In situ aircraft measurements of the sizes and concentrations of liquid cloud droplets and ice crystals with maximum dimensions (D_max) less than ~50 μm have been measured mainly using forward scattering probes over the past half century. The operating principle of forward scattering probes is that the measured intensity of light scattered by a cloud particle at specific forward scattering angles can be related to the size of that particle assuming the shape and thermodynamic phase of the target are known. Current forward-scattering probes assume spherical liquid cloud droplets and use the Lorenz–Mie theory to convert the scattered light to particle size. Uncertainties in sizing ice crystals using forward scattering probes are unavoidable since the single-scattering properties of ice crystals differ from those of spherical liquid cloud droplets and because their shapes can vary. In this study, directional scattering intensities of four different aspect ratios (ARs = 0.25, 0.50, 1.00, and 2.00) of hexagonal ice crystals with random orientations and of spherical liquid cloud droplets were calculated using the discrete dipole approximation (i.e., ADDA) and Lorenz–Mie code, respectively, to quantify the errors in sizing small ice crystals and cloud droplets using current forward scattering probes and to determine the ranges of optimal scattering angles that would be used in future forward scattering probes. The calculations showed that current forward scattering probes have average 5.0% and 17.4% errors in sizing liquid cloud droplets in the forward (4–12°) and backward (168–176°) direction, respectively. For measurements of hexagonal ice crystals, average sizing errors were 42.1% (23.9%) in the forward (backward) direction and depended on the ARs of hexagonal ice crystals, which are larger than those for liquid cloud droplets. A newly developed size conversion table based on the calculated single-scattering properties of hexagonal ice crystals using the ADDA reduced the sizing errors for the hexagonal ice crystals down to 14.2% (21.9%) in the forward (backward) direction. This study is a purely theoretical examination of the operating principle of forward scattering probes and there are several limitations, such as assumed hexagonal ice crystals with smooth surfaces and random orientations.

We estimated source-based aerosol optical properties for polydisperse aerosols according to a chemical-species-resolved mass contribution method based on source apportionment. We investigated the sensitivity of aerosol optical properties based on PM2.5 (particulate matter that have a diameter of less than 2.5 micrometers) monitoring results. These aerosols were composed of ions, metals, elemental carbon, and water-soluble organic carbon which includes humic-like carbon substances and water-soluble organic carbon. We calculated aerosols’ extinction coefficients based on the PM2.5 composition data and the results of a multivariate receptor model (Solver for Mixture Problem model, SMP). Based on the mass concentration of chemical composition and nine sources calculated with the SMP receptor model, we estimated the size-resolved mass extinction efficiencies for each aerosol source using a multilinear regression model. Consequently, this study quantitatively determined the size resolved sources contributing to the apportionment-based aerosol optical properties and calculated their respective contributions. The results show that source-resolved mass concentrations and extinction coefficients had varying contributions. This discrepancy between the source-based mass concentration and extinction coefficient was mainly due to differences between the source-dependent aerosol size distribution and the aerosol optical properties from different sources.

In this study, the sensitivity of the optical properties of carbonaceous aerosols, especially humic-like substances (HULIS), are investigated based on a one-year measurement of ambient fine atmospheric particulate matter (PM_2.5) at a Global Atmospheric Watch (GAW) station in South Korea. The extinction, absorption coefficient, and radiative forcing (RF) are calculated from the analysis data of water soluble (WSOC) and insoluble (WISOC) organic aerosols, elemental carbon (EC), and HULIS. The sensitivity of the optical properties on the variations of refractive index, hygroscopicity, and light absorption properties of HULIS as well as the polydispersity of organic aerosols are studied. The results showed that the seasonal absorption coefficient of HULIS varied from 0.09 to 11.64 Mm⁻¹ and EC varied from 0.11 to 3.04 Mm⁻¹ if the geometric mean diameter varied from 0.1 to 1.0 µm and the geometric standard deviation varied from 1.1 to 2.0, with the imaginary refractive index (IRI) of HULIS varying from 0.006 to 0.3. Subsequently, this study shows that the RF of HULIS was larger than other constituents, which suggested that HULIS contributed significantly to radiative forcing.

The international journal of Aerosol and Air Quality Research (AAQR) covers all aspects of aerosol science and technology, atmospheric science and air quality related issues.