Identifying fire plumes in the Arctic with tropospheric FTIR measurements and transport models
Author:
Viatte C., Strong K.ORCID, Hannigan J., Nussbaumer E., Emmons L.ORCID, Conway S., Paton-Walsh C.ORCID, Hartley J., Benmergui J., Lin J.ORCID
Abstract
Abstract. 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°5' 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 five-year FTIR timeseries. Analyses of Hybrid Single Particle Lagrangian Integrated Trajectory Model (HYSPLIT) back-trajectories coupled with Moderate Resolution Imaging Spectroradiometer (MODIS) fire hot spot data, Stochastic Time-Inverted Lagrangian Transport model (STILT) 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 datasets are 0.39 ± 0.15 g kg−1 for HCN, 1.23 ± 0.49 g kg−1 for C2H6, 0.34 ± 0.16 g kg−1 for C2H2, 2.13 ± 0.92 g kg−1 for HCOOH, and 3.14 ± 1.28 g kg−1 for CH3OH. 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 highlight an underestimation of its emission. Results show that modelled 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.
Publisher
Copernicus GmbH
Reference79 articles.
1. Andreae, M. O. and Merlet, P.: Emission of trace gases and aerosols from biomass burning, Global Biogeochem. Cy., 15, 955–966, https://doi.org/10.1029/2000GB001382, 2001. 2. Akagi, S. K., Yokelson, R. J., Wiedinmyer, C., Alvarado, M. J., Reid, J. S., Karl, T., Crounse, J. D., and Wennberg, P. O.: Emission factors for open and domestic biomass burning for use in atmospheric models, Atmos. Chem. Phys., 11, 4039–4072, https://doi.org/10.5194/acp-11-4039-2011, 2011. 3. Amiro, B. D., Cantin, A., Flannigan, M. D., and de Groot, W. J.: Future emissions from Canadian boreal forest fires, Can. J. Forest Res., 39, 383–395, https://doi.org/10.1139/X08-154, 2009. 4. Barrett, C., Kelly, R., Higuera, P. E., and Hu, F. S.: Climatic and land-cover influences on the spatiotemporal dynamics of Holocene boreal fire regimes, Ecology, 94, 389–402, https://doi.org/10.1890/12-0840.1, 2013. 5. Bian, H., Colarco, P. R., Chin, M., Chen, G., Rodriguez, J. M., Liang, Q., Blake, D., Chu, D. A., da Silva, A., Darmenov, A. S., Diskin, G., Fuelberg, H. E., Huey, G., Kondo, Y., Nielsen, J. E., Pan, X., and Wisthaler, A.: Source attributions of pollution to the Western Arctic during the NASA ARCTAS field campaign, Atmos. Chem. Phys., 13, 4707–4721, https://doi.org/10.5194/acp-13-4707-2013, 2013.
|
|