With the study of three specific molecules, Na3(C2E"), HCN(X 'Z'), and 03(D'B2), each showing a distinctly different dynamical behavior at the energies studied, we show how techniques of nonlinear classical mechanics can be applied to simulate low resolution vibrational spectra and to extract the underlying dynamics from them. Particularly the importance of the single unstable periodic orbits in the chaotic regions of phase space is demonstrated.