Coherent Spin Dynamics in Molecular Cr₈Zn Wheels

Controlling and understanding transitions between molecular spin states allows selection of the most suitable ones for qubit encoding. Here we present a detailed investigation of single crystals of a polynuclear Cr₈Zn molecular wheel using 241 GHz electron paramagnetic resonance (EPR) spectroscopy in high magnetic field. Continuous wave spectra are well reproduced by spin Hamiltonian calculations, which evidence that transitions in correspondence to a well-defined anticrossing involve mixed states with different total spin. We studied, by means of spin echo experiments, the temperature dependence of the dephasing time (<i>T</i>₂) down to 1.35 K. These results are reproduced by considering both hyperfine and intermolecular dipolar interactions, evidencing that the dipolar contribution is completely suppressed at the lowest temperature. Overall, these results shed light on the effects of the decoherence mechanisms, whose understanding is crucial to exploit chemically engineered molecular states as a resource for quantum information processing