1Department of Civil & Environmental Engineering, Michigan Technological University, Houghton, Michigan, USA
2Department of Geological and Mining Engineering and Sciences, Michigan Technological University, Houghton, Michigan, USA
3US EPA, Research Triangle Park, North Carolina, USA
4Institute of Alpine and Arctic Research, University of Colorado at Boulder, Boulder, Colorado, USA
5Department of Atmospheric Sciences, Colorado State University, Fort Collins, Colorado, USA
6Department of Atmospheric & Oceanic Sciences, University of California Los Angeles, Los Angeles, California, USA
*now at: ARCADIS, Novi, Michigan, USA
Abstract. In-situ measurements of carbon monoxide (CO) and ozone (O3) at the Pico Mountain Observatory (PMO) located in the Azores, Portugal are analyzed together with results from atmospheric chemical transport modeling (GEOS-Chem) and satellite remote sensing (AIRS for CO and TES for O3) to examine the evolution of free-troposphere CO and O3 over the North Atlantic for 2001–2011. GEOS-Chem captured the seasonal cycles for CO and O3 well but significantly underestimated the mixing ratios of CO, particularly in spring. Statistically significant (using a significance level of 0.05) decreasing trends were found for both CO and O3 based on harmonic regression analysis of the measurement data. The best estimates of the trend for CO and O3 measurements are −0.31 ± 0.30 (2-σ) ppbv yr−1 and −0.21 ± 0.11 (2-σ) ppbv yr−1, respectively. Similar decreasing trends for both species were obtained with GEOS-Chem simulation results. The major factor contributing to the reported decrease in CO and O3 mixing ratios at PMO over the past decade is the decline in anthropogenic CO and O3-precursor emissions in regions such as North America and Europe. The increase in Asian emissions does not seem to outweigh the impact of these declines resulting in overall decreasing trends for both CO and O3. For O3, however, increase in atmospheric water vapor content associated with climate change also appears to be a contributing factor causing enhanced destruction of the O3 during transport from source regions. These hypotheses are supported by results from the GEOS-Chem tagged CO and tagged O3 simulations.