Inorganic Chemistry, Vol.54, No.24, 12027-12031, 2015
Qubit Control Limited by Spin-Lattice Relaxation in a Nuclear Spin-Free Iron(III) Complex
High-spin transition metal complexes are of interest as candidates for quantum information processing owing to the tunability of the pairs of M-S levels for use as quantum bits (qubits). Thus, the design of high-spin systems that afford qubits with stable superposition states is of primary importance. Nuclear spins are a potent instigator of superposition instability; thus, we probed the Ph4P+ salt of the nuclear spin-free complex [Fe(C5O5)(3)](3-) (1) to see if long-lived superpositions were possible in such a system. Continuous-wave and pulsed electron paramagnetic resonance (EPR) spectroscopic measurements reveal a strong EPR transition at X-band that can be utilized as a qubit. However, at 5 K the coherent lifetime, T-2, for this resonance is 721(3) ns and decreases rapidly with increasing temperature. Simultaneously, the spin-lattice relaxation time is extremely short, 11.33(1) mu s, at 5 K, and also rapidly decreases with increasing temperature. The coincidence of these two temperature-dependent data sets suggests that T-2 in 1 is strongly limited by the short T-1. Importantly, these results highlight the need for new design parameters in pursuit of high-spin species with appreciable coherence times.