The cleaning of mirrored surfaces by a patented ultraviolet laser-cleaning process is effective in removing molecular and particulate contaminants. The cleaning process, developed for use in the semiconductor industry, uses a pulsed excimer laser, typically operating at 308 nm, as an energy source. The raw-beam intensity profiles is homogenized to a ''top-hat'' profile to ensure precise, controlled removal of contaminants. The technology has been shown to be effective in removing, without damage to the surface, such contaminants as water (liquid or frozen), dioctyl phthalate, diffusion pump oils, fingerprints, silicon-dioxide particles, dust, and many other potential contaminants from quartz (bare and antireflection-coated), nickel, gold, beryllium, polymeric, and other surfaces. The cleaning process is equally effective in ambient and cryogenic/vacuum environments. Beam-energy densities of less than 0.5-J/sq cm pulse are generally sufficient to achieve complete cleaning. Examination of cleaned surfaces by optical, electrooptical, and light-scattering measurement techniques show that the cleaning process returns the substrate surface quality to the original level.