Source contributions to Northern Hemisphere CO and black carbon during spring and summer 2008 from POLARCAT and START08/preHIPPO observations and MOZART-4 S. Tilmes1, L. K. Emmons1, K. S. Law2, G. Ancellet2, H. Schlager3, J.-D. Paris4, H. E. Fuelberg5, D. G. Streets6, C. Wiedinmyer1, G. S. Diskin7, Y. Kondo8, J. Holloway9,10, J. P. Schwarz9,10, J. R. Spackman9,10, T. Campos1, P. Nédélec11, and M. V. Panchenko12 1National Center for Atmospheric Research, Boulder, Colorado, USA 2LATMOS-IPSL; UPMC Univ. Paris 06; Univ. Versailles St-Quentin; CNRS/INSU, Paris, France 3Institute for Physics of the Atmosphere, Oberpfaffenhofen, Wessling, Germany 4Laboratoire des Sciences du Climat et de l'Environnement/IPSL, CNRS-CEA-UVSQ, Orme des Merisiers, CEA Saclay, Gif sur Yvette, France 5Florida State University, USA 6Argonne National Laboratory, DIS/221 9700 South Cass Avenue Argonne, Illinois 60439, USA 7NASA Langley Research Center, Hampton, Virginia, USA 8Research Center for Advanced Science and Technology, The University of Tokyo 4-6-1 Komaba, Meguro, Tokyo 153-8904, Japan 9NOAA Earth System Research Laboratory, Boulder, CO, USA 10Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado, Boulder, USA 11Laboratoire d'Aérologie, CNRS-UPS, Toulouse, France 12Institute of Atmospheric Optics, SB-RAS, Tomsk, Russia
Received: 24 January 2011 – Accepted: 07 February 2011 – Published: 21 February 2011
Abstract. Anthropogenic pollution and wildfires are main producers of carbon monoxide (CO)
and black carbon (BC) in the Northern Hemisphere. High concentrations of these compounds are
transported into the Arctic troposphere, influencing the ecosystem in high northern
latitudes and the global
climate. The global chemical transport model MOZART-4 is used to quantify the
seasonal evolution of the contribution of CO and BC from different source regions in spring and
summer 2008 by tagging their emissions. Aircraft observations from the POLARCAT
experiments, in particular NASA ARCTAS, NOAA ARCPAC, POLARCAT-France, DLR GRACE and
YAK-AEROSIB, as well as the NSF START08/preHIPPO experiments during Spring-Summer 2008 are combined
to quantify the representation of simulated tracer characteristics in anthropogenic and fire plumes.
In general, the model reproduces CO and BC well. Based on aircraft measurements and FLEXPART back-trajectories, the altitude
contribution of emissions coming from different source regions is well captured in the model.
Uncertainties of the MOZART-4 model are identified by comparing the data with
model results on the flight tracks and using MOPITT satellite observations.
Anthropogenic emissions are underestimated by about 10% in high
northern latitudes in spring, and shortcomings exist in simulating fire plumes.
The remote impact of East-Siberian fire emissions is underestimated for spring, whereas
the impact of Southeast Asian fire emissions to mid-latitude CO values is overestimated by the model.
In summer, mid-latitude CO values agree well between model and observations, whereas summer high latitude
East-Siberian fire emissions in the model are overestimated by 20% in comparison to observations in the
region. On the other hand, CO concentrations are underestimated by about 30% over Alaska and Canada
at altitudes above 4 km. BC values are overestimated by the model at altitudes above 4 km in summer.
Based on MOZART-4, with tagged CO and BC tracers, anthropogenic emissions of Asia, Europe
and the US have the largest contribution to the CO and BC in mid- and high latitudes in spring and summer.
Southeast Asian, Chinese and Indian fires have a large impact on CO pollution in spring in low latitudes
with a maximum between 20° and 30°, whereas Siberian fires contribute largely
to the pollution in high latitudes, up to 10% in spring and up to 30% in summer. The largest
contributions to BC values in high latitudes are from anthropogenic emissions (about 70%).
CO and BC have larger mass loadings in April than in July, as a result of photochemistry and dynamics.
Citation: Tilmes, S., Emmons, L. K., Law, K. S., Ancellet, G., Schlager, H., Paris, J.-D., Fuelberg, H. E., Streets, D. G., Wiedinmyer, C., Diskin, G. S., Kondo, Y., Holloway, J., Schwarz, J. P., Spackman, J. R., Campos, T., Nédélec, P., and Panchenko, M. V.: Source contributions to Northern Hemisphere CO and black carbon during spring and summer 2008 from POLARCAT and START08/preHIPPO observations and MOZART-4, Atmos. Chem. Phys. Discuss., 11, 5935-5983, doi:10.5194/acpd-11-5935-2011, 2011.