MAX-DOAS measurements of bromine explosion events in McMurdo Sound, Antarctica
Reactive halogen species (RHS) are responsible for ozone depletion and oxidation of gaseous elemental mercury and dimethyl sulphide in the polar boundary layer, but the sources and mechanisms controlling their catalytic reaction cycles are still not completely understood. To further investigate thes...
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| Format: | Other/Unknown Material |
| Language: | English |
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University of Canterbury. Physics and Astronomy
2010
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| Online Access: | http://hdl.handle.net/10092/5394 https://doi.org/10.26021/8512 |
| Summary: | Reactive halogen species (RHS) are responsible for ozone depletion and oxidation of gaseous elemental mercury and dimethyl sulphide in the polar boundary layer, but the sources and mechanisms controlling their catalytic reaction cycles are still not completely understood. To further investigate these processes, ground– based Multi–Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) observations of boundary layer BrO and IO were made from a portable instrument platform in McMurdo Sound during the Antarctic spring of 2006 and 2007. Measurements of surface ozone, temperature, pressure, humidity, and wind speed and direction were also made, along with fourteen tethersonde soundings and the collection of snow samples for mercury analysis. A spherical multiple scattering Monte Carlo radiative transfer model (RTM) was developed for the simulation of box-air-mass-factors (box-AMFs), which are used to determine the weighting functions and forward model differential slant column densities (DSCDs) required for optimal estimation. The RTM employed the backward adjoint simulation technique for the fast calculation of box-AMFs for specific solar zenith angles (SZA) and MAX-DOAS measurement geometries. Rayleigh and Henyey-Greenstein scattering, ground topography and reflection, refraction, and molecular absorption by multiple species were included. Radiance and box-AMF simulations for MAX-DOAS measurements were compared with nine other RTMs and showed good agreement. A maximum a posteriori (MAP) optimal estimation algorithm was developed to retrieve trace gas concentration profiles from the DSCDs derived from the DOAS analysis of the measured absorption spectra. The retrieval algorithm was validated by performing an inversion of artificial DSCDs, simulated from known NO2 profiles. Profiles with a maximum concentration near the ground were generally well reproduced, but the retrieval of elevated layers was less accurate. Retrieved partial vertical column densities (VCDs) were similar to the known values, and ... |
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