The dynamics of molecules in the gas and liquid phase is investigated using ultrafast optical techniques. The development of sub-25 fs ultrafast sources using noncollinear optical parametric amplification is discussed. These intense pulses are utilized in coherent anti-Stokes Raman scattering to investigate vibrational motion in I2 Br2 and IBr. For larger bio-molecules relevant dynamics may not be related to the absorption of light. Here, a new technique is introduced, in which an optically excitable molecule is incorporated into the bio-molecule. Photoisomerization of the trigger molecule initiates structural rearrangement in the larger system. To demonstrate this approach, azobenzene was synthesized into short strands of DNA to time-resolve base pair destacking dynamics and DNA melting. The isomerization of azobenzene in thin polymer films (and their corresponding change in optical properties) was also used to write birefringence and surface relief gratings. This method was used to demonstrate a rewritable Bragg filter for telecom wavelengths. Lastly, an alternative to typical crystal based wavemixing is presented for the generation of ultrafast tunable ultraviolet and deep ultraviolet pulses. The approach utilizes difference frequency four wave mixing in hollow waveguides filled with noble gas.