Geoffrey S. Dutton

Urban/industrial pollution for the New York City–Washington, D. C., corridor, 1996–1998: 1. Providing independent verification of CO and PCE emissions inventories

Atmospheric mixing ratios of carbon monoxide (CO) and perchloroethylene (PCE, C 2 Cl 4 ) were measured above the canopy at Harvard forest, MA every half-hour for 3 years starting in January 1996. Pollution enhancements are strongly correlated with winds from the southwest, the direction of the New York City-Washington, D. C., corridor, as compared to background levels observed during northwest winds traveling from Canada. We establish the ratio of CO to PCE pollution enhancements by wind direction, by season, and by year and use these results to test the quality of county-level and national source emission inventories for these two gases. The EPA carbon monoxide emission county-level inventories and the McCulloch and Midgley sales-based national-level PCE release estimates are found to be in accord with our independent observations of urban/industrial releases. For the New York City-Washington, D. C., corridor the inventory-based CO I l PCE I emissions ratio of 584 (kg/kg) for 1996 falls well within the range of observationally-based ACO/APCE pollution plume ratios of 388 to 706 (kg/kg) and is only 11% higher than the observed mean of 521 ± 90 (kg/kg). On the basis of this agreement, PCE emission estimates for 1997 and 1998 are derived from the CO inventory emissions values and the observed ΔCO/ΔPCE ratios in pollution plumes for those years; despite the call for voluntary cutbacks, urban/industrial emissions of PCE appear to be on the rise.

Vertical transport rates in the stratosphere in 1993 from observations or CO2, N2O and CH4

Measurements of CO2, N2O and CH4 are analyzed to define hemispheric average vertical exchange rates in the lower stratosphere from November 1992 to October 1993. Effective vertical diffusion coefficients were small in summer, ≤ 1 m²s−1 at altitudes below 25 km; values were similar near the tropopause in winter, but increased markedly with altitude. The analysis suggests possibly longer residence times for exhaust from stratospheric aircraft, and more efficient transport from 20 km to the middle stratosphere, than predicted by many current models. Seasonally-resolved measurements of stratospheric CO2 and N2O provide significant new constraints on rates for global-scale vertical transport.

Changes in the levels and variability of halocarbons and the compliance with the Montreal Protocol from an urban view

Ambient levels and variability of major atmospheric halocarbons, i.e. CFC-12, CFC-11, CFC-113, CCl4, CH3CCl3, C2HCl3, and C2Cl4 in a major metropolis (Taipei, Taiwan) were re-investigated after fourteen years by flask sampling in 2012. Our data indicates that the variability expressed as standard deviations (SD) of CFC-113 and CCl4 remained small (2.0 ppt and 1.9 ppt, respectively) for the 10th-90th percentile range in both sampling periods; whereas the variability of CFC-12, CFC-11, C2HCl3, and C2Cl4 measured in 2012 became noticeably smaller than observed in 1998, suggesting their emissions were reduced over time. By comparing with the background data of a global network (NOAA/ESRL/GMD baseline observatories), the ambient levels and distribution of these major halocarbons in Taipei approximated those at a background site (Mauna Loa) in 2012, suggesting that the fingerprint of the major halocarbons in a used-to-be prominent source area has gradually approached to that of the background atmosphere.