Airborne DOAS measurements over the South African highveld

Abstract

A thesis submitted to the Faculty of Geography, Archaeology, and Environmental Studies University of the Witwatersrand, Johannesburg, in fulfilment of the requirements of the degree of Doctor of Philosophy. 2015.An imaging DOAS instrument, along with in situ trace-gas and aerosol instrumentation was deployed on board a research aircraft over the Highveld region of South Africa, to make regional-scale measurements of nitrogen dioxide (NO2). The presence of a “hotspot” of NO2 over the Highveld is confirmed. Case-study estimates of NO2 emission flux were made downwind of a power station (10 tons.hr−1), a petrochemical plant (36 tons.hr−1) and the entire Highveld region (395 tons.hr−1). Vertical profile measurements were used to develop scenarios for a radiative transfer sensitivity study. From this, suitable air-mass factors for the DOAS measurements were determined. Comparisons between the airborne DOAS and satellite instruments show a good agreement where the spatial scales of the satellite ground pixels and the features in the two-dimensional trace-gas distribution are matched. A long-term record of satellite data was analysed. Analysis of radiative transfer revealed a possible artefact in the adjacent positive and negative trends evident on the Highveld. A correction to the satellite record for a seasonal bias was made, and found to be important over biomass burning regions in Angola and Zambia. Spatial features in a seasonal model of the satellite record are shown to correspond with known urban, industrial and biomass burning sources in the region. Signatures of soil emissions are also detected

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