Chemical tuning of spin clock transitions in molecular monomers based on nuclear spin-free Ni(II)

Abstract

We report the existence of a sizeable quantum tunnelling splitting between the two lowest electronic spin levels of mononuclear Ni complexes. The level anti-crossing, or magnetic clock transition, associated with this gap has been directly monitored by heat capacity experiments. The comparison of these results with those obtained for a Co derivative, for which tunnelling is forbidden by symmetry, shows that the clock transition leads to an effective suppression of intermolecular spin-spin interactions. In addition, we show that the quantum tunnelling splitting admits a chemical tuning via the modification of the ligand shell that determines the crystal field and the magnetic anisotropy. These properties are crucial to realize model spin qubits that combine the necessary resilience against decoherence, a proper interfacing with other qubits and with the control circuitry and the ability to initialize them by cooling.

arXiv comment22 pages, 11 figures and supplemental information

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Cited by in corpus (6)

• A perspective on scaling up quantum computation with molecular spins
• Electrical two-qubit gates within a pair of clock-qubit magnetic molecules
• Clock Transitions Guard Against Spin Decoherence in Singlet Fission
• Computational Insights into Electronic Excitations, Spin-Orbit Coupling Effects, and Spin Decoherence in Cr(IV)-based Molecular Qubits
• Enhancing Coherence with a Clock Transition and Dynamical Decoupling in the Cr${}_7$Mn Molecular Nanomagnet
• Floquet Engineering Clock Transitions in Magnetic Molecules