissions from North America by FLEXPART retroplume analysis and Moderate Resolution Imaging Spectroradiometer (MODIS) fire counts. This was confirmed with biomass burning markers detected in WSOC species and with the morphology and mixing state of particles as determined by scanning electron microscopy. The presence of markers characteristic of aqueous-phase reactions of biomass burning phenolic species suggests that the aerosol collected at the Pico Mountain Observatory had undergone cloud processing before reaching the site. Finally, the air masses on 9/25 were more aged (∼15 days) and influenced by marine emissions, as indicated by organosulfates and other species characteristic for marine aerosol such as fatty acids. The change in air masses for the two samples was corroborated by the changes in ozone and the non-methane hydrocarbons ethane and propane, morphology of particles, as well as by the FLEXPART retroplume simulations. This manuscript presents the first detailed molecular characterization of free tropospheric aged aerosol intercepted at a lower free troposphere remote location in the North Atlantic.

scholarly journals Long-range transport of Siberian biomass burning emissions to North America during FIREX-AQ

2021 ◽  
pp. 118241
Author(s):  
Matthew S. Johnson ◽  
Kevin Strawbridge ◽  
K. Emma Knowland ◽  
Christoph Keller ◽  
Michael Travis
Keyword(s):  
North America ◽  
Long Range ◽  
Biomass Burning ◽  
Long Range Transport ◽  
Range Transport

scholarly journals Biomass burning events measured by lidars in EARLINET. Part II. Results and discussions

2020 ◽  
Author(s):  
Mariana Adam ◽  
Doina Nicolae ◽  
Livio Belegante ◽  
Iwona S. Stachlewska ◽  
Lucja Janicka ◽  
...  
Keyword(s):  
North America ◽  
Long Range ◽  
Biomass Burning ◽  
Long Range Transport ◽  
Depolarization Ratio ◽  
Smoke Particles ◽  
Geographical Regions ◽  
Range Transport ◽  
Ångström Exponent ◽  
Lidar Ratio

Abstract. Biomass burning events are analysed using the European Aerosol Research Lidar Network database for atmospheric profiling of aerosols by lidars. Atmospheric profiles containing forest fires layers were identified in data collected by fourteen stations during 2008–2017. The data ranged from complete data sets (particle backscatter coefficient, extinction coefficient and linear depolarization ratio) to single profiles (particle backscatter coefficient). The data analysis methodology was described in Part I (Biomass burning events measured by lidars in EARLINET. Part I. Data analysis methodology, under discussions to ACP, the EARLINET special issue). The results are analysed by means of intensive parameters in three directions: (I) common biomass burning source (fire) recorded by at least two stations, (II) long range transport of smoke particles from North America (here, we divided the events into pure North America and mixed-North America and local) smoke groups, and (III) analysis of smoke particles over four geographical regions (SE Europe, NE Europe, Central Europe and SW Europe). Five events were found for case (I), while 24 events were determined for case (II). A statistical analysis over the four geographical regions considered revealed that smoke originated from different regions. The smoke detected in the Central Europe region (Cabauw, Leipzig, and Hohenpeißenberg) was mostly brought over from North America (87 % of the fires), by long range transport. The smoke in the South West region (Barcelona, Evora, and Granada) came mostly from the Iberian Peninsula and North Africa, the long-range transport from North America accounting for only 9 % here. The smoke in the North Europe region (Belsk, Minsk, and Warsaw) originated mostly in East Europe (Ukraine and Russia), and had a 31 % contribution from smoke by long-range transport from North America. For the South East region (Athens, Bucharest, Potenza, Sofia, Thessaloniki) the origin of the smoke was mostly located in SE Europe (only 3 % from North America). Specific features for the lidar-derived intensive parameters based on smoke continental origin were determined for each region. Based on the whole dataset, the following signatures were observed: (i) the colour ratio of the lidar ratio and the backscatter Ångström exponent increase with travel time, while the extinction Ångström exponent and the colour ratio of the particle depolarization ratio decrease; (ii) an increase of the colour ratio of the particle depolarization ratio corresponds to both a decrease of the colour ratio of the lidar ratios and an increase of the extinction Ångström exponent; (iii) the measured smoke originating from all continental regions is characterized in average as aged smoke, except for a few cases; (iv) in general, the local smoke shows a smaller lidar ratio while the long range transported smoke shows a higher lidar ratio; and (v) the depolarization is smaller for long range transported smoke. A complete characterization of the smoke particles type (either fresh or aged) is presented for each of the four geographical regions versus different continental source regions.

scholarly journals Source apportionment and impact of long-range transport on carbonaceous aerosol particles in central Germany during HCCT-2010

2021 ◽  
Vol 21 (5) ◽  
pp. 3667-3684
Author(s):  
Laurent Poulain ◽  
Benjamin Fahlbusch ◽  
Gerald Spindler ◽  
Konrad Müller ◽  
Dominik van Pinxteren ◽  
...  
Keyword(s):  
Black Carbon ◽  
Long Range ◽  
Biomass Burning ◽  
Mass Concentration ◽  
Carbonaceous Aerosol ◽  
Long Range Transport ◽  
Air Masses ◽  
Central Germany ◽  
Range Transport ◽  
Local Emissions

