Towards Aerosol Light-Absorption Measurements with a 7-Wavelength Aethalometer: Evaluation with a Photoacoustic Instrument and 3-Wavelength Nephelometer

Abstract

Two extreme cases of aerosol optics from the Reno Aerosol Optics Experiment are used to develop a model-based calibration scheme for the 7-wavelength aethalometer. The cases include those of very white and very dark aerosol samples. The former allows for an assessment of the scattering offset associated with this filter-based method, with the wavelength-dependent scattering measured from a 3-wavelength nephelometer, and interpolated and extrapolated to the 7 wavelengths of the aethalometer. A photoacoustic instrument operating at 532 nm is used to evaluate the filter loading effect caused by aerosol light absorption. Multiple scattering theory is used to analytically obtain a filter-loading correction function. This theory shows that the exponential behavior of light absorption in the strong multiple scattering limit scales as the square root of the total absorption optical depth rather than linearly with optical depth as is commonly assumed with Beer's law. The multiple scattering model also provides a theoretical justification for subtracting a small fraction of aerosol light scattering away from measured apparent light absorption by the filter method. The model is tested against ambient measurements and is found to require coefficients that are situation specific. Several hypotheses are given for this specificity, and suggested methods for reducing it are discussed. Specific findings are as follows. Simultaneous aerosol light-scattering measurements are required for accurate interpretation of aethalometer data for high aerosol single-scattering albedo. Instantaneous errors of up to ±50% are possible for uncorrected data, depending on filter loading. The aethalometer overpredicts black carbon (BC) concentration on a fresh filter and underpredicts BC on a loaded filter. BC and photoacoustic light absorption can be tightly correlated if the data are averaged over the full range of filter loadings and the aerosol source is constant. Theory predicts that the Aethalometer response may be sensitive to filter face velocity, and hence flow rate, to the extent that particle penetration depth depends on face velocity.