Samples of atmospheric particulate material were collected in the plume of Augustine volcano in February 1976 by using the high-volume filtration system abroad the National Center for Atmospheric Research Lockheed Electra. The samples were analyzed for 38 elements by a combination of instrumental neutron activation analysis and atomic absorption spectrometry. The results indicate that the volatile elements Zn, Cu, Au, Pb, As, Cd, Cl, Br, Se, Sb, Hg, and S are enriched in the atmospheric samples in relation to bulk ash by factors ranging from 10 to several thousand. The enrichments compare closely with those observed for other volcanic emanations and for background aerosols in remote areas of the earth. Samples collected early in the eruption cycle had a much higher quantity of volatile elements in relation to ash than the later samples, indicating a substantial change in the emission of volatiles with time and eruptive cycle.