This thesis reports the effects of ultrashort laser pulse irradiation of various materials. The morphology after irradiation was examined using several microscopy techniques. Emphasis was placed on the identification of crystallographic changes and the analysis of laser-induced periodic surface structures. Grooves were machined in silicon by translating the target under the focused laser beam. The resulting depths were measured as a function of pulse energy, translation speed, and number of consecutive passes, for 800 and 400nm wavelength irradiation. The wall morphology and a corrugation along the bottom of the grooves were characterized. Various polarization configurations relative to the translation direction were compared. Such characterizations are relevant for the practical application of femtosecond laser micromachining. Silicon and gallium phosphide exhibited periodic structures after irradiation using photon energies less than the bandgap energy, with periods as small as ~20% of the irradiation wavelength. The significantly sub-wavelength periodic structures had a shallow profile on silicon, appearing as fine lines or grids of protrusions and depressions. On gallium phosphide, the surface evolved into planar-like structures with a large aspect ratio, possessing crystalline centers coated with amorphous material. These investigations, along with additional experiments, would help identify the precise physical origins of the short-period structures. On silicon and germanium, the target crystal orientation was shown to affect the formation of certain morphological features. For multiple-pulse irradiation, the (100) and (111) surface orientations exhibited significantly different tendencies for large conical structure formation. A thin layer of defected material coated the conical structures, with some defects present within the periodic structures. The different crystalline orientations did not affect periodic structuring. Cross-sectional transmission electron microscopy of silicon after irradiation by single pulses revealed amorphous material and dislocations in the bulk for sufficiently high pulse fluences. On a sample consisting of a metal layer on thermally-grown oxide on silicon, a range of pulse fluences was found which removed the metal layer without observed thinning of the oxide layer. Within this fluence range, above a particular fluence substantial defects were formed in the underlying silicon. Although ultrashort pulse irradiation of materials is frequently considered to be 'damage-free', attention should be paid to sub-surface modifications not evident from surface imaging. For the drilling of holes in copper foils, the pulse duration did not strongly affect the final morphology for durations under several picoseconds. A photodiode below the foil during drilling recorded transmitted light, indicating the number of pulses required for penetration under a variety of conditions, and characterizing hole evolution during drilling. Periodic surface structuring on the walls of holes depended on the irradiation atmosphere, pulse duration, and laser polarization. These measurements provide insight into the physical processes of material modification, and for the selection of irradiation parameters in practical applications. / Thesis / Doctor of Philosophy (PhD)