Polarization Studies of Highly Oriented Carbon Dioxide Super Rotors

Controlling molecular motion could enable manipulation of energy flow between molecules.~ We have used a high power optical centrifuge IR spectrometer to investigate energy transfer between molecular super rotors with oriented angular momenta.~ The polarizable electron cloud of the molecules interacts with the electric field of linearly polarized light that angularly accelerates over the time of the optical pulse.~ This process drives molecules into high angular momentum states that are oriented with the optical field and have energies far from equilibrium.~ High resolution transient IR spectroscopy reveals the dynamics of collisional energy transfer for these super excited rotors.~ We make time-dependent measurements of individual rotational states of carbon dioxide ranging from J$=$0 to J$=$100.~ Polarization-dependent studies show that the initial angular momentum orientation persists even after thousands of collisions, indicating that molecules in an optical centrifuge behave as quantum gyroscopes.