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We report on the mixed-orbital ground state compounds analogous to themixed-valence ones. Orbital doublet and singlet ground states of the Fe2+ iondisplayed in Moessbauer spectra of the Prussian blue analoguesAyFe3-y[Co(CN)6]2xH2O (y<1) are interconverting to each other as temperaturechanges for A = K, Na. Relative weight of orbital singlet ground statesincreases with lowering temperature. In the alcali-free cobalticyanides, theMoessbauer spectra are dominated by quadrupole-splt doublets of the same originwith a large splitting characteristic of the Fe2+ species coordinated by two(at least) oxygen atoms of water molecules in cis-configuration. Single typeoctahedral coordination of Fe2+ is isolated in A-filled cobalticyanides forA=Rb, Cs to be characterized by the narrower quadrupole spectrum associatedwith the orbital doublet ground states. Ionic exchange of K for Cs inKFe[Co(CN)6]H2O results in predominance of the orbital singlet, i.e., inenhanced anisotropy of the Fe2+ valence electrons. We found hence that the Fe2+charge distribution can be modified together with crystal size at the step ofsynthesis owing to distortion isomerism.

Mixed Orbital Ground States of Fe2+ in Prussian Blues