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A vibrational analysis of various poly(o-aminophenol) structures has been undertaken using first principles methods. It is shown that a mixture of quinoid and keto forms of poly(o-aminophenol) gives rise to a simulated spectrum that replicates the experimental infrared spectra of plasma-produced poly(o-aminophenol) better than either the quinoid or keto poly(o-aminophenol) spectra alone. An unassigned peak in the spectrum is attributed to hydrogen bonding to the silica substrate.