Models of filter-based particle light absorption measurements

Light absorption by aerosol is very important in the visible, near UN, and near I.R region of the electromagnetic spectrum. Aerosol particles in the atmosphere have a great influence on the flux of solar energy, and also impact health in a negative sense when they are breathed into lungs. Aerosol absorption measurements are usually performed by filter-based methods that are derived from the change in light transmission through a filter where particles have been deposited. These methods suffer from interference between light-absorbing and light-scattering aerosol components. The Aethalometer is the most commonly used filter-based instrument for aerosol light absorption measurement.; This dissertation describes new understanding of aerosol light absorption obtained by the filter method. The theory uses a multiple scattering model for the combination of filter and particle optics. The theory is evaluated using Aethalometer data from laboratory and ambient measurements in comparison with photoacoustic measurements of aerosol light absorption. Two models were developed to calculate aerosol light absorption coefficients from the Aethalometer data, and were compared to the in-situ aerosol light absorption coefficients. The first is an approximate model and the second is a "full" model. In the approximate model two extreme cases of aerosol optics were used to develop a model-based calibration scheme for the 7-wavelength Aethalometer. These cases include those of very strong scattering aerosols (Ammonium sulfate sample) and very absorbing aerosols (kerosene soot sample). The exponential behavior of light absorption in the strong multiple scattering limit is shown to be the square root of the total absorption optical depth rather than linear with optical depth as is commonly assumed with Beer's law.; 2-stream radiative transfer theory was used to develop the full model to calculate the aerosol light absorption coefficients from the Aethalometer data. This comprehensive model allows for studying very general cases of particles of various sizes embedded on arbitrary filter media. Application of this model to the Reno Aerosol Optics Study (Laboratory data) shows that the aerosol light absorption coefficients are about half of the Aethalometer attenuation coefficients, and there is a reasonable agreement between the model calculated absorption coefficients at 521 nm and the measured photoacoustic absorption coefficients at 532 nm. For ambient data obtained during the Las Vegas study, it shows that the model absorption coefficients at 521 nm are larger than the photoacoustic coefficients at 532 nm. Use of the 2-stream model shows that particle penetration depth into the filter has a strong influence on the interpretation of filter-based aerosol light absorption measurements. This is likely explanation for the difference found between model results for filter-based aerosol light absorption and those from photoacoustic measurements for ambient and laboratory aerosol.