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

Journal Article · · Elementa
DOI:https://doi.org/10.1525/elementa.194· OSTI ID:1425464
 [1];  [2];  [3];  [4];  [5];  [6];  [3];  [3]
  1. Michigan Technological Univ., Houghton, MI (United States). Atmospheric Sciences; National Inst. of Aerospace, Hampton, VA (United States)
  2. Michigan Technological Univ., Houghton, MI (United States). Atmospheric Sciences; Environmental Protection Agency (EPA), Research Triangle Park, NC (United States)
  3. Michigan Technological Univ., Houghton, MI (United States). Atmospheric Sciences
  4. Univ. of Colorado, Boulder, CO (United States). Inst. of Arctic and Alpine Research
  5. Univ. of Sheffield (United Kingdom). Chemical and Biological Engineering
  6. Michigan Technological Univ., Houghton, MI (United States). Atmospheric Sciences; Univ. of Birmingham (United Kingdom)
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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.

Research Organization:
Michigan Technological Univ., Houghton, MI (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Biological and Environmental Research (BER); National Science Foundation (NSF)
Grant/Contract Number:
SC0006941; ATM-0720955; AGS-1110059
OSTI ID:
1425464
Journal Information:
Elementa, Vol. 5; ISSN 2325-1026
Publisher:
University of California PressCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 13 works
Citation information provided by
Web of Science

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Cited By (2)

Molecular and physical characteristics of aerosol at a remote free troposphere site: implications for atmospheric aging journal January 2018
Ozone and carbon monoxide observations over open oceans on R/V Mirai from 67° S to 75° N during 2012 to 2017: testing global chemical reanalysis in terms of Arctic processes, low ozone levels at low latitudes, and pollution transport journal January 2019

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Related Subjects

54 ENVIRONMENTAL SCIENCES
long-range transport patterns to Azores
long-term observations of ozone and ozone precursors
non-methane hydrocarbon aging