Abstract
Three time‐revolved four‐wave mixing techniques for measuring orientational relaxation of molecules in solution are compared. A unified theoretical treatment of two‐pulse polarization spectroscopy and three‐pulse transient grating diffraction from both population and purely orientational gratings is developed by incorporating the slowly varying reorientation of the transition dipoles into the equations of motion for the density matrix elements. All three methods, as well as fluorescence polarization, yield the same experimental reorientation times. The practical advantages and limitations of these techniques and their applicability to the study of other dynamical processes are discussed.
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