Photo-thermo-refractive (PTR) glass is an ideal photosensitive material for recording phase volume holograms. It is a homogeneous multi-component silicate glass that demonstrates all the advantages of optical glass: thermal stability, high laser damage threshold, and a wide transparency range. Moreover the ability to record phase patterns (i.e. spatial refractive index variations) into PTR glass has resulted in the fabrication of volume holograms with diffraction efficiency greater than 99%. The conventional method of recording a hologram in PTR glass relies on exposure to continuous-wave ultraviolet laser radiation.;In this dissertation the interaction between infrared ultrashort laser pulses and PTR glass is studied. It is shown that photosensitivity in PTR glass can be extended from the UV region to longer wavelengths (near-infrared) by exposure to ultrashort laser pulses. It is found that there exists a focusing geometry and laser pulse intensity interval for which photoionization and refractive index change in PTR glass after thermal development occur without laser-induced optical damage. Photoionization of PTR glass by IR ultrashort laser pulses is explained in terms of strong electric field ionization. This phenomenon is used to fabricate phase optical elements in PTR glass.;The interaction between ultrashort laser pulses and volume holograms in PTR glass is studied in two laser intensity regimes. At intensities below ∼10 12 W/cm2 properties such as diffraction efficiency, angular divergence, selectivity, and pulse front tilt are shown to agree with the theory of linear diffraction for broad spectral width lasers. A volume grating pair arrangement is shown to correct the laser pulse distortions arising from pulse front tilt and angular divergence. At higher intensities of irradiation, nonlinear generation and diffraction of third harmonic is observed for three types of interactions: sum-frequency generation, front-surface THG generation, and THG due to