The infrared spectra of γ‐aminobutyric acid (GABA) in the solid state and inert gas matrices at several temperatures and concentrations have been analyzed. Evidence of a neutral molecular form of GABA is shown for the first time; this compound was known until now only in its zwitterionic or cationic forms. The intermolecular mechanism is also established for the formation of the GABA zwitterion. This final step is shown to be preceeded by hydrogen‐bonded intermediates.

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