Infrared spectra of one-monolayer Langmuir-Blodgett (LB) films of chlorophyll-<i>a</i> (Chl-<i>a</i>) can be obtained with a high signal-to-noise ratio by using the attenuated total reflection (ATR) technique. The observed spectra indicate that Chl-<i>a</i> assumes a five-coordinated monomer in the LB films; it seems that both the ester and keto C=O groups are free from any interactions, and a water molecule coordinates to the Mg atom. Comparison of the spectra of the one-monolayer LB films with those of the cast films shows that the structure of Chl-<i>a</i> is quite different between the two kinds of films; in contrast to the LB films the cast films are liable to have the dimer or oligomer of Chl-<i>a</i>. The fact that the five-coordinated monomer is predominant in the LB films suggests that Chl-<i>a</i> molecules are highly oriented in the one-monolayer LB films.

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