Gas‐phase chemical characteristics of Asian emission plumes observed during ITCT 2K2 over the eastern North Pacific Ocean

Abstract

The gas‐phase chemical characteristics of emission plumes transported from Asia across the Pacific Ocean observed during the Intercontinental Transport and Chemical Transformation experiment in 2002 (ITCT 2K2) are described. Plumes measured in the troposphere from an aircraft were separated from the background air in data analysis using 1‐s measurements of carbon monoxide (CO), total reactive nitrogen (NOy), and other gas‐phase species along with back trajectory analysis. On the basis of these measurements, Asian transport plumes with CO mixing ratios greater than 150 ppbv were observed on seven flights. Correlations between 1‐s observations of CO, ozone (O3), and NOy are used to characterize the plumes. The NOy/CO ratios were similar in each plume and significantly lower than those derived from estimated Asian emission ratios, indicating substantial removal of soluble NOy species during transport. Observations of nitric oxide (NO), nitrogen dioxide (NO2), nitric acid (HNO3), peroxyacetyl nitrate (PAN), peroxypropionyl nitrate (PPN), and alkyl nitrates are used with the NOy measurements to further distinguish the transport plumes by their NOy partitioning. NOy was primarily in the form of PAN in plumes that were transported in cold high‐latitude and high‐altitude regions, whereas in plumes transported in warmer, lower latitude and altitude regions, NOy was mainly HNO3. Additional gas‐phase species enhanced in these plumes include sulfuric acid, methanol, acetone, propane, and ethane. The O3/CO ratio varied among the plumes and was affected by the mixing of anthropogenic and stratospheric influences. The complexity of this mixing prevents the determination of the relative contribution of anthropogenic and stratospheric influences to the observed O3 levels.