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Extremely fast rotating molecules carrying significantly more energy in theirrotation than in any other degree of freedom are known as "super rotors". Ithas been speculated that super rotors may exhibit a number of uniqueproperties. Theoretical studies showed that ultrafast molecular rotation maychange the character of molecular scattering from solid surfaces, altermolecular trajectories in external fields, make super rotors stable againstcollisions, and lead to the formation of gas vortices. New ways of molecularcooling and selective chemical bond breaking by ultrafast spinning have beensuggested. Bringing a large number of molecules to fast, directional andsynchronous rotation is rather challenging. An efficient method of acceleratingmolecular rotation with an "optical centrifuge" has been proposed andsuccessfully implemented, yet only indirect evidence of super rotors has beenreported to date. Here we demonstrate the first direct observation of molecularsuper rotors and study their spectroscopic, dynamical and magneto-opticalproperties. Using the centrifuge technique, we control the degree of rotationalexcitation and detect molecular rotation with high spectral and temporalresolution. Frequency-resolved detection enables us to map out the energy ofextreme rotation levels, two orders of magnitude above the room temperaturelimit, and quantify the onset of the centrifugal distortion. Femtosecond timeresolution reveals highly coherent rotational dynamics with lower de-coherencerates at higher values of the molecular angular momentum, and the increase ofthe molecular moment of inertia due to the rotation-induced chemical bondstretching. In the presence of an external magnetic field, ultrafast molecularrotation is found to result in an optical birefringence of the molecularensemble.

Complete control, direct observation and study of molecular super rotors