| Background and pollution trends and cycles of fourteen trace gases over the Northeastern U.S. are inferred from continuous atmospheric observations at the Harvard Forest research station located in Petersham, Massachusetts. This site receives background 'clean' air from the northwest (Canada) and 'dirty' polluted air from the southwest (New York City--Washington, D.C. corridor). Mixing ratios of gases regulated by the Montreal Protocol or other policies (CO, PCE, CFC11, CFC12, CFC113, CH 3CCl3, CCl4, and Halon-1211) and of those not subject to restrictions (H2, CH4, CHCl3, TCE, N2O, and SF6) were measured over the three-year period, 1996 to 1998, every 24 minutes by a fully automated gas chromatographic instrument with electron capture detectors. Evidence for polar vortex venting is found consistently in the month of June of the background seasonal cycles. The ratio of CO and PCE enhancements borne on southwesterly winds are in excellent agreement with county-level EPA and sales-based inventories for the New York City--Washington, D.C. region. From this firm footing, we use CO and PCE as reference compounds to determine the urban/industrial source strengths for the other species. A broad historical and geographic study of emissions reveals that the international treaty has by and large been a success. Locally, despite the passing of the 1996 Montreal Protocol ban, only emissions of CFC12 and CH3CCl3 are abating. Though source strengths are waning, the sources are not spent and continued releases to the atmosphere may be expected for some years to come. For CH3CCl3, whose rate of decline is central to our understanding of atmospheric processes, we estimate that absolute concentrations may persist until around the year 2010. The long-term high frequency time series of hydrogen provided here represents the first such data set of its kind. The H2 diurnal cycle is established and explained in terms of its sources and sinks. The ratio of H2 to CO in pollution plumes is found to be a seasonal and unchanged since early automobile exhaust studies of the 1960s, despite the many restrictions placed on car emissions and fuels since that time. Based on this result, a spatial inventory of H2 emissions from fossil fuel combustion is developed at the county level for the entire Northeastern U.S. |
