The complex refractive indices of eight volcanic ash samples, chosen to have a representative range of SiO2 contents, were retrieved from simultaneous measurements of their spectral mass extinction coefficient and size distribution. The mass extinction coefficients, at 0.33–19 μm, were measured using two optical systems: a Fourier transform spectrometer in the infrared and two diffraction grating spectrometers covering visible and ultraviolet wavelengths. The particle size distribution was measured using a scanning mobility particle sizer and an optical particle counter; values for the effective radius of ash particles measured in this study varied from 0.574 to 1.16 μm. Verification retrievals on high‐purity silica aerosol demonstrated that the Rayleigh continuous distribution of ellipsoids (CDEs) scattering model significantly outperformed Mie theory in retrieving the complex refractive index, when compared to literature values. Assuming the silica particles provided a good analogue of volcanic ash, the CDE scattering model was applied to retrieve the complex refractive index of the eight ash samples. The Lorentz formulation of the complex refractive index was used within the retrievals as a convenient way to ensure consistency with the Kramers‐Kronig relation. The short‐wavelength limit of the electric susceptibility was constrained by using independently measured reference values of the complex refractive index of the ash samples at a visible wavelength. The retrieved values of the complex refractive indices of the ash samples showed considerable variation, highlighting the importance of using accurate refractive index data in ash cloud radiative transfer models.

The detection and quantification of volcanic ash is extremely important to the aviation industry, civil defense organizations, and those in peril from volcanic ashfall. To exploit the remote sensing techniques that are used to monitor a volcanic cloud and return information on its properties, the effective complex refractive index of the volcanic ash is required. This paper presents the complex refractive index determined in the laboratory at 450.0 nm, 546.7 nm, and 650.0 nm for volcanic ash samples from eruptions of Aso (Japan), Grímsvötn (Iceland), Chaitén (Chile), Etna (Italy), Eyjafjallajökull (Iceland), Tongariro (New Zealand), Askja (Iceland), Nisyros (Greece), Okmok (Alaska), Augustine (Alaska), and Spurr (Alaska). The Becke line method was used to measure the real part of the refractive index with an accuracy of 0.01. The values measured differed between eruptions and were in the range 1.51-1.63 at 450.0 nm, 1.50-1.61 at 546.7 nm, and 1.50-1.59 at 650.0 nm. A novel method is introduced to derive the imaginary part of the refractive index from the attenuation of light by ash. The method has a precision in the range 10 −3 -10 −4 . The values for the ash imaginary refractive index ranged 0.22-1.70 × 10 −3 at 450.0 nm, 0.16-1.93 × 10 −3 at 546.7 nm, and 0.15-2.08 × 10 −3 at 650.0 nm. The accuracy of Becke and attenuation methods was assessed by measuring the complex refractive index of Hoya neutral density glass and found to have an accuracy of < 0.01 and < 2 × 10 −5 for the real and imaginary parts of the refractive index, respectively.

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We investigate the accuracy in retrieving the real refractive index of submicron aerosol particles, at a visible wavelength, from near critical angle reflectance measurements of a dilute suspension of the aerosol. A coherent scattering model (CSM) is used to model the coherent reflectance from the colloidal suspension. We use an extension of the model for polydisperse particles to properly account for the modified size distribution close to the incident medium to colloid interface. We perform a rigorous sensitivity analysis, for both the monodisperse and polydisperse models, to determine how experimental uncertainties propagate into uncertainty in the retrieval of real refractive index. The effect of non-spherical scattering was included in the sensitivity analysis by using T-matrix methods. Experimental reflectance data, at a wavelength of 635 nm, were obtained for monodisperse spherical latex particles, a polydisperse sand sample and a polydisperse volcanic ash sample. We show that the retrieved real refractive index for these particles is consistent with values obtained using other techniques.