Harvard forest regional-scale air mass composition by Patterns in Atmospheric Transport History (PATH)

We calculated 4 years (1990-1993) of back trajectories arriving at Harvard Forest and used them to define patterns in atmospheric transport history. This information was used to assess the degree to which regional-scale transport modulates the chemical composition of air masses sampled at Harvard Forest. Different seasonal signals in trace-gas concentration are derived for different flow patterns. Throughout the year, high-speed transport of cool, dry, cloud-free air from the north and northwest represents background conditions for the Harvard Forest site. These synoptic conditions describe the atmosphere after passage of a cold front. The most polluted conditions in each season occurred under SW flow, with warmer temperatures, higher water vapor mixing ratios, low mixed-layer depths at the site, and a higher frequency of cloudy conditions. These regional-scale air mass characteristics describe synoptic conditions of warm sector transport. In addition to average air mass characteristics, we have analyzed the covariation of species (e.g., O-3 versus NOy-NOx; O-3 versus CO) to address chemical processes based on transport history. For summer daytime measurements, we show that relatively fresh pollutants arrive in SW flow while the most aged air masses with higher O-3 to NOz slopes arrive with W flow, suggesting a Midwestern contribution to regional high-oxidant episodes. These observations of patterns in chemical characteristics related to patterns in transport are corroborated with probability maps indicating the likelihood of transport from upwind regions using trajectories selected for chemical distribution end-members(10(th) and 90(th) percentiles).