A novel technique based on optical patternation is described for three-dimensional diagnostic studies of aerosols used in analytical spectroscopies. The aerosol is illuminated with a thin laser light sheet to capture images of the fluorescence and Lorenz-Mie light-scattering signals from the aerosol field with a charge-coupled detector. These measurements allow for the rapid and nonintrusive elucidation of two-dimensional spray structures, planar mass distributions, and spatial droplet size distributions. The ratio of the fluorescence image to the Lorenz-Mie image is then utilized to construct a spatially resolved map of the volume-to-surface area mean of the aerosol (Sauter mean diameter). Three-dimensional maps of spray structure, mass distribution, and droplet size distribution are obtained for the entire aerosol field by image stacking. The technique is applied to the measurement of the droplet size over the aerosol field at distances of 5-30 mm from the nebulizer tip where droplet sizes ranged from 6 to 12 microm for a direct injection high efficiency nebulizer used in inductively coupled plasma spectrometries.