The high-resolution infrared absorption spectra of the Atmospheric Trace Molecule Spectroscopy (ATMOS) experiment are utilized to derive vertical profiles of sulfate aerosol volume density and extinction coefficient. Following the eruption of Mt. Pinatubo in June 1991, the ATMOS spectra obtained on three Space Shuttle missions (1992, 1993, and 1994) provide a unique opportunity to study the global stratospheric sulfate aerosol layer shortly after a major volcanic eruption and periodically during the decay phase. Synthetic sulfate aerosol spectra are fit to the observed spectra, and a global fitting inversion routine is used to derive vertical profiles of sulfate aerosol volume density. Vertical profiles of sulfate aerosol volume density for the three missions over portions of the globe are presented, with the peak in aerosol volume density occurring from as low as 10 km (polar latitudes) to as high as 20 km (subtropical latitudes). Derived aerosol volume density is as high as 2--3.5 ¿m3 cm-3 ¿10% in 1992, decreasing to 0.2--0.5 ¿m3 cm-3 ¿20% in 1994, in agreement with other experiments. Vertical extinction profiles derived from ATMOS are compared with profiles from Improved Stratospheric And Mesospheric Sounder (ISAMS) and Cryogenic Limb Array Etalon Spectrometer (CLAES) that coincide in space and time and show good general agreement. The uncertainty of the ATMOS vertical profiles is similar to CLAES and consistently smaller than ISAMS at similar altitudes.