Eigenstate resolved infrared–infrared double-resonance study of intramolecular vibrational relaxation in benzene: First overtone of the CH stretch

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Abstract
The first eigenstate resolved, near the infrared spectrum of benzene in the region of the first C–H stretch overtone (6000 cm−1) has been obtained with an IR–IR double-resonance molecular beam optothermal spectrometer. Using a hierarchical tree analysis and level spacing statistics, we show that the intramolecular vibrational relaxation occurs nonergodically over at least seven different time scales ranging from 100 fs to 2 ns.

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