Spin coherence and magnetization dynamics of TMA[KCoFe(CN)] toward coordination-framework spin qubits.

Metal compounds with = 1/2 coordination-frameworks have been emerging as new powerful qubit candidates. In this study, we have reported the CN-based coordination framework TMA[KCoFe(CN)] to be a qubit. We explored the magnetization dynamics and spin coherence of the magnetic dilution of the = 1/2 Fe(III) complex TMA[KFe(CN)] (TMA = tetramethylammonium) in its Co(III)-based diamagnetic analogue TMA[KCo(CN)]. Alternating-current (AC) susceptibility data illustrate a slow magnetic relaxation upon applying a field of 0.1 T, which follows the phonon-bottleneck relaxation mechanism along with the Raman process. A magnetic relaxation time () of 0.3 s (2% Fe) was realized at 1.8 K. Moreover, pulsed EPR data reveal a coherence duration of 1 μs (0.1% Fe) at 4 K with successful observation of Rabi oscillation at 4 K and 13 K (2% Fe) using MW pulses with variable irradiation-field strengths. The overall results indicate that TMA[KCoFe(CN)] represents a promising qubit candidate, as it is capable of being placed in any superposition of the two distinct states ( = +1/2 and = -1/2).