In this dissertation a combination of experimental and computational techniques are used to investigate the interaction of high intensity ultrashort pulses with nonlinear optical materials and devices. In particular, degenerate four-wave mixing in the forward two-pulse geometry was combined with the numerical solution to the optical Bloch equations to extract an electronic dephasing time in the infrared absorbing organic dye IR140. Additionally, finite difference time-domain simulations were used to investigate the reflective properties of three dielectric structures, a quarter-wave dielectric stack, a continuously varying rugate and a discretely varying rugate for the case of high intensity ultrashort pulses. Finally a combination of linear and nonlinear spectroscopies were used to investigate the optical properties ofgreen fluorescent protein. Ab initio and semi-empirical quantum chemistry techniques were used as an aid to interpreting the experimental data.
