Picosecond fluorescence depletion spectroscopy. III. Intramolecular vibrational relaxation in the excited electronic state of p-cyclohexylaniline

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Abstract
This paper presents the results of the picosecond time‐resolved study of intramolecular vibrational relaxation (IVR) in the molecule p‐cyclohexylaniline. The results represent the second extensive study of a molecule using the technique which we have developed known as time‐resolved fluorescence depletion (TRFD). Fluorescence depletion decays and dispersed fluorescence spectra of 19 S 1 vibronic features are presented. The decays show a progression of dynamic behavior, including stationary behavior at low densities of states, quantum beating at intermediate densities, and fast decay of the initially prepared state at high state densities. The data allow us to assign IVR lifetimes which range from 250 ps at 820 cm− 1 of excess vibrational energy to 2.2 ps at 2362 cm− 1. Even at the highest frequencies we observe, the decays do not tend toward a simple exponential, but instead exhibit weak damped quantum beats.

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