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SynopsisSolution-phase Raman spectra of diastereomeric alanyl dipeptides, BAla-L-Ala and L-Ala-L-Ala, and various mono-and dideuterated isotopomers in H, O and D,O, are reported. Spectral differences between the diastereomeric forms are interpreted, using the Raman analog of the coupled oscillator model, in terms of geometric differences between certain vibrations in the diastereomeric forms. Application of the coupledoscillator formalism allows the determination of a dihedral angle between the coupling vibrations. The results are compared with vibrational coupling employed by other workers in the determination of the vibrational spectra of peptides.