摘要
Systematic monitoring of the fluctuations in atmospheric SO2 oxidation efficiency—measured as a molar ratio of SO42- to total SOx (SOx=SO2+SO42-), referred as S-ratio—have been performed during a major long range plume transport to northeast India (Shillong: 25.67°N, 91.91°E, 1064 m ASL) in March 2009. Anomalously low S-ratios (median, 0.03) were observed during the episode—associated with a cyclonic circulation—and the SO42- and SO2 exhibited unusual features in the ‘relative phase’ of their peaks. During initial days, when SO2 levels were dictated by the long range influx, the SO42- and SO2 variabilities were in anti-phase—for the differing mobility/loss mechanisms. When SO2 levels were governed by the boundary layer diurnality in the latter days, the anti-phase is explained by a ‘depleted OH level’—major portion being consumed in the initial period by the elevated SO2 and other pollutants. Simulations with a global 3D chemical transport model, GEOS-Chem (v8-03-01), also indicated ‘suppressed oxidation conditions’—with characteristic low S-ratios and poor phase agreements. The modelled OH decreased steadily from the initial days, and OH normalized to SO2—referred as OHspecific—was consistently low during the ‘suppressed S-ratio period’. Further, the geographical distribution of modelled OH showed a pronounced minimum over the region surrounding (20°N, 95°E) spanning parts of northeast India and the adjacent regions to the southeast of it—prevalent throughout the year, though the magnitude and the area of influence have a seasonality to it—with significant implications for reducing the oxidizing power of the regional atmosphere. A second set of measurements during January 2010—when prominent long range transports were absent—exhibited no anomalies, and the S-ratios were well within the acceptable limits (median, 0.32). This work highlights the GEOS-Chem model skill in simulating/detecting the ‘transient fluctuations’ in the oxidation efficiency, down to a regional scale.
Systematic monitoring of the fluctuations in atmospheric SO2 oxidation efficiency—measured as a molar ratio of SO42- to total SOx (SOx=SO2+SO42-), referred as S-ratio—have been performed during a major long range plume transport to northeast India (Shillong: 25.67°N, 91.91°E, 1064 m ASL) in March 2009. Anomalously low S-ratios (median, 0.03) were observed during the episode—associated with a cyclonic circulation—and the SO42- and SO2 exhibited unusual features in the ‘relative phase’ of their peaks. During initial days, when SO2 levels were dictated by the long range influx, the SO42- and SO2 variabilities were in anti-phase—for the differing mobility/loss mechanisms. When SO2 levels were governed by the boundary layer diurnality in the latter days, the anti-phase is explained by a ‘depleted OH level’—major portion being consumed in the initial period by the elevated SO2 and other pollutants. Simulations with a global 3D chemical transport model, GEOS-Chem (v8-03-01), also indicated ‘suppressed oxidation conditions’—with characteristic low S-ratios and poor phase agreements. The modelled OH decreased steadily from the initial days, and OH normalized to SO2—referred as OHspecific—was consistently low during the ‘suppressed S-ratio period’. Further, the geographical distribution of modelled OH showed a pronounced minimum over the region surrounding (20°N, 95°E) spanning parts of northeast India and the adjacent regions to the southeast of it—prevalent throughout the year, though the magnitude and the area of influence have a seasonality to it—with significant implications for reducing the oxidizing power of the regional atmosphere. A second set of measurements during January 2010—when prominent long range transports were absent—exhibited no anomalies, and the S-ratios were well within the acceptable limits (median, 0.32). This work highlights the GEOS-Chem model skill in simulating/detecting the ‘transient fluctuations’ in the oxidation efficiency, down to a regional scale.
