Abstract
Linearly chirped femtosecond laser pulses are used to excite ro-vibrational wave packets in lithium dimers from a single well-prepared launch state. Two-photon resonant Raman transitions excite a manifold of rotational states in a coherent superposition. Excitation with positively chirped laser pulses is shown to enhance a quantum beat involving states with lower rotational quantum numbers, whereas negatively chirped pulses enhance a quantum beat between states with higher rotational quantum numbers, thus steering the rotational coherences to higher or lower rotational states. Time-dependent perturbation theory calculations verify the magnitudes and directions of the enhancement as a function of the applied chirp. The quantitative calculations and experimental results demonstrate that excitation with chirped pulses is an effective method for enhancing specific rotational coherences involving higher or lower rotational states.
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