Applications of Ionic liquids have become common in radiolytic environments such as solar cells and nuclear reactors. The photodetachment of an electron from an ion in the liquid creates an initially delocalized and highly reactive species that subsequently localizes to a cavity in less than a picosecond. This is followed by relaxation and cooling that spans decades in time. We apply pump-probe spectroscopy to quantify the reactivity and localization time scales. In order to gain more detailed insight into the structure of the excess electron we apply resonance enhanced femtosecond stimulated Raman spectroscopy (FSRS) to probe the structure and dynamics following photo-detachment in aliphatic ionic liquids. The results will be discussed in the context of the molecular structure of solvated electrons in these liquids and how that structure evolves during localization and solvation. The figure provides an example of time-resolved resonance Raman spectroscopy of the electrons following photodetachment at 266 nm from a pyrrolidinium dicyanamide ionic liquid (molecular structure shown at the right).

Time resolved nonlinear spectroscopy of excess electrons in aliphatic ionic liquids

ACS Fall 2021

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