Can a hemispherical scanning imaging differential optical absorption spectroscopy technique be used to improve understanding of the emissions, dynamics and chemistry of nitrogen dioxide in the urban boundary layer?

摘要

Air quality is an international issue which has been the subject of several European directives on pollution levels as atmospheric pollutants can have significant effects on human health, ecosystems and climate change, especially at high levels. In the UK the largest sources of atmospheric pollutants are products of combustion from power generation and motor vehicles including NO[subscript x] (NO and NO[subscript 2]), CO, VOCs and particulate matter. Hence it is becoming increasingly important to measure changes in these air pollutants especially in urban areas where these pollutants are at the highest levels.\udDifferential Optical Absorption Spectroscopy is now commonly used as an air quality tool; primarily through the measurements of nitrogen dioxide (NO[subscript 2]). CityScan is a Hemispherical Scanning Imaging Differential Optical Absorption Spectrometer (HSI-DOAS) which has been optimised to measure concentrations of NO[subscript 2]. This thesis will describe the development and subsequent deployment of three CityScan instruments and the first results from these deployments.\udCityScan has a 95° field of view (FOV) between the zenith and 5° below the horizon. Across this FOV there are 128 resolved elements which are measured concurrently, the spectrometer is rotated azimuthally 1° per second providing full hemispherical coverage every 6 minutes.\udThree CityScan instruments were built between 2009 and 2012 and deployed in various locations, including Leicester, London and Bologna. Data from one of these instruments has been validated with a MAX-DOAS instrument (TROPOGAS) and in situ monitors. The comparison with the TROPOGAS instrument produced gradient values between 0.7 and 1 with R² values rarely lower than 0.7. An NO[subscript 2] detection limit of CityScan has been calculated to be 4 x 10[superscript 15] mol cm[superscript -2].\udThe extensive field of view of the CityScan instruments has allowed NO[subscript 2] concentrations to be mapped on city-wide scales allowing areas of high and low pollution to be identified with a spatial resolution which has never been possible before without the use of models.