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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Femtosecond photon echo as probe for ultrafast optical dephasing and optical band shape in condensed molecular systems

Игорь Сергеевич Осадько, M. V. Stashek

Published May 10, 1996• 0 citations
Publisher

Abstract

Femtosecond photon echo decay due to ultrafast optical dephasing in condensed molecular systems can be related to an impurity optical band shape. A relation is found and discussed.© (1996) COPYRIGHT SPIE--The International Society for Optical Engineering. Downloading of the abstract is permitted for personal use only.
DOI
10.1117/12.239470

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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.
A theory of optical echo spectroscopies of large polyatomic molecules in condensed phases is developed. Using phase space correlation functions, we examine the interrelationships among the following optical measurements: ordinary photon echo, stimulated photon echo, accumulated photon echo, incoherent accumulated photon echo, and pump–probe absorption. Conditions for the elimination of inhomogeneous broadening in these experiments are specified. A multimode Brownian oscillator model is used to account for high frequency molecular vibrations, as well as solvent modes, and electronic dephasing processes. The effects of quantum beats, spectral diffusion, and homogeneous dephasing on the echo signals are studied and compared in detail with pump–probe and hole burning spectroscopy.
Two pulse photon echoes were observed in organic dye molecules in solution using 6-fs optical pulses. The results show an initial rapid dephasing of the echo due to level multiplicity followed by quantum beaks. The temporal decay of the quantum beats is characterized by a T2{\mathrm{T}}_{2}T2​ of about 60 fs.