Analysis of atmospheric transport and the effects of seasonal and interannual transport variability on measurements made at the Pico Mountain observatory

A non-hierarchical K-means algorithm is used to cluster 47 years (1960–2006) of 10-day HYSPLIT backward trajectories to the Pico Mountain (PM) observatory on a seasonal basis. The resulting cluster centers identify the major transport pathways and collectively comprise a long-term climatology of transport to the observatory. The transport climatology improves our ability to interpret the observations made there and our understanding of pollution source regions to the station and the central North Atlantic region. I determine which pathways dominate transport to the observatory and examine the impacts of these transport patterns on the O3, NOy, NOx, and CO measurements made there during 2001–2006. Transport from the U.S., Canada, and the Atlantic most frequently reaches the station, but Europe, east Africa, and the Pacific can also contribute significantly depending on the season. Transport from Canada was correlated with the North Atlantic Oscillation (NAO) in spring and winter, and transport from the Pacific was uncorrelated with the NAO. The highest CO and O3 are observed during spring. Summer is also characterized by high CO and O3 and the highest NOy and NOx of any season. Previous studies at the station attributed the summer time high CO and O3 to transport of boreal wildfire emissions (for 2002–2004), and boreal fires continued to affect the station during 2005 and 2006. The particle dispersion model FLEXPART was used to calculate anthropogenic and biomass-burning CO tracer values at the station in an attempt to identify the regions responsible for the high CO and O3 observations during spring and biomass-burning impacts in summer.

Long-Range Pollution Transport: Trans-Atlantic Mechanisms and Lagrangian Modeling Methods

Over the past several decades, it has become apparent that anthropogenic activities have resulted in the large-scale enhancement of the levels of many trace gases throughout the troposphere. More recently, attention has been given to the transport pathway taken by these emissions as they are dispersed throughout the atmosphere. The transport pathway determines the physical characteristics of emissions plumes and therefore plays an important role in the chemical transformations that can occur downwind of source regions. For example, the production of ozone (O3) is strongly dependent upon the transport its precursors undergo. O3 can initially be formed within air masses while still over polluted source regions. These polluted air masses can experience continued O3 production or O3 destruction downwind, depending on the air mass's chemical and transport characteristics. At present, however, there are a number of uncertainties in the relationships between transport and O3 production in the North Atlantic lower free troposphere. The first phase of the study presented here used measurements made at the Pico Mountain observatory and model simulations to determine transport pathways for US emissions to the observatory. The Pico Mountain observatory was established in the summer of 2001 in order to address the need to understand the relationships between transport and O3 production. Measurements from the observatory were analyzed in conjunction with model simulations from the Lagrangian particle dispersion model (LPDM), FLEX-PART, in order to determine the transport pathway for events observed at the Pico Mountain observatory during July 2003. A total of 16 events were observed, 4 of which were analyzed in detail. The transport time for these 16 events varied from 4.5 to 7 days, while the transport altitudes over the ocean ranged from 2-8 km, but were typically less than 3 km. In three of the case studies, eastward advection and transport in a weak warm conveyor belt (WCB) airflow was responsible for the export of North American emissions into the FT, while transport in the FT was governed by easterly winds driven by the Azores/Bermuda High (ABH) and transient northerly lows. In the fourth case study, North American emissions were lofted to 6-8 km in a WCB before being entrained in the same cyclone's dry airstream and transported down to the observatory. The results of this study show that the lower marine FT may provide an important transport environment where O3 production may continue, in contrast to transport in the marine boundary layer, where O3 destruction is believed to dominate. The second phase of the study presented here focused on improving the analysis methods that are available with LPDMs. While LPDMs are popular and useful for the analysis of atmospheric trace gas measurements, identifying the transport pathway of emissions from their source to a receptor (the Pico Mountain observatory in our case) using the standard gridded model output, particularly during complex meteorological scenarios can be difficult can be difficult or impossible. The transport study in phase 1 was limited to only 1 month out of more than 3 years of available data and included only 4 case studies out of the 16 events specifically due to this confounding factor. The second phase of this study addressed this difficulty by presenting a method to clearly and easily identify the pathway taken by only those emissions that arrive at a receptor at a particular time, by combining the standard gridded output from forward (i.e., concentrations) and backward (i.e., residence time) LPDM simulations, greatly simplifying similar analyses. The ability of the method to successfully determine the source-to-receptor pathway, restoring this Lagrangian information that is lost when the data are gridded, is proven by comparing the pathway determined from this method with the particle trajectories from both the forward and backward models. A sample analysis is also presented, demonstrating that this method is more accurate and easier to use than existing methods using standard LPDM products. Finally, we discuss potential future work that would be possible by combining the backward LPDM simulation with gridded data from other sources (e.g., chemical transport models) to obtain a Lagrangian sampling of the air that will eventually arrive at a receptor.