Tunable Cr4+ Molecular Color Centers,Journal of the American Chemical Society

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Tunable Cr4+ Molecular Color Centers
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2021-11-24 , DOI: 10.1021/jacs.1c10145
Daniel W Laorenza _{1,

2} , Arailym Kairalapova ₃ , Sam L Bayliss ₄ , Tamar Goldzak ₃ , Samuel M Greene ₃ , Leah R Weiss ₄ , Pratiti Deb _{4,

5} , Peter J Mintun ₄ , Kelsey A Collins ₂ , David D Awschalom _{4,

5,

6} , Timothy C Berkelbach _{3,

7} , Danna E Freedman _{1,

2}

Affiliation

The inherent atomistic precision of synthetic chemistry enables bottom-up structural control over quantum bits, or qubits, for quantum technologies. Tuning paramagnetic molecular qubits that feature optical-spin initialization and readout is a crucial step toward designing bespoke qubits for applications in quantum sensing, networking, and computing. Here, we demonstrate that the electronic structure that enables optical-spin initialization and readout for S = 1, Cr(aryl)₄, where aryl = 2,4-dimethylphenyl (1), o-tolyl (2), and 2,3-dimethylphenyl (3), is readily translated into Cr(alkyl)₄ compounds, where alkyl = 2,2,2-triphenylethyl (4), (trimethylsilyl)methyl (5), and cyclohexyl (6). The small ground state zero field splitting values (<5 GHz) for 1–6 allowed for coherent spin manipulation at X-band microwave frequency, enabling temperature-, concentration-, and orientation-dependent investigations of the spin dynamics. Electronic absorption and emission spectroscopy confirmed the desired electronic structures for 4–6, which exhibit photoluminescence from 897 to 923 nm, while theoretical calculations elucidated the varied bonding interactions of the aryl and alkyl Cr⁴⁺ compounds. The combined experimental and theoretical comparison of Cr(aryl)₄ and Cr(alkyