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The activation of methanol (CD 3 OD and CD 3 OH) by small cationic gold clusters has been investigated via infrared multiphoton dissociation (IR-MPD) spectroscopy in the 615–1760 cm −1  frequency range. The C–O stretch mode around 925 cm −1  and a coupled CD 3  deformation/C–O stretch mode around 1085 cm −1  are identified to be sensitive to the interaction between methanol and the gold clusters, whereas all other modes in the investigated spectral region remain unaffected. Based on the spectral shift of these modes, the largest C–O bond activation is observed for the mono-gold Au(CD 3 OD) +  cluster. This activation decreases with increasing the cluster size (number of gold atoms) and the number of adsorbed methanol molecules. Supporting density functional theory (DFT) calculations reveal that the C–O bond activation is caused by a methanol to gold charge donation, whereas the C–D and O–D bonds are not significantly activated by this process. The results are discussed with respect to previous experimental and theoretical investigations of neutral and cationic gold-methanol complexes focusing on the C–O stretch mode.

Methanol C–O Bond Activation by Free Gold Clusters Probed via Infrared Photodissociation Spectroscopy