A 9.2-GHz clock transition in a Lu(II) molecular spin qubit arising from a 3,467-MHz hyperfine interaction
A 9.2-GHz clock transition in a Lu(II) molecular spin qubit arising from a 3,467-MHz hyperfine interaction
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DOI：
10.1038/s41557-022-00894-4
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发表时间：
2022-03-14
期刊：
影响因子：
21.8
通讯作者：
Hill, Stephen
中科院分区：
文献类型：
--
作者：
Kundu, Krishnendu;White, Jessica R. K.;Hill, Stephen
分子中的自旋是下一代量子技术特别有吸引力的目标，使化学可编程量子位和通过自组装扩大规模的潜力成为可能。在这里，我们报告了一个分子系统，A（iso）= 3，467 +/- 50 MHz，以及一个非常大的相关时钟跃迁的最大的超精细相互作用之一的观察。这是通过化学控制与一系列自旋1/2 La（II）和Lu（II）配合物相关的自旋轴承d轨道的s轨道混合程度来实现的。增加的s-轨道特征降低了自旋-轨道耦合，增强了电子-核费米接触相互作用。这两种结果都有利于量子应用。前者减少自旋晶格弛豫，后者最大限度地提高了超精细相互作用，这反过来又产生了9 GHz的时钟转换，导致相位记忆时间从1.0 +/- 0.4增加到12 +/- 1 μ s的一个Lu（II）配合物。这些发现为分子量子技术的发展提出了策略，类似于捕获离子系统。
Spins in molecules are particularly attractive targets for next-generation quantum technologies, enabling chemically programmable qubits and potential for scale-up via self-assembly. Here we report the observation of one of the largest hyperfine interactions for a molecular system, A(iso) = 3,467 +/- 50 MHz, as well as a very large associated clock transition. This is achieved through chemical control of the degree of s-orbital mixing into the spin-bearing d orbital associated with a series of spin-1/2 La(II) and Lu(II) complexes. Increased s-orbital character reduces spin-orbit coupling and enhances the electron-nuclear Fermi contact interaction. Both outcomes are advantageous for quantum applications. The former reduces spin-lattice relaxation, and the latter maximizes the hyperfine interaction, which, in turn, generates a 9-GHz clock transition, leading to an increase in phase memory time from 1.0 +/- 0.4 to 12 +/- 1 mu s for one of the Lu(II) complexes. These findings suggest strategies for the development of molecular quantum technologies, akin to trapped ion systems.