Three-pulse scattering for femtosecond dephasing studies: theory and experiment

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Abstract
A novel transient three-pulse scattering technique for measuring ultrafast dephasing times in condensed matter is analyzed using a perturbative solution of the density matrix equation. The advantages of this technique include subpulsewidth resolution, a clear distinction between homogeneous and inhomogeneous broadening, and sensitivity to spectral cross-relaxation. Its application to the case of a multilevel resonance is also considered. We report results of femtosecond dephasing experiments with dye molecules in liquids and in a polymer host. The dephasing time is determined to be less than 20 fsec for dyes in solution at room temperature. At low temperatures in polymers, a transition from homogeneous to inhomogeneous broadening has been observed and studied as a function of temperature.

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