基于核自旋自由Ni（II）的分子单体中自旋钟跃迁的化学调谐
Chemical tuning of spin clock transitions in molecular monomers based on nuclear spin-free Ni(II)
摘要：
我们报告了单核镍配合物的两个最低电子自旋能级之间存在相当大的量子隧穿分裂。与此间隙相关的水平反交叉或磁钟跃迁已通过热容实验直接监测。这些结果的比较与那些获得的Co衍生物，隧道是禁止对称性，表明时钟过渡导致有效抑制分子间自旋-自旋相互作用。此外，我们表明，量子隧穿分裂承认化学调谐通过修改的配体壳，确定的晶体场和磁各向异性。这些特性对于实现模型自旋量子比特至关重要，这些模型自旋量子比特结合了对退相干的必要弹性，与其他量子比特和控制电路的适当接口以及通过冷却来初始化它们的能力。
英文摘要：
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.
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