Vibrationally energized molecules: Unimolecular energy flow, chaos, and level specific chemistry

The goal has been to develop experimental and theoretical methods capable of characterizing the structure and dynamics of molecules undergoing large amplitude vibrational motions and/or chaotic dynamics. Progress was made toward this goal using the Stimulated Emission Pumping technique combined with statistical pattern-recognition schemes. The SEP study of HCP samples the HCP HPC isomerization barrier. Three statistical pattern recognition techniques - Statistical Fourier Transform, Spectral Cross-Correlation, and Extended Autocorrelation, were developed and applied to experimental and computed spectra of HCN, HCP, acetylene, and NO2.