These calculations indicate that despite the bent molecular geometry, a strong crystal field is imposed by the two bound amides, and that the transverse field imposed by the tethered alkene does not significantly diminish this (Figure ). This is evidenced by a large splitting of the electronic states, an essentially pure maximal mJ = ±15/2 Kramers doublet ground state with Ising-like magnetic anisotropy (gx = gy = 0, gz = 19.9), and relatively high purities of the excited states (Table ). Single-phonon magnetic relaxation is expected to proceed over a barrier formed by the third excited mJ state (where gx, gy > 1, 1749 cm -1 above the ground state, 85% mJ = ±7/2, 29° between excited gz and ground gz)