The seasonal evolution of NMHCs and light alkyl nitrates at middle to high northern latitudes during TOPSE

Nicola J. Blake, Donald R. Blake, Barkley C. Sive, Aaron S. Katzenstein, Simone Meinardi, Oliver W. Wingenter, Elliot L Atlas, Frank Flocke, Brian A. Ridley, F. Sherwood Rowland

Research output: Contribution to journalArticle

42 Citations (Scopus)

Abstract

The Tropospheric Ozone Production about the Spring Equinox (TOPSE) experiment was designed to follow the role of photochemistry in the evolution of the springtime maximum of tropospheric ozone (O3) in the Northern Hemisphere (NH) at high latitudes. Determination of the composition and seasonal evolution of volatile organic carbon (VOC) species, which take part in and are good indicators for photochemical processes in the troposphere, was an important part of this study. We report measurements of a large number Of C2-C10 nonmethane hydrocarbons (NMHCs), selected C1-C2 halocarbons, and C1-C4 alkyl nitrates. These gases were quantified in whole air samples collected aboard the National Center for Atmospheric Research (NCAR) C-130 aircraft at altitudes between 30 m and 8 km. Seven TOPSE sampling trips were flown between early February and mid-May 2000 covering the region from Colorado (40°N) to Churchill (in Manitoba, Canada), Thule (in northern Greenland), and as far north as 85°N. These measurements represent the most comprehensive spatial characterization of the North American Arctic to date and revealed strong latitudinal, vertical, and temporal NMHC gradients. In the midtroposphere north of Churchill (58°N), ΣNMHCs decreased by ∼6.2 ppbC between February and May (1.6 ppbC month-1) and the magnitude of this change diminished with altitude. Over the same period, midtropospheric O3 levels increased by ∼16 ppbv (4.2 ppbv month-1). Free tropospheric NMHC decreases were consistent with removal by hydroxyl (OH) radicals at an average mixing ratio for mid-March to mid-May of 4.1 × 105 mol cm-3 . The alkyl nitrates, which are a reservoir species for tropospheric reactive odd nitrogen (NOY), revealed similar latitudinal, vertical, and temporal gradients to their parent NMHCs. Their total decreased by ∼4 pptv month -1, representing 10% or less of NOY. In conjunction with meteorological trajectory analysis, different trace gas signatures provided significant clues to the origins of individual polluted air masses. Several of these air masses were rapidly advected over the Pole from source regions in northeastern and western Europe as well as an air mass that originated over the southwestern United States/Baja California that contained unusually high levels of alkanes. In addition, episodes of low boundary layer (BL) O3 associated with low NMHC mixing ratios and trajectories from over the Arctic Ocean were frequently sampled toward the latter part of the experiment. The TOPSE data described here provide a unique picture of NH trace gas evolution from winter to summer that will be invaluable to models investigating the role that anthropogenic emissions play in high latitude O3 chemistry.

Original languageEnglish (US)
Pages (from-to)7-1
Number of pages7
JournalJournal of Geophysical Research C: Oceans
Volume108
Issue number4
StatePublished - Feb 27 2003
Externally publishedYes

Fingerprint

nonmethane hydrocarbon
Ozone
Hydrocarbons
Nitrates
ozone
nitrates
hydrocarbons
nitrate
air masses
air mass
Gases
Northern Hemisphere
mixing ratios
Air
trace gas
mixing ratio
polar regions
C-130 aircraft
trajectory
Trajectories

Keywords

  • Airborne measurements
  • Alkyl nitrates
  • Arctic troposphere
  • Methyl nitrate
  • NMHCs
  • Seasonal cycle

ASJC Scopus subject areas

  • Earth and Planetary Sciences (miscellaneous)
  • Atmospheric Science
  • Geochemistry and Petrology
  • Geophysics
  • Oceanography
  • Space and Planetary Science
  • Astronomy and Astrophysics

Cite this

Blake, N. J., Blake, D. R., Sive, B. C., Katzenstein, A. S., Meinardi, S., Wingenter, O. W., ... Rowland, F. S. (2003). The seasonal evolution of NMHCs and light alkyl nitrates at middle to high northern latitudes during TOPSE. Journal of Geophysical Research C: Oceans, 108(4), 7-1.

The seasonal evolution of NMHCs and light alkyl nitrates at middle to high northern latitudes during TOPSE. / Blake, Nicola J.; Blake, Donald R.; Sive, Barkley C.; Katzenstein, Aaron S.; Meinardi, Simone; Wingenter, Oliver W.; Atlas, Elliot L; Flocke, Frank; Ridley, Brian A.; Rowland, F. Sherwood.

