Using molecules as a quantum interface to store ultrashort optical vortices

Abstract

We exploit gas-phase molecules as light-matter interface to store an orbital angular momentum (OAM) or a superposition of OAM states (OAM-based photonic qubits) carried by ultrashort laser pulses. The interplay between spin angular momentum and OAM is exploited to encode the amplitude and spatial phase information of light beams into rotational coherences of molecules. This last is restored on-demand over tens of picoseconds with a reading beam by taking advantage of field-free molecular alignment. The underlying mechanism at the origin of the storage can be interpreted by the spatial structuring of the molecular sample induced by the field. The excitation indeed produces an inhomogeneous spatial distribution of molecular alignment (amplitude & orientation) whose periodical revivals associated with the quantum beatings of the rotational wavepacket enables to restore the spatial beam structure on-demand. The strategy is successfully demonstrated in CO2 molecules at room temperature. Besides applicability as storage medium with THz bandwidth application, the use of molecules as light-matter interface opens new functionalities in terms of optical processing and versatile control of OAM fields.