Abstract
A new method is presented for the detection and manipulation of magnetic sublevel coherences in excited molecular states. A radio-frequency field induces coherences between a set of molecular levels which were excited by a short optical pulse. The time evolution of the coherences is directly monitored in the modulated fluorescence decay by quantum beat detection. The system can be brought into particular superposition states with radio-frequency pulses of selected lengths and amplitudes. The method is demonstrated for a Zeeman splitJ=1 state in the electronically excited3A2 triplet of the12CS2 molecule. The interpretation and analysis of the experimental results based on the theoretical description have been further elucidated and corroborated by computer simulations. The presented method extends the quantum beat technique and is applicable for labelling of transitions and determination of molecular parameters in complex level structures such as hyperfine structures.
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