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The four-coordinate iron(II) phosphoraniminato complex PhB(MesIm)₃Fe−NPPh₃ undergoes an S = 0 to S = 2 spin transition with T_C = 81 K, as determined by variable-temperature magnetic measurements and Mössbauer spectroscopy. Variable-temperature single-crystal X-ray diffraction revealed that the S = 0 to S = 2 transition is associated with an increase in the Fe−C and Fe−N bond distances and a decrease in the N−P bond distance. These structural changes have been interpreted in terms of electronic structure theory.