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Quantum Electronics and Laser Science Conference

Measurement of coherent photon-phonon interaction in solids using the deflection of femtosecond laser pulses

Harald Schulz, F. Kohns, Andreas Scheidt, Ping Zhou

Published Jun 7, 1996• 0 citations
OpenAlex

Abstract

Summary form only given. An amplified pulse of a Ti:sapphire femtosecond laser was split into an intense pump and a weak probe pulse. The delay time 7 between pump and probe pulse was adjusted from 0-50 ps in steps of 10 fs. The interaction volume given by the spatial overlap of pump and probe was in the bulk of the sample. Amorphous samples of glass and different single crystals with a typical thickness of 1 mm were used. Measurements with experimental setup A showed a beam scattering according to the degenerate four wave mixing (DFWM) process with fixed scattering angle, independent of the pump pulse intensity and delay time.

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Summary form only given. An amplified pulse of a Ti:sapphire femtosecond laser was split into an intense pump and a weak probe pulse. The delay time 7 between pump and probe pulse was adjusted from 0-50 ps in steps of 10 fs. The interaction volume given by the spatial overlap of pump and probe was in the bulk of the sample. Amorphous samples of glass and different single crystals with a typical thickness of 1 mm were used. Measurements with experimental setup A showed a beam scattering according to the degenerate four wave mixing (DFWM) process with fixed scattering angle, independent of the pump pulse intensity and delay time.
Summary form only given.We report on a general approach to coherent control in semiconductors, based on optical waveforms with synthesized intensity and phase versus time. This technique is limited only by the bandwidth of the initial laser pulses and the spectral resolution of the pulse-shaping apparatus. It is therefore especially suitable to investigate effects such as off-resonant Rabi oscillations and polaritons in multiple quantum wells. Experiments were performed in four-wave mixing (FWM) and differential reflection geometry based on a mode-locked Ti:sapphire laser emitting 100-fs pulses.
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.
The delayed or time-domain four-wave-mixing experiment is treated in the regime of intense near-resonant pulses. The interaction with the radiation during both pump and probe pulses is considered to all powers of the electric field amplitude. Analytical results are obtained for an effective four-level system. These include the dependence of the coherence amplitudes on the ratio of the pump-field intensities when there is a large vibrational discrepancy between ground and excited electronic states and a general solution for the unitary time development during the probe pulse. For the first time, delayed coherent anti-Stokes Raman scattering is detected from highly dilute (10-ppm) guest molecules. Illustrative examples are presented for the system of pentacene in benzoic acid at low temperature. Vibronic-free induction decay and the effect of field inhomogeneity across the beam profile are found to be essential for understanding the observed intensity and spectral distribution of the signal beam in the region of optimum pulse intensity.