Sophisticated optical methods provide some of the most promising tools for complete control of a molecule’s energy and orientation, which enables a more complete understanding of chemical reactivity and structure. This dissertation investigates the collision dynamics of molecular super rotors with oriented angular momentum prepared in an optical centrifuge. Molecules with anisotropic polarizabilities are trapped in the electric field of linearly polarized light and then angularly accelerated from 0 to 35 THz over the duration of the optical pulse. This process drives molecules to extreme rotational states and the ensemble of molecules has a unidirectional sense of rotation determined by the propagation of the optical field. High resolution transient IR absorption spectroscopy of the super rotor molecules reveals the dynamics of collisional energy transfer.

These studies show that high energy CO2 and CO rotors release large amounts of translational energy through impulsive collisions.  Time-evolution of the translational energy distribution of the CO2 J=0-100 state shows that depletion from low J states involves molecules with sub-thermal velocities.  Polarization-dependent Doppler profiles of CO rotors show anisotropic kinetic energy release and reveal a majority population of molecular rotors in the initial plane of rotation.  Experimental modifications improved signal to noise levels by a factor of 10, enabling new transient studies in the low-pressure, single-collision regime.  Polarization-dependent studies show that CO2 rotors in the J=54-100 states retain their initial angular momentum orientation, and that this effect increases as a function of rotational angular momentum.  These studies show that rotating molecules behave like classical gyroscopes.  Polarization-dependent measurements of CO2 rotors in the presence of He and Ar buffer gases show that CO2 super rotors are more strongly relaxed by He collisions, demonstrating the importance of rotational adiabaticity in the relaxation process.  Quantum scattering calculations of the He-CO2 and Ar-CO2 collision systems were performed to interpret the qualitative features of the experimental results.  This work provides a detailed mechanistic understanding of the unique collisional dynamics of super rotor molecules.