Line-narrowing transient Raman technique which resolves closely spaced hydrogen-bonded aggregates

An ultrafast coherent Raman spectroscopy with tunable excitation is presented. It is applied to the analysis of vibrational spectra of hydrogen-bonded aggregates of pyridine and methanol. Whereas the spontaneous Raman spectrum exhibits a broad and featureless band, the line-narrowed spectra reveal three distinct lines. The concentration dependence of these lines suggests an assignment to well-defined aggregates of different sizes.