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Chemical Physics Letters

Phase-dependent absorption and stimulated emission in femtosecond pump-probe experiments

Benjamin Fain, S. H. Lin

Published May 1, 1993• 17 citations
Publisher
DOI
10.1016/0009-2614(93)89002-y

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In ultrashort (femtosecond) pump-probe spectroscopy, the pump pulse creates a nonstationary medium while the probe pulse propagates in such a medium. The analysis of this situation is performed in the framework of linear nonstationary optics. Constitutive equations and electrodynamics of the nonstationary media are analyzed. The propagation of the probe-pulse energy is characterized by the coarse-grained susceptibility introduced in the previous works of the authors [S. H. Lin and B. Fain, Chem. Phys. Lett. 157, 233 (1989); B. Fain, S. H. Lin, and N. Hamer, J. Chem. Phys. 91, 4485 (1989); B. Fain and S. H. Lin, Chem. Phys. 161, 515 (1992)]. The main objective of the paper is the derivation and analysis of the delay-time-dependent absorption and dispersion line shapes of the probe pulse. This line shape has a very specific form corresponding to phase-dependent Raman absorption (emission). The latter phenomenon is introduced and described in the present paper.

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Ralf Brinkmann, W. Sohler, H. Suche

We report Erbium-doped Ti-indiffused single-mode optical waveguides of good quality in LiNbO3 fabricated by Erimplantation followed by annealing. Besides ground state absorption also xcited-tate-bsorption (ESA) has been investigated indicating that even at 1. 48 pm pump wavelength ESA occurs as a three stage process. The guided-wave spontaneous fluorescence was investigated. In a " pump and probe" experiment for the first time wavelength ranges could be identified where the stimulated emission overcomes the Er-absorption.

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Feb 1, 1991•13 citations
In ultrashort (femtosecond) pump-probe spectroscopy, the pump pulse creates a nonstationary medium while the probe pulse propagates in such a medium. The analysis of this situation is performed in the framework of linear nonstationary optics. Constitutive equations and electrodynamics of the nonstationary media are analyzed. The propagation of the probe-pulse energy is characterized by the coarse-grained susceptibility introduced in the previous works of the authors [S. H. Lin and B. Fain, Chem. Phys. Lett. 157, 233 (1989); B. Fain, S. H. Lin, and N. Hamer, J. Chem. Phys. 91, 4485 (1989); B. Fain and S. H. Lin, Chem. Phys. 161, 515 (1992)]. The main objective of the paper is the derivation and analysis of the delay-time-dependent absorption and dispersion line shapes of the probe pulse. This line shape has a very specific form corresponding to phase-dependent Raman absorption (emission). The latter phenomenon is introduced and described in the present paper.
Controlling stimulated emission is of importance because it competes with absorption and fluorescence under intense laser excitation. We performed resonant nonlinear optical spectroscopy measurements using femtosecond pulses shaped by π- or π/2-step phase functions and carried out calculations based on density matrix representation to elucidate the experimental results. In addition, we compared enhancements obtained when using other pulse shaping functions (chirp, third-order dispersion, and a time-delayed probe). The light transmitted through the high optical density solution was dominated by an intense stimulated emission feature that was 14 times greater for shaped pulses than for transform limited pulses. Coherent enhancement depending on the frequency, temporal, and phase characteristics of the shaped pulse is responsible for the experimental observations.
We report Erbium-doped Ti-indiffused single-mode optical waveguides of good quality in LiNbO3 fabricated by Erimplantation followed by annealing. Besides ground state absorption also xcited-tate-bsorption (ESA) has been investigated indicating that even at 1. 48 pm pump wavelength ESA occurs as a three stage process. The guided-wave spontaneous fluorescence was investigated. In a " pump and probe" experiment for the first time wavelength ranges could be identified where the stimulated emission overcomes the Er-absorption.