| Abstract
| - Three pulse infrared nonlinear studies with 100 fs pulses at 3 μm of the N−H mode of pyrrole in carbontetrachloride were carried out in various experimental configurations including integrated transient gratings,polarized pump−probe, heterodyned three pulse echoes, and time integrated three pulse echoes. Essentialfeatures of the N−H dynamics were obtained from the measured properties that include the population relaxationtime (T1 = 81 ± 15 ps), the orientational diffusion coefficients (D⊥ = (9.18 ± 1.09) × 1010 s-1, D∥ = (3.23± 0.71) × 1011 s-1), and the N−H vibrational frequency correlation function expressed as a sum of threeexponentials with correlation times 18 fs, 4.4 ps, and >10 ps.
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