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Far-infrared spectroscopy has been performed on [Fe(2-picolylamine)3]Cl2EtOH(Fe-pic) single crystals, to probe changes in the molecular vibrations upon thephotoinduced and temperature-induced spin crossovers. Synchrotron radiation hasbeen used as the farinfrared source to overcome the strong absorption and thesmall sizes of the samples. Absorption lines due to FeN6 cluster vibrations,observed below 400 cm-1, show strong intensity variations upon the crossoverdue to the deformation of FeN6 between high-spin and low-spin states. However,they remain almost unchanged between the photo- and temperature-inducedhigh-spin states. This is in sharp contrast to the lines at 500-700 cm-1 due tointramolecular vibrations of the picolylamine ligands, which show markedvariations between the two high-spin states. It is concluded that the mostimportant microscopic difference between the two high-spin states arises fromthe ligands, which is likely to reflect different states of intermolecularbonding between them.Comment: 10 pages, 4 figure

Photoinduced spin crossover in a Fe-picolylamine complex: A far-infrared study on single crystals