Dispersion curves for the polyglycine I chain are calculated for both the in‐plane and out‐of‐plane modes of vibration, and the force constants are fitted by comparison with observed infrared frequencies. Frequency distributions for polyglycine I and polyglycine II are calculated from inelastic neutron scattering. The intensity difference of the C–N torsional band between polyglycine I and polyglycine II suggests the presence of additional C–H···O‐type hydrogen bonding between chains in the helical (II) form. An estimate of the sum of conformational and lattice energy difference in the two forms is made.

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