Consequences of a Linear Two-Coordinate Geometry for the Orbital Magnetism and Jahn-Teller Distortion Behavior of the High Spin Iron(II) Complex Fe[N(t-Bu)2]2

Mossbauer, EPR, magnetic susceptibility, and DFT studies of the unusual two-coordinate iron(II) amide Fe[N(t-Bu)(2)](2) show that it retains a linear N-Fe-N framework due to the nonbonding delta nature of the (xy, x(2)-y(2)) orbitals. The resulting near-degenerate ground state gives rise to a large magnetic moment and a remarkably large internal hyperfine field. The results confirm that extraordinary orbital magnetic effects can arise in linear transition metal complexes in which orbital degeneracies are not broken by Jahn-Teller or Renner-Teller distortions.