Tracing the Coherent Manipulation of Rotational Dynamics by Shaped Femtosecond Pulse-Induced Two-Dimensional Rotational Coherent Spectrum.

The temporal delayed orthogonal pulse pairs generated by the phase shaping technique are used to study the coherent control of the rotational wave packet dynamics in air. By continuously changing the intrapulse delay of the pump pulse, we measured the corresponding revival signals and obtained a two-dimensional rotational coherent spectrum (2D RCS). An additive property of the rotational dynamics is observed from the revival signals. Moreover, combining with the coherent control model, we find that the 2D RCS can be used to demonstrate the control over the underlying Raman rotational excitation. A beat frequency-dependent oscillation of each rotational transition is obtained. The transition process is revealed from the Fourier transformation about the pump delay. The scheme of this work can be used for further control and detection of the rotational wave packet and can be extended to other molecular dynamic researches.