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World Scientific series in 20th century chemistry

Optical Molecular Dephasing: Principles of and Probings by Coherent Laser Spectroscopy

Ahmed H. Zewail

Published Sep 1, 1994• 1 citation
Publisher
DOI
10.1142/9789814287616_0019

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The noise tenaciously appearing in the optically heterodyne detected (OHD) transient optical Kerr effect (OKE) o f simple molecular liquids is investigated. We show that, for liquid samples of interest to us, coherent coupling does exist and appears as noise when not properly resolved. The strength of coherent coupling relative to the OKE depends critically on the sample position, with respect to the beam waist of the probe laser, as well as the angle subtended by the pump and probe beams. When the optics alignment is optimized for the OKE against coherent coupling the OHD-OKE signal is found to increase linearly with the local oscillator strength; the coherent coupling signal also appears to increase though the trend is not clear-cut. PACS. 42.50.Md- Optical transient phenomena: quantum beats, photon echo, freeinduction decay, dephasings and revivals, optical nutation, and self-induced transparency. PACS. 78.47.+p- Time-resolved optical spectroscopies and other ultrafast optical measurements in condensed matter. I.
Coherent optical phenomena such as the optical Stark effect, Rabi flopping, photon echo and quantum beating which are well-known in atomic spectroscopy can also be observed in semiconductors by using femtosecond laser pulses. On these short time scales, the quantum coherence of the optical excitations in the solid do not only influence the optical properties but change at the same time the relaxation and dephasing kinetics. The quasi-classical Boltzmann kinetics has to be replaced by quantum kinetics. Coherence leads to the appearance of memory in the scattering integrals. For femtosecond four-wave mixing and pump-and-probe spectroscopy the use of quantum kinetics for LO-phonon and for carrier-carrier scattering will be reviewed.