Complete control, direct observation and study of molecular super rotors (1304.0438v3)

Abstract: Extremely fast rotating molecules carrying significantly more energy in their rotation than in any other degree of freedom are known as "super rotors". It has been speculated that super rotors may exhibit a number of unique properties. Theoretical studies showed that ultrafast molecular rotation may change the character of molecular scattering from solid surfaces, alter molecular trajectories in external fields, make super rotors stable against collisions, and lead to the formation of gas vortices. New ways of molecular cooling and selective chemical bond breaking by ultrafast spinning have been suggested. Bringing a large number of molecules to fast, directional and synchronous rotation is rather challenging. An efficient method of accelerating molecular rotation with an "optical centrifuge" has been proposed and successfully implemented, yet only indirect evidence of super rotors has been reported to date. Here we demonstrate the first direct observation of molecular super rotors and study their spectroscopic, dynamical and magneto-optical properties. Using the centrifuge technique, we control the degree of rotational excitation and detect molecular rotation with high spectral and temporal resolution. Frequency-resolved detection enables us to map out the energy of extreme rotation levels, two orders of magnitude above the room temperature limit, and quantify the onset of the centrifugal distortion. Femtosecond time resolution reveals highly coherent rotational dynamics with lower de-coherence rates at higher values of the molecular angular momentum, and the increase of the molecular moment of inertia due to the rotation-induced chemical bond stretching. In the presence of an external magnetic field, ultrafast molecular rotation is found to result in an optical birefringence of the molecular ensemble.