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Manipulation of ro-vibronic wave packet composition using chirped ultrafast laser pulses

Eliza-Beth W Lerch, Xingcan Dai1, Elva A Torres2, Joshua B Ballard3, Hans U Stauffer4 and Stephen R Leone

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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.


PACS

33.20.Vq Vibration-rotation analysis

33.15.Mt Rotation, vibration, and vibration-rotation constants

33.20.Sn Rotational analysis

33.80.Wz Other multiphoton processes

42.50.Md Optical transient phenomena: quantum beats, photon echo, free-induction decay, dephasings and revivals, optical nutation, and self-induced transparency

31.15.xp Perturbation theory

Subjects

Atomic and molecular physics

Computational physics

Optics, quantum optics and lasers

Dates

Issue 7 (14 April 2008)

Received 21 September 2007, in final form 7 December 2007

Published 25 March 2008



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