Two-dimensional spectroscopic techniques are powerful tools for extracting information on the system-bath interactions. Different analysis procedures, such as the center line slope, slope of phase, ellipticity, and the inhomogeneity index, can be used to quantify line shape changes and the results can be related to the frequency fluctuation correlation function. Recently we demonstrated a method for extracting the dynamic Stokes shift from the two-dimensional electronic spectra which can also be related to the frequency fluctuation correlation function. Analyzing the dynamic Stokes shift function at different excitation frequencies we extract frequency dependent relaxation times. The fastest timescale is attributed to the solvent inertial response. Here we compare the correlation function from the extracted dynamic Stokes shift to that extracted from the analysis of the inhomogeneity index. We find that the fastest timescale extracted from the inhomogeneity index is consistent with that from the dynamic Stokes shift, corroborating the isolation of the ultrafast solvent response.

Extracting correlation functions from two-dimensional electronic spectra

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

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