Ultrafast liquid dynamics studied by third and fifth order three pulse photon echoes

We report a new spectroscopic measurement based on fifth order nonlinear response from a molecule in a room temperature liquid. In conjunction with conventional three pulse stimulated photon echo, detailed information on solvent–solute dynamics for a wide range of time scales has been obtained. Both the ultrafast inertial components and much slower dynamics of the solvent are found to make important contributions to the solvent relaxation. The potential of the fifth order measurements is discussed via numerical calculations using model solvent spectral densities.

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