Abstract
The vibrational frequencies of the N−H stretching modes of aniline and diethylamine (DEA), after forming a strong H-bonded complex, are measured with infrared depletion spectroscopy that uses cluster-size-selective REMPI time-of-flight mass spectrometry. Three strong infrared absorption features observed at 3294, 3369, and 3473 cm-1 are assigned to the NH stretching vibration of DEA and H-bonded and free N−H stretching vibrations of aniline, respectively, in the 1:1 aniline−DEA complex. The spectral broadening observed for the free and H-bonded N−H stretching modes of aniline indicates mode-specific vibrational energy dynamics. Although the narrow bandwidth (≈4 cm-1) of the N−H stretch at 3473 cm-1 incorporates all of the common broadening mechanisms including intramolecular vibrational relaxation (IVR), the broader (≈13 cm-1) absorption feature at 3369 cm-1 suggests vibrational predissociation/IVR of the H-bonded complex, with a subpicosecond lifetime. The red-shifts of the N−H stretching vibrations of a...
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