Porous glassy particles are a potentially significant but unexplored component of atmospheric aerosol that can form by aerosol processing through the ice phase of high convective clouds. The optical properties of porous glassy aerosols formed from a freeze-dry cycle simulating freezing and sublimation of ice particles were measured using a cavity ring down aerosol spectrometer (CRD-AS) at 532 nm and 355 nm wavelength. The measured extinction efficiency was significantly reduced for porous organic and mixed organic-ammonium sulfate particles as compared to the extinction efficiency of the homogeneous aerosol of the same composition prior to the freeze-drying process. A number of theoretical approaches for modeling the optical extinction of porous aerosols were explored. These include effective medium approximations, extended effective medium approximations, multilayer concentric sphere models, Rayleigh-Debye-Gans theory, and the discrete dipole approximation. Though such approaches are commonly used to describe porous particles in astrophysical and atmospheric contexts, in the current study, these approaches predicted an even lower extinction than the measured one. Rather, the best representation of the measured extinction was obtained with an effective refractive index retrieved from a fit to Mie scattering theory assuming spherical particles with a fixed void content. The single-scattering albedo of the porous glassy aerosols was derived using this effective refractive index and was found to be lower than that of the corresponding homogeneous aerosol, indicating stronger relative absorption at the wavelengths measured. The reduced extinction and increased absorption may be of significance in assessing direct, indirect, and semidirect forcing in regions where porous aerosols are expected to be prevalent.
Bibliographical noteFunding Information:
The authors acknowledge financial support from the Minerva Foundation with funding from the federal German Ministry for Education and Research and from FP7-ENV-2010-265148-PEGASOS. C.H. acknowledges partial support from the Israel Science Foundation (grant 1314/10). C.H. thanks Alexander Moroz for providing the multilayer Mie scattering algorithm and for previous consultation on its use, Qiang Fu for providing the Fu-Sun Mie scattering algorithm and for consultation on its use, V. Ramaswamy for a short discussion on the dynamic effective medium approximation, Bruce Draine for consultation regarding setting up the input for the runs of DDSCAT and for ongoing correspondence on the discrete dipole method, in general and Piotr Flatau for general suggestions regarding calculations of scattering by porous particles.
© 2014. American Geophysical Union. All Rights Reserved.