In: Journal of Geophysical Research C: Oceans, Vol. 108, No. 4, 27.02.2003, p. 7-1.

Research output: Contribution to journalArticle

Blake, NJ, Blake, DR, Sive, BC, Katzenstein, AS, Meinardi, S, Wingenter, OW, Atlas, EL, Flocke, F, Ridley, BA & Rowland, FS 2003, 'The seasonal evolution of NMHCs and light alkyl nitrates at middle to high northern latitudes during TOPSE', Journal of Geophysical Research C: Oceans, vol. 108, no. 4, pp. 7-1.
Blake NJ, Blake DR, Sive BC, Katzenstein AS, Meinardi S, Wingenter OW et al. The seasonal evolution of NMHCs and light alkyl nitrates at middle to high northern latitudes during TOPSE. Journal of Geophysical Research C: Oceans. 2003 Feb 27;108(4):7-1.
Blake, Nicola J. ; Blake, Donald R. ; Sive, Barkley C. ; Katzenstein, Aaron S. ; Meinardi, Simone ; Wingenter, Oliver W. ; Atlas, Elliot L ; Flocke, Frank ; Ridley, Brian A. ; Rowland, F. Sherwood. / The seasonal evolution of NMHCs and light alkyl nitrates at middle to high northern latitudes during TOPSE. In: Journal of Geophysical Research C: Oceans. 2003 ; Vol. 108, No. 4. pp. 7-1.
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T1 - The seasonal evolution of NMHCs and light alkyl nitrates at middle to high northern latitudes during TOPSE

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AU - Blake, Donald R.

AU - Sive, Barkley C.

AU - Katzenstein, Aaron S.

AU - Meinardi, Simone

AU - Wingenter, Oliver W.

AU - Atlas, Elliot L

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AU - Rowland, F. Sherwood

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AB - The Tropospheric Ozone Production about the Spring Equinox (TOPSE) experiment was designed to follow the role of photochemistry in the evolution of the springtime maximum of tropospheric ozone (O3) in the Northern Hemisphere (NH) at high latitudes. Determination of the composition and seasonal evolution of volatile organic carbon (VOC) species, which take part in and are good indicators for photochemical processes in the troposphere, was an important part of this study. We report measurements of a large number Of C2-C10 nonmethane hydrocarbons (NMHCs), selected C1-C2 halocarbons, and C1-C4 alkyl nitrates. These gases were quantified in whole air samples collected aboard the National Center for Atmospheric Research (NCAR) C-130 aircraft at altitudes between 30 m and 8 km. Seven TOPSE sampling trips were flown between early February and mid-May 2000 covering the region from Colorado (40°N) to Churchill (in Manitoba, Canada), Thule (in northern Greenland), and as far north as 85°N. These measurements represent the most comprehensive spatial characterization of the North American Arctic to date and revealed strong latitudinal, vertical, and temporal NMHC gradients. In the midtroposphere north of Churchill (58°N), ΣNMHCs decreased by ∼6.2 ppbC between February and May (1.6 ppbC month-1) and the magnitude of this change diminished with altitude. Over the same period, midtropospheric O3 levels increased by ∼16 ppbv (4.2 ppbv month-1). Free tropospheric NMHC decreases were consistent with removal by hydroxyl (OH) radicals at an average mixing ratio for mid-March to mid-May of 4.1 × 105 mol cm-3 . The alkyl nitrates, which are a reservoir species for tropospheric reactive odd nitrogen (NOY), revealed similar latitudinal, vertical, and temporal gradients to their parent NMHCs. Their total decreased by ∼4 pptv month -1, representing 10% or less of NOY. In conjunction with meteorological trajectory analysis, different trace gas signatures provided significant clues to the origins of individual polluted air masses. Several of these air masses were rapidly advected over the Pole from source regions in northeastern and western Europe as well as an air mass that originated over the southwestern United States/Baja California that contained unusually high levels of alkanes. In addition, episodes of low boundary layer (BL) O3 associated with low NMHC mixing ratios and trajectories from over the Arctic Ocean were frequently sampled toward the latter part of the experiment. The TOPSE data described here provide a unique picture of NH trace gas evolution from winter to summer that will be invaluable to models investigating the role that anthropogenic emissions play in high latitude O3 chemistry.

KW - Airborne measurements

KW - Alkyl nitrates

KW - Arctic troposphere

KW - Methyl nitrate

KW - NMHCs

KW - Seasonal cycle

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