We excite diatomic oxygen and nitrogen to high rotational states with an optical centrifuge and study their dynamics in external magnetic field. Ion imaging is employed to directly visualize, and follow in time, the rotation plane of molecular superrotors. The two different mechanisms of interaction between the magnetic field and the molecular angular momentum in paramagnetic oxygen and non-magnetic nitrogen lead to the qualitatively different behaviour. In nitrogen, we observe the precession of the molecular angular momentum around the field vector. In oxygen, strong spin-rotation coupling results in faster and richer dynamics, encompassing the splitting of the rotation plane in three separate components. As the centrifuged molecules evolve with no significant dispersion of the molecular wave function, the observed magnetic interaction presents an efficient mechanism for controlling the plane of molecular rotation.
PACS numbers:Magnetic field is one of the most powerful tools for controlling atomic and molecular dynamics. Both translational and rotational degrees of freedom of molecules have been successfully manipulated via various types of magnetic interaction. Alignment of molecular axes has been accomplished by creating pendular states in paramagnetic molecules at low temperature [1,2]. Gyroscopic precession along the direction of the applied magnetic field has been suggested for non-magnetic molecules in dispersionless "cogwheel" states [3,4]. Spin-rotational coupling has been recently utilized for converting unidirectional molecular rotation into axial alignment, manifested through magneto-rotational optical birefringence under ambient conditions [5,6].Recent progress in creating and detecting unidirectional rotation of molecules [7][8][9][10][11]18] revived the interest in controlling molecular rotation with external magnetic fields. Magnetic effects could further broaden the controllability provided by tunable rotational excitation, including control of molecular collisions [12,13] and scattering of molecules at gas-solid interfaces [14], molecular trajectories [15] and formation of gas vortices [16], optical [5, 17] and acoustic [19,20] properties of a gas of rotating molecules.With the invention of the optical centrifuge technique [21,22], a very flexible control over the degree of rotational excitation became available. The technique proved capable of producing synchronously rotating molecules with narrow rotational state distribution in a wide variety of species up to extremely high angular frequencies [5,23]. However, the spatial orientation of the induced angular momentum is often defined by the propagation direction of the excitation laser beam, and is therefore not easy to manipulate.Here we demonstrate how an applied magnetic field can be used to rotate the plane of molecular rotation. The described method is applicable to a wide variety of molecules and relies on the coupling between the rotation of a molecule and its magnetic moment. An applied magnetic field causes this moment to precess, "...