Journal cover Journal topic
Atmospheric Chemistry and Physics An interactive open-access journal of the European Geosciences Union
Atmos. Chem. Phys., 15, 3575-3603, 2015
© Author(s) 2015. This work is distributed
under the Creative Commons Attribution 3.0 License.
Research article
31 Mar 2015
Multi-model study of chemical and physical controls on transport of anthropogenic and biomass burning pollution to the Arctic
S. A. Monks1,*,**, S. R. Arnold1, L. K. Emmons2, K. S. Law3, S. Turquety4, B. N. Duncan5, J. Flemming6, V. Huijnen7, S. Tilmes2, J. Langner8, J. Mao9, Y. Long4, J. L. Thomas3, S. D. Steenrod5, J. C. Raut3, C. Wilson1, M. P. Chipperfield1, G. S. Diskin10, A. Weinheimer2, H. Schlager11, and G. Ancellet3 1Institute for Climate and Atmospheric Science, School of Earth and Environment, University of Leeds, Leeds, UK
2National Center for Atmospheric Research, Boulder, Colorado, USA
3Sorbonne Universités, UPMC Univ. Paris 06, Université Versailles St-Quentin, CNRS/INSU, LATMOS-IPSL, Paris, France
4Laboratoire de Météorologie Dynamique, IPSL, CNRS, UMR8539, 91128 Palaiseau CEDEX, France
5NASA Goddard Space Flight Center, Greenbelt, USA
6European Centre for Medium range Weather Forecasting, Reading, UK
7Royal Netherlands Meteorological Institute (KNMI), De Bilt, the Netherlands
8Swedish Meteorological and Hydrological Institute, 60176 Norrköping, Sweden
9Program in Atmospheric and Oceanic Sciences, Princeton University and Geophysical Fluid Dynamics Laboratory/National Oceanic and Atmospheric Administration, Princeton, New Jersey, USA
10Chemistry and Dynamics Branch, NASA Langley Research Center, Hampton, VA, USA
11Deutsches Zentrum für Luft- und Raumfahrt (DLR), Institute of Atmospheric Physics, Oberpfaffenhofen, Germany
*now at: Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, Colorado, USA
**now at: Chemical Sciences Division, NOAA Earth System Research Laboratory, Boulder, Colorado, USA
Abstract. Using observations from aircraft, surface stations and a satellite instrument, we comprehensively evaluate multi-model simulations of carbon monoxide (CO) and ozone (O3) in the Arctic and over lower latitude emission regions, as part of the POLARCAT Model Inter-comparison Project (POLMIP). Evaluation of 11- atmospheric models with chemistry shows that they generally underestimate CO throughout the Arctic troposphere, with the largest biases found during winter and spring. Negative CO biases are also found throughout the Northern Hemisphere, with multi-model mean gross errors (9–12%) suggesting models perform similarly over Asia, North America and Europe. A multi-model annual mean tropospheric OH (10.8 ± 0.6 × 105 molec cm−3) is found to be slightly higher than previous estimates of OH constrained by methyl chloroform, suggesting negative CO biases in models may be improved through better constraints on OH. Models that have lower Arctic OH do not always show a substantial improvement in their negative CO biases, suggesting that Arctic OH is not the dominant factor controlling the Arctic CO burden in these models. In addition to these general biases, models do not capture the magnitude of CO enhancements observed in the Arctic free troposphere in summer, suggesting model errors in the simulation of plumes that are transported from anthropogenic and biomass burning sources at lower latitudes. O3 in the Arctic is also generally underestimated, particularly at the surface and in the upper troposphere. Summer O3 comparisons over lower latitudes show several models overestimate upper tropospheric concentrations.

Simulated CO, O3 and OH all demonstrate a substantial degree of inter-model variability. Idealised CO-like tracers are used to quantitatively compare the impact of inter-model differences in transport and OH on CO in the Arctic troposphere. The tracers show that model differences in transport from Europe in winter and from Asia throughout the year are important sources of model variability at Barrow. Unlike transport, inter-model variability in OH similarly affects all regional tracers at Barrow. Comparisons of fixed-lifetime and OH-loss idealised CO-like tracers throughout the Arctic troposphere show that OH differences are a much larger source of inter-model variability than transport differences. Model OH concentrations are correlated with H2O concentrations, suggesting water vapour concentrations are linked to differences in simulated concentrations of CO and OH at high latitudes in these simulations. Despite inter-model differences in transport and OH, the relative contributions from the different source regions (North America, Europe and Asia) and different source types (anthropogenic and biomass burning) are comparable across the models. Fire emissions from the boreal regions in 2008 contribute 33, 43 and 19% to the total Arctic CO-like tracer in spring, summer and autumn, respectively, highlighting the importance of boreal fire emissions in controlling pollutant burdens in the Arctic.

Citation: Monks, S. A., Arnold, S. R., Emmons, L. K., Law, K. S., Turquety, S., Duncan, B. N., Flemming, J., Huijnen, V., Tilmes, S., Langner, J., Mao, J., Long, Y., Thomas, J. L., Steenrod, S. D., Raut, J. C., Wilson, C., Chipperfield, M. P., Diskin, G. S., Weinheimer, A., Schlager, H., and Ancellet, G.: Multi-model study of chemical and physical controls on transport of anthropogenic and biomass burning pollution to the Arctic, Atmos. Chem. Phys., 15, 3575-3603, doi:10.5194/acp-15-3575-2015, 2015.
Publications Copernicus
Short summary
Multi-model simulations of Arctic CO, O3 and OH are evaluated using observations. Models show highly variable concentrations but the relative importance of emission regions and types is robust across the models, demonstrating the importance of biomass burning as a source. Idealised tracer experiments suggest that some of the model spread is due to variations in simulated transport from Europe in winter and from Asia throughout the year.
Multi-model simulations of Arctic CO, O3 and OH are evaluated using observations. Models show...