Measuring Ultrafast Spectral Diffusion and Correlation Dynamics by Two-Dimensional Electronic Spectroscopy

The frequency fluctuation correlation function (FFCF) measures the spectral diffusion of a state's transition while the frequency fluctuation cross-correlation function (FXCF) measures the correlation dynamics between the transitions of two separate states. These quantities contain a wealth of information on how the chromophores or excitonic states interact and couple with its environment and with each other. We summarize the experimental implementations and theoretical considerations of using two-dimensional electronic spectroscopy to characterize FFCFs and FXCFs. Applications can be found in systems such as the chlorophyll pigment molecules in light-harvesting complexes and CdSe nanomaterials.