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Chemical Physics Letters

Photon echo pulse sequences with femtosecond shaped laser pulses as a vehicle for molecule-based quantum computation

Vadim V. Lozovoy, Marcos M. Dantus

Published Jan 1, 2002• 21 citations
Publisher
DOI
10.1016/s0009-2614(01)01388-4

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State‐to‐State Collisional Dynamics by Coherent Laser Pulse Phase, Shape, and Frequency Modification

Mark A. Banash, Warren S. Warren

Conventional coherent pulse sequences such as photon echoes measure only highly averaged relaxation rates in complex multilevel systems, such as molecules undergoing state‐changing collisions. Pulse frequency, phase, and shape control lets us generate sequences which give a more detailed understanding of the dynamics. Results of dual frequency, crafted shape sequences on I2 are presented which show that the "coherence dephasing" time T2 is primarily due to population redistribution (energy changing collisions) in the electronically excited state, and that the electronic ground state has a much smaller cross section for such collisions. Quantitative analysis is only possible with modified laser pulse shapes which excite a single velocity component, and requires pulse sequences which correct for the hyperfine dependence of predissociation. Since this correction is rarely made in previously reported coherent transient measurements, literature values of T2 and T1 may not be reliable in the zero pressure limit.

Laser Chemistry•Jan 1, 1986•11 citations
We report on a physical mechanism of coherent control with intense shaped femtosecond laser pulses. We study photoelectron spectra from multi-photon ionization of potassium atoms and dimers using tailored femtosecond laser pulses. Our results are interpreted in terms of Selective Population of Dressed States (SPODS). Two realizations of SPODS by Photon Locking (PL) via pulse sequences and Rapid Adiabatic Passage (RAP) via chirped pulses are discussed. New physical mechanisms arise, when both PL and RAP are at play simultaneously. Control by the combined effect of PL and RAP is studied by mapping out a two-parameter Quantum Control Landscape (QCL) for selective population of dressed states.
Femtosecond photon echos in semiconductors are studied on the basis of a stochastic description of the polarization decay. A satisfactory agreement with experimental results [ Phys. Rev. Lett.61, 1647 ( 1988)] is found with respect to the nonexponential decay of the echo energy as a function of the time delay between the laser pulses. Moreover, the shape of the echo is studied, and the detuning of the laser frequency with respect to the band edge is found to depend significantly on the shape of the light pulses.
Conventional coherent pulse sequences such as photon echoes measure only highly averaged relaxation rates in complex multilevel systems, such as molecules undergoing state‐changing collisions. Pulse frequency, phase, and shape control lets us generate sequences which give a more detailed understanding of the dynamics. Results of dual frequency, crafted shape sequences on I2 are presented which show that the "coherence dephasing" time T2 is primarily due to population redistribution (energy changing collisions) in the electronically excited state, and that the electronic ground state has a much smaller cross section for such collisions. Quantitative analysis is only possible with modified laser pulse shapes which excite a single velocity component, and requires pulse sequences which correct for the hyperfine dependence of predissociation. Since this correction is rarely made in previously reported coherent transient measurements, literature values of T2 and T1 may not be reliable in the zero pressure limit.