Origin of unique hyper-Raman signals of trifluoroethanol.

We report the hyper-Raman (HR) spectrum of trifluoroethanol, excited with 532 nm light, in an aqueous solution at basic pH. The HR spectrum exhibits a distinct spectral pattern that diverges entirely from the infrared and Raman spectra of trifluoroethanol. This observed unique HR signal was attributed to the products of photoinduced radical reactions in the aqueous solution. This result exemplifies the exceptional capabilities of HR spectroscopy based on resonance conditions.