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Titel |
Identifying fire plumes in the Arctic with tropospheric FTIR measurements and transport models |
VerfasserIn |
C. Viatte, K. Strong, J. Hannigan, E. Nussbaumer, L. K. Emmons, S. Conway, C. Paton-Walsh, J. Hartley, J. Benmergui, J. Lin |
Medientyp |
Artikel
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Sprache |
Englisch
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ISSN |
1680-7316
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Digitales Dokument |
URL |
Erschienen |
In: Atmospheric Chemistry and Physics ; 15, no. 5 ; Nr. 15, no. 5 (2015-03-02), S.2227-2246 |
Datensatznummer |
250119481
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Publikation (Nr.) |
copernicus.org/acp-15-2227-2015.pdf |
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Zusammenfassung |
We investigate Arctic tropospheric composition using ground-based Fourier
transform infrared (FTIR) solar absorption spectra, recorded at the Polar
Environment Atmospheric Research Laboratory (PEARL, Eureka, Nunavut, Canada,
80°05' N, 86°42' W) and at Thule
(Greenland, 76°53' N, −68°74' W) from
2008 to 2012. The target species, carbon monoxide (CO), hydrogen cyanide
(HCN), ethane (C2H6), acetylene (C2H2), formic acid
(HCOOH), and formaldehyde (H2CO) are emitted by biomass burning and can
be transported from mid-latitudes to the Arctic.
By detecting simultaneous enhancements of three biomass burning tracers (HCN,
CO, and C2H6), ten and eight fire events are identified at Eureka
and Thule, respectively, within the 5-year FTIR time series. Analyses of
Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model
back-trajectories coupled with Moderate Resolution Imaging Spectroradiometer
(MODIS) fire hotspot data, Stochastic Time-Inverted Lagrangian Transport
(STILT) model footprints, and Ozone Monitoring Instrument (OMI) UV aerosol
index maps, are used to attribute burning source regions and travel time
durations of the plumes. By taking into account the effect of aging of the
smoke plumes, measured FTIR enhancement ratios were corrected to obtain
emission ratios and equivalent emission factors. The means of emission
factors for extratropical forest estimated with the two FTIR data sets are
0.40 ± 0.21 g kg−1 for HCN, 1.24 ± 0.71 g kg−1 for
C2H6, 0.34 ± 0.21 g kg−1 for C2H2, and
2.92 ± 1.30 g kg−1 for HCOOH. The emission factor for CH3OH
estimated at Eureka is 3.44 ± 1.68 g kg−1.
To improve our knowledge concerning the dynamical and chemical processes
associated with Arctic pollution from fires, the two sets of FTIR
measurements were compared to the Model for OZone And Related chemical Tracers, version 4
(MOZART-4). Seasonal cycles and day-to-day variabilities were compared to
assess the ability of the model to reproduce emissions from fires and their
transport. Good agreement in winter confirms that transport is well
implemented in the model. For C2H6, however, the lower wintertime
concentration estimated by the model as compared to the FTIR observations
highlights an underestimation of its emission. Results show that modeled and
measured total columns are correlated (linear correlation coefficient
r > 0.6 for all gases except for H2CO at Eureka and HCOOH at
Thule), but suggest a general underestimation of the concentrations in the
model for all seven tropospheric species in the high Arctic. |
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