Magnetization Dynamics and Coherent Spin Manipulation of a Propeller Gd(III) Complex with the Smallest Helicene Ligand

[Image: see text] A homoleptic gadolinium(III) complex with the smallest helicene-type ligand, 1,10-phenanthroline-N,N′-dioxide (phendo) [Gd(phendo)(4)](NO(3))(3)·xMeOH (phendo = 1,10-phenanthroline-N,N′-dioxide, MeOH = methanol), shows slow relaxation of the magnetization characteristic for Single Ion Magnets (SIM), despite negligible magnetic anisotropy, confirmed by ab initio calculations. Solid state dilution magnetic and EPR studies reveal that the magnetization dynamics of the [Gd(phendo)(4)](3+) cation is controlled mainly by a Raman process. Pulsed EPR experiments demonstrate long phase memory times (up to 2.7 μs at 5 K), enabling the detection of Rabi oscillations at 20 K, which confirms coherent control of its spin state.