Decomposition of atmospheric aerosol phase function by particle size and asphericity from measurements of single particle optical scattering patterns

We demonstrate an experimental approach that provides insight into how particle size and shape affect the scattering phase function of atmospheric aerosol particles. Central to our approach is the design of an apparatus that measures the forward and backward scattering hemispheres (scattering patterns) of individual atmospheric aerosol particles in the coarse mode range. We captured over 30000 scattering patterns during winter (January 2007) at an urban site in Las Cruces, NM. The size and shape of each particle is discerned from the corresponding scattering pattern. In particular, autocorrelation analysis is used to differentiate between spherical and non-spherical particles, the calculated asphericity factor is used to characterize the morphology of non-spherical particles, and the integrated irradiance is used for particle sizing. We found that the fraction of spherical particles decays exponentially with particle size, decreasing from 11% for particles on the order of 1μm to less than 1% for particles over 5μm. The average phase functions of subpopulations of particles, grouped by size and morphology, are determined by averaging their corresponding scattering patterns. The phase functions of spherical and non-spherical atmospheric particles are shown to diverge with increasing size. In addition, the phase function of non-spherical particles is found to vary little as a function of the asphericity factor. Our results support the current remote sensing practice of characterizing atmospheric aerosol particles as a composition of spherical and non-spherical particles with less concern about the diversity of morphology within non-spherical particles. In addition, our results suggest that assuming a constant spherical fraction independent of particle size may not accurately reflect the real morphological distribution of atmospheric aerosol particles. •Elastic scattering patterns of single atmospheric aerosol particles were captured.•Single particle shape and size were quantified from scattering patterns.•The fraction of spherical particles decreased with increasing scattering size.•Scattering phase functions of particle subpopulations were determined.