Ultrafast dichroism spectroscopy of anthracene in solution. II. Solvation dynamics from a one-dimensional experiment

Experiments to determine the frequency autocorrelation function of an elect ronic transition (the "solvation function") inherently depend on a multidim ensional response function. However, a degenerate transient absorption expe riment, or "single-wave length transient hole burning" (SW-THB), provides a one-dimensional cut through this multidimensional space with sufficient in formation to uniquely determine the desired solvation function. We derive a n analytical formula that relates the solvation function to the one-dimensi onal SW-THB signal. Sample calculations examine the effects of strong versu s weak coupling to the solvent, the wavelength of the laser relative to the absorption spectrum and of unresolved fast relaxation components. We concl ude that for many systems, SW-THB provides a simpler alternative to multidi mensional methods for measuring solvation dynamics. (C) 2001 American Insti tute of Physics.