Abstract
Analysis of the Mossbauer hyperfine interaction data for the octahedral 3d(t2g5) FeIII complex in K3Co1-xFex(CN)6 results in a magnetic contact term of (HC/2S)=+255+or-5 kOe and an (r-3)m approximately 1.0 au for the 3d(t2g) wavefunction. A comparison with the corresponding theoretical free-ion values for Fe3+, -126 kOe and 5.7 au, discloses an extensive overall expansion of the 3d(t2g) wavefunction accompanied by a significant 4s participation in the bonding of the central transition metal ion. Similar results are obtained from the analysis of EPR data for the 3d(t2g5) electronic configuration in K4Fe1-xMnx(CN)6.3H2O. These results are in accord with the available EPR data for several octahedral covalent complexes of V4+, Cr5+ and Mo5+, which have the complementary electronic configurations 3d(t2g1) and 4d(t2g1). Supporting evidence is derived from the analysis of the quadrupole splitting, isomer shift and molecular vibrations in K3Fe(CN)6.
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