Neutron-capture prompt γ-ray analysis (PGAA) is an exceptionally good method for the determination of the major and minor elements Na, Mg, Al, Si, K, Ca, Ti, Mn and Fe in most geological matrices. The trace elements H, B, S, Cl, Cd, Sm and Gd can often be readily measured in most geological materials. This technique was applied to volcanic ash samples collected in Washington and Montana by various groups following the May 18 eruption of the Mt. St. Helens volcano, as well as to several particulate samples collected at altitudes between 13 and 18 km by a NASA U-2 research aircraft. Groundfall ash samples show distinct elemental variations versus distance from the volcano. For example, Si/Al ratios vary from 2.85 near the volcano to about 3.70 at≽400 km to the east. Samples collected sequentially at a given location (Almira, Washington) also exhibit variations in the elemental ratios. These sequential samples were also subjected to leaching studies to determine soluble B, Cl and S. On the average, PGAA is able to account for 99.4±1.7% of the mass of each sample when the elements are considered to be in their common oxide forms. The stratospheric samples were collected May 19 on IPC cellulose filters on apparatus in a wing tank of the U-2. The PGAA results indicate that the sample from the greatest altitude resembles ashfall near the volcano, while those at lower altitudes somewhat resemble more distant ashfall.