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 ◽  
...  

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.

2015 ◽  
Vol 15 (9) ◽  
pp. 5047-5068 ◽  
Author(s):  
K. Dzepina ◽  
C. Mazzoleni ◽  
P. Fialho ◽  
S. China ◽  
B. Zhang ◽  
...  

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.


2012 ◽  
Vol 12 (4) ◽  
pp. 2077-2098 ◽  
Author(s):  
M. Parrington ◽  
P. I. Palmer ◽  
D. K. Henze ◽  
D. W. Tarasick ◽  
E. J. Hyer ◽  
...  

Abstract. We have analysed the sensitivity of the tropospheric ozone distribution over North America and the North Atlantic to boreal biomass burning emissions during the summer of 2010 using the GEOS-Chem 3-D global tropospheric chemical transport model and observations from in situ and satellite instruments. We show that the model ozone distribution is consistent with observations from the Pico Mountain Observatory in the Azores, ozonesondes across Canada, and the Tropospheric Emission Spectrometer (TES) and Infrared Atmospheric Sounding Instrument (IASI) satellite instruments. Mean biases between the model and observed ozone mixing ratio in the free troposphere were less than 10 ppbv. We used the adjoint of GEOS-Chem to show the model ozone distribution in the free troposphere over Maritime Canada is largely sensitive to NOx emissions from biomass burning sources in Central Canada, lightning sources in the central US, and anthropogenic sources in the eastern US and south-eastern Canada. We also used the adjoint of GEOS-Chem to evaluate the Fire Locating And Monitoring of Burning Emissions (FLAMBE) inventory through assimilation of CO observations from the Measurements Of Pollution In The Troposphere (MOPITT) satellite instrument. The CO inversion showed that, on average, the FLAMBE emissions needed to be reduced to 89% of their original values, with scaling factors ranging from 12% to 102%, to fit the MOPITT observations in the boreal regions. Applying the CO scaling factors to all species emitted from boreal biomass burning sources led to a decrease of the model tropospheric distributions of CO, PAN, and NOx by as much as −20 ppbv, −50 pptv, and −20 pptv respectively. The modification of the biomass burning emission estimates reduced the model ozone distribution by approximately −3 ppbv (−8%) and on average improved the agreement of the model ozone distribution compared to the observations throughout the free troposphere, reducing the mean model bias from 5.5 to 4.0 ppbv for the Pico Mountain Observatory, 3.0 to 0.9 ppbv for ozonesondes, 2.0 to 0.9 ppbv for TES, and 2.8 to 1.4 ppbv for IASI.


2011 ◽  
Vol 11 (9) ◽  
pp. 25099-25153 ◽  
Author(s):  
M. Parrington ◽  
P. I. Palmer ◽  
D. K. Henze ◽  
D. W. Tarasick ◽  
E. J. Hyer ◽  
...  

Abstract. We analyse the tropospheric ozone distribution over North America and the North Atlantic to boreal biomass burning emissions during the summer of 2010 using the GEOS-Chem 3-D global tropospheric chemical transport model, and observations from in situ and satellite instruments. In comparison to observations from the PICO-NARE observatory in the Azores, ozonesondes across Canada, and the Tropospheric Emission Spectrometer (TES) and Infrared Atmospheric Sounding Instrument (IASI) satellite instruments, the model ozone distribution is shown to be in reasonable agreement with mean biases less than 10 ppbv. We use the adjoint of GEOS-Chem to show the model ozone distribution in the free troposphere over Maritime Canada is largely sensitive to NOx emissions from biomass burning sources in Central Canada, lightning sources in the central US, and anthropogenic sources in eastern US and south-eastern Canada. We also use the adjoint of GEOS-Chem to evaluate the Fire Locating And Monitoring of Burning Emissions (FLAMBE) inventory through assimilation of CO observations from the Measurements Of Pollution In The Troposphere (MOPITT) satellite instrument. The CO inversion showed that, on average the FLAMBE emissions needed to be reduced to 89 % of their original values, with scaling factors ranging from 12 % to 102 %, to fit the MOPITT observations in the boreal regions. Applying the CO scaling factors to all species emitted from boreal biomass burning sources led to a decrease of the model tropospheric distributions of CO, PAN, and NOx by as much as −20 ppbv, −50 ppbv, and −20 ppbv respectively. The impact of optimizing the biomass burning emissions was to reduce the model ozone distribution by approximately −3 ppbv (−8 %) and on average improved the agreement of the model ozone distribution compared to the observations throughout the free troposphere reducing the mean model bias from 5.5 to 4.0 ppbv for the PICO-NARE observatory, 3.0 to 0.9 ppbv for ozonesondes, 2.0 to 0.9 ppbv for TES, and 2.8 to 1.4 ppbv for IASI.


1945 ◽  
Vol 49 (410) ◽  
pp. 51-54
Author(s):  
A. Gouge

A Study of the air routes of the world brings out almost at once the fact that some of the most difficult route are also the most attractive. For instance, the North Atlantic route which couples North America with Europe is certainly one of the most difficult in the world, but also by the fact that it couples two of the most densely populated, as well as the most wealthy groups of people in the world, one of the most attractive.


Author(s):  
Peter S. Wells ◽  
Naoise Mac Sweeney

Iron Age Europe, once studied as a relatively closed, coherent continent, is being seen increasingly as a dynamic part of the much larger, interconnected world. Interactions, direct and indirect, with communities in Asia, Africa, and, by the end of the first millennium AD, North America, had significant effects on the peoples of Iron Age Europe. In the Near East and Egypt, and much later in the North Atlantic, the interactions can be linked directly to historically documented peoples and their rulers, while in temperate Europe the evidence is exclusively archaeological until the very end of the prehistoric Iron Age. The evidence attests to often long-distance interactions and their effects in regard to the movement of peoples, and the introduction into Europe of raw materials, crafted objects, styles, motifs, and cultural practices, as well as the ideas that accompanied them.


2019 ◽  
Vol 19 (10) ◽  
pp. 6621-6636 ◽  
Author(s):  
Thorsten Kaluza ◽  
Daniel Kunkel ◽  
Peter Hoor

Abstract. The evolution of the tropopause inversion layer (TIL) during cyclogenesis in the North Atlantic storm track is investigated using operational meteorological analysis data (Integrated Forecast System from the European Centre for Medium-Range Weather Forecasts). For this a total of 130 cyclones have been analysed during the months August through October between 2010 and 2014 over the North Atlantic. Their paths of migration along with associated flow features in the upper troposphere and lower stratosphere (UTLS) have been tracked based on the mean sea level pressure field. Subsets of the 130 cyclones have been used for composite analysis using minimum sea level pressure to filter the cyclones based on their strength. The composite structure of the TIL strength distribution in connection with the overall UTLS flow strongly resembles the structure of the individual cyclones. Key results are that a strong dipole in TIL strength forms in regions of cyclonic wrap-up of UTLS air masses of different origin and isentropic potential vorticity. These air masses are associated with the cyclonic rotation of the underlying cyclones. The maximum values of enhanced static stability above the tropopause occur north and northeast of the cyclone centre, vertically aligned with outflow regions of strong updraft and cloud formation up to the tropopause, which are situated in anticyclonic flow patterns in the upper troposphere. These regions are co-located with a maximum of vertical shear of the horizontal wind. The strong wind shear within the TIL results in a local minimum of Richardson numbers, representing the possibility for turbulent instability and potential mixing (or air mass exchange) within regions of enhanced static stability in the lowermost stratosphere.


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