Ten-year chemical signatures associated with long-range transport observed in the free troposphere over the central North Atlantic

Ten-year observations of trace gases at Pico Mountain Observatory (PMO), a free troposphere site in the central North Atlantic, were classified by transport patterns using the Lagrangian particle dispersion model, FLEXPART. The classification enabled identifying trace gas mixing ratios associated wi...

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Main Authors: B. Zhang, R. C. Owen, J. A. Perlinger, D. Helmig, M. Val Martín, L. Kramer, L. R. Mazzoleni, C. Mazzoleni
Format: Article
Language:English
Published: BioOne 2017-03-01
Series:Elementa: Science of the Anthropocene
Subjects:
Online Access:https://www.elementascience.org/articles/194
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author B. Zhang
R. C. Owen
J. A. Perlinger
D. Helmig
M. Val Martín
L. Kramer
L. R. Mazzoleni
C. Mazzoleni
author_facet B. Zhang
R. C. Owen
J. A. Perlinger
D. Helmig
M. Val Martín
L. Kramer
L. R. Mazzoleni
C. Mazzoleni
author_sort B. Zhang
collection DOAJ
description Ten-year observations of trace gases at Pico Mountain Observatory (PMO), a free troposphere site in the central North Atlantic, were classified by transport patterns using the Lagrangian particle dispersion model, FLEXPART. The classification enabled identifying trace gas mixing ratios associated with background air and long- range transport of continental emissions, which were defined as chemical signatures. Comparison between the chemical signatures revealed the impacts of natural and anthropogenic sources, as well as chemical and physical processes during long transport, on air composition in the remote North Atlantic. Transport of North American anthropogenic emissions (NA-Anthro) and summertime wildfire plumes (Fire) significantly enhanced CO and O3 at PMO. Summertime CO enhancements caused by NA-Anthro were found to have been decreasing by a rate of 0.67 ± 0.60 ppbv/year in the ten-year period, due possibly to reduction of emissions in North America. Downward mixing from the upper troposphere and stratosphere due to the persistent Azores-Bermuda anticyclone causes enhanced O3 and nitrogen oxides. The 'd' [O3]/'d' [CO] value was used to investigate O3 sources and chemistry in different transport patterns. The transport pattern affected by Fire had the lowest 'd' [O3]/'d' [CO], which was likely due to intense CO production and depressed O3 production in wildfire plumes. Slightly enhanced O3 and 'd' [O3]/'d' [CO] were found in the background air, suggesting that weak downward mixing from the upper troposphere is common at PMO. Enhancements of both butane isomers were found during upslope flow periods, indicating contributions from local sources. The consistent ratio of butane isomers associated with the background air and NA-anthro implies no clear difference in the oxidation rates of the butane isomers during long transport. Based on observed relationships between non-methane hydrocarbons, the averaged photochemical age of the air masses at PMO was estimated to be 11 ± 4 days.
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spelling doaj.art-865005d01d0446d8833a0ee075072da72022-12-21T17:57:35ZengBioOneElementa: Science of the Anthropocene2325-10262017-03-01510.1525/elementa.194148Ten-year chemical signatures associated with long-range transport observed in the free troposphere over the central North AtlanticB. Zhang0R. C. Owen1J. A. Perlinger2D. Helmig3M. Val Martín4L. Kramer5L. R. Mazzoleni6C. Mazzoleni7Atmospheric Sciences, Michigan Technological University, Houghton; and National Institute of Aerospace, HamptonAtmospheric Sciences, Michigan Technological University, Houghton; and Environmental Protection Agency, Research Triangle ParkAtmospheric Sciences, Michigan Technological University, HoughtonInstitute of Arctic and Alpine Research, University of Colorado, BoulderChemical and Biological Engineering, University of Sheffield, SheffieldAtmospheric Sciences, Michigan Technological University, Houghton, United States; and University of Birmingham, BirminghamAtmospheric Sciences, Michigan Technological University, HoughtonAtmospheric Sciences, Michigan Technological University, HoughtonTen-year observations of trace gases at Pico Mountain Observatory (PMO), a free troposphere site in the central North Atlantic, were classified by transport patterns using the Lagrangian particle dispersion model, FLEXPART. The classification enabled identifying trace gas mixing ratios associated with background air and long- range transport of continental emissions, which were defined as chemical signatures. Comparison between the chemical signatures revealed the impacts of natural and anthropogenic sources, as well as chemical and physical processes during long transport, on air composition in the remote North Atlantic. Transport of North American anthropogenic emissions (NA-Anthro) and summertime wildfire plumes (Fire) significantly enhanced CO and O3 at PMO. Summertime CO enhancements caused by NA-Anthro were found to have been decreasing by a rate of 0.67 ± 0.60 ppbv/year in the ten-year period, due possibly to reduction of emissions in North America. Downward mixing from the upper troposphere and stratosphere due to the persistent Azores-Bermuda anticyclone causes enhanced O3 and nitrogen oxides. The 'd' [O3]/'d' [CO] value was used to investigate O3 sources and chemistry in different transport patterns. The transport pattern affected by Fire had the lowest 'd' [O3]/'d' [CO], which was likely due to intense CO production and depressed O3 production in wildfire plumes. Slightly enhanced O3 and 'd' [O3]/'d' [CO] were found in the background air, suggesting that weak downward mixing from the upper troposphere is common at PMO. Enhancements of both butane isomers were found during upslope flow periods, indicating contributions from local sources. The consistent ratio of butane isomers associated with the background air and NA-anthro implies no clear difference in the oxidation rates of the butane isomers during long transport. Based on observed relationships between non-methane hydrocarbons, the averaged photochemical age of the air masses at PMO was estimated to be 11 ± 4 days.https://www.elementascience.org/articles/194Long-range transport patterns to AzoresLong-term observations of ozone and ozone precursorsNon-methane hydrocarbon aging
spellingShingle B. Zhang
R. C. Owen
J. A. Perlinger
D. Helmig
M. Val Martín
L. Kramer
L. R. Mazzoleni
C. Mazzoleni
Ten-year chemical signatures associated with long-range transport observed in the free troposphere over the central North Atlantic
Elementa: Science of the Anthropocene
Long-range transport patterns to Azores
Long-term observations of ozone and ozone precursors
Non-methane hydrocarbon aging
title Ten-year chemical signatures associated with long-range transport observed in the free troposphere over the central North Atlantic
title_full Ten-year chemical signatures associated with long-range transport observed in the free troposphere over the central North Atlantic
title_fullStr Ten-year chemical signatures associated with long-range transport observed in the free troposphere over the central North Atlantic
title_full_unstemmed Ten-year chemical signatures associated with long-range transport observed in the free troposphere over the central North Atlantic
title_short Ten-year chemical signatures associated with long-range transport observed in the free troposphere over the central North Atlantic
title_sort ten year chemical signatures associated with long range transport observed in the free troposphere over the central north atlantic
topic Long-range transport patterns to Azores
Long-term observations of ozone and ozone precursors
Non-methane hydrocarbon aging
url https://www.elementascience.org/articles/194
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