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A highly epitaxial delafossite CuFe1-xGaxO2 film was made with pulse laser deposition in high vacuum. The sample thickness was around 48nm and it was terminated with CuFeO2. This delafossite sample was exposed to a CO2 atmosphere under controlled conditions and chemisorption of CO2 on the surface was observed. Transmittance and reflectance spectroscopies were recorded for the sample post surface heat treatment held in a vacuum chamber (0.05Kpa) and after exposure to CO2. Both spectra were recorded over a wavelength range of 350–1100nm. Chemisorption of CO2 was correlated with an increase in transmittance and decrease in reflectance in the pressure range 0–60kPa. These observations were confirmed with X-ray photoelectron spectroscopy and thermal programmed desorption data obtained in an independent experiment. The CO2 is bound to the surface forming a carboxylate structure via coordination of a bent CO2−δ molecule to a Cu center.