Abstract. The identification of different sources of the carbonaceous aerosol (organics and black carbon) was investigated at a mountain forest site located in central Germany from September to October 2010 to characterize incoming air masses during the Hill Cap Cloud Thuringia 2010 (HCCT-2010) experiment. The near-PM1 chemical composition, as measured by a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), was dominated by organic aerosol (OA; 41 %) followed by sulfate (19 %) and nitrate (18 %). Source apportionment of the OA fraction was performed using the multilinear engine (ME-2) approach, resulting in the identification of the following five factors: hydrocarbon-like OA (HOA; 3 % of OA mass), biomass burning OA (BBOA; 13 %), semi-volatile-like OA (SV-OOA; 19 %), and two oxygenated OA (OOA) factors. The more oxidized OOA (MO-OOA, 28 %) was interpreted as being influenced by aged, polluted continental air masses, whereas the less oxidized OOA (LO-OOA, 37 %) was found to be more linked to aged biogenic sources. Equivalent black carbon (eBC), measured by a multi-angle absorption photometer (MAAP) represented 10 % of the total particulate matter (PM). The eBC was clearly associated with HOA, BBOA, and MO-OOA factors (all together R2=0.83). Therefore, eBC's contribution to each factor was achieved using a multi-linear regression model. More than half of the eBC (52 %) was associated with long-range transport (i.e., MO-OOA), whereas liquid fuel eBC (35 %) and biomass burning eBC (13 %) were associated with local emissions, leading to a complete apportionment of the carbonaceous aerosol. The separation between local and transported eBC was well supported by the mass size distribution of elemental carbon (EC) from Berner impactor samples. Air masses with the strongest marine influence, based on back trajectory analysis, corresponded with a low particle mass concentration (6.4–7.5 µg m−3) and organic fraction (≈30 %). However, they also had the largest contribution of primary OA (HOA ≈ 4 % and BBOA 15 %–20 %), which was associated with local emissions. Continental air masses had the highest mass concentration (11.4–12.6 µg m−3), and a larger fraction of oxygenated OA (≈45 %) indicated highly processed OA. The present results emphasize the key role played by long-range transport processes not only in the OA fraction but also in the eBC mass concentration and the importance of improving our knowledge on the identification of eBC sources.

scholarly journals Source apportionment and impact of long-range transport on carbonaceous aerosol particles in Central Germany during HCCT-2010

2020 ◽  
Author(s):  
Laurent Poulain ◽  
Benjamin Fahlbusch ◽  
Gerald Spindler ◽  
Konrad Müller ◽  
Dominik van Pinxteren ◽  
...  
Keyword(s):  
Black Carbon ◽  
Long Range ◽  
Biomass Burning ◽  
Mass Concentration ◽  
Carbonaceous Aerosol ◽  
Long Range Transport ◽  
Air Masses ◽  
Central Germany ◽  
Range Transport ◽  
Local Emissions

Abstract. The identification of different sources of the carbonaceous aerosol (organics and black carbon) was investigated at a mountain forest site located in central Germany from September to October 2010 to characterize incoming air masses during the Hill Cap Cloud Thuringia 2010 (HCCT-2010) experiment. The near-PM1 chemical composition, as measured by an Aerosol Mass Spectrometer (HR-ToF-AMS), was dominated by organics (OA, 41 %), followed by sulfate (19 %) and nitrate (18 %). Source apportionment of the OA fraction was performed using the Multilinear Engine approach (ME-2), resulting in the identification of five factors: Hydrocarbon-like OA (HOA, 3 % of OA mass), biomass burning OA (BBOA, 13 %), semi-volatile-like OA (SVOOA, 19 %), and two oxygenated OA (OOA) factors. The more-oxidized OOA (MO-OOA, 28 %) was interpreted as being influenced by aged polluted continental air masses, whereas the less-oxidized OOA (LO-OOA, 37 %) was found to be more linked to aged biogenic sources. Equivalent black carbon (eBC) measured by a multi-angle absorption photometer, MAAP, represented 10 % of the total PM. The eBC was clearly associated with the three factors HOA, BBOA, and MO-OOA (all together R2 = 0.83). Therefore, eBC's contribution to each factor was achieved using a multi-linear regression model. More than half of the eBC (52 %) was associated with long-range transport (i.e. MO-OOA), whereas liquid fuel eBC (35 %) and biomass burning eBC (13 %) were associated with local emissions leading to a complete apportionment of the carbonaceous aerosol. The separation between local and transported eBC was well supported by the mass size distribution of elemental carbon (EC) from Berner-impactor samples. Air masses with the strongest marine influence based on back trajectory analysis corresponded with a low particle mass concentration (6.4–7.5 µg m−3) and organic fraction (≈ 30 %). However, they also had the largest contribution of primary OA (HOA ≈ 4 % and BBOA 15–20 %), which was associated with local emissions. Continental air masses had the highest mass concentration (11.4–12.6 µg m−3) and a larger fraction of oxygenated OA (≈ 45 %) indicated highly processed OA. The present results emphasize the key role played by long-range transport processes not only on the OA fraction but also on the eBC mass concentration and the importance of improving our knowledge on the identification of eBC sources.

Elemental carbon deposition to Svalbard snow from Norwegian settlements and long-range transport

Tellus B ◽  
2011 ◽  
Vol 63 (3) ◽  
Author(s):  
Borgar Aamaas ◽  
Carl Egede Bøggild ◽  
Frode Stordal ◽  
Terje Berntsen ◽  
Kim Holmén ◽  
...  
Keyword(s):  
Long Range ◽  
Elemental Carbon ◽  
Carbon Deposition ◽  
Long Range Transport ◽  
Range Transport
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