Coherent control through near-resonant Raman transitions

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Xingcan Dai, Eliza-Beth W. Lerch, and Stephen R. Leone
Department of Chemistry and Department of Physics, and Lawrence Berkeley National Laboratory, University of California, Berkeley, California 94720, USA

Received 21 October 2005; published 6 February 2006

Thephase of an electronic wave function is shown to playan important role in coherent control experiments. By using apulse shaping system with a femtosecond laser, we explore thephase relationships among resonant and off-resonant Raman transitions in Li₂by measuring the phases of the resulting wave packets, orquantum beats. Specific pixels in a liquid-crystal spatial light modulatorare used to isolate the resonant and off-resonant portions ofthe Raman transitions in Li₂. The off-resonant Raman transitions havean approximately 90° phase shift with respect to the resonantRaman transition, and there is an approximately 180° phase shiftbetween the blue-detuned and the red-detuned off-resonant Raman transitions. Calculationsusing second-order time-dependent perturbation theory for the electronic transitions agreewith the experimental results for the laser pulse intensities usedhere. Interferences between the off-resonant Raman transitions as a functionof detuning are used to demonstrate coherent control of theRaman quantum wave packet.

URL:	http://link.aps.org/doi/10.1103/PhysRevA.73.023404
DOI:	10.1103/PhysRevA.73.023404
PACS:	42.50.Md; 33.80.Eh; 32.80.Qk; 82.53.Hn 42.50.Md Optical transient phenomena including quantum beats, photon echo, free-induction decay, dephasings and revivals, optical nutation, and self-induced transparency 33.80.Eh Autoionization, photoionization, and photodetachment of molecules 32.80.Qk Coherent control of atomic interactions with photons 82.53.Hn Pump probe experiments with bound states (femtochemistry) YEAR: 2006
KEYWORDS:	lithium, quantum optics, Raman spectra, perturbation theory, optical pulse shaping, spatial light modulators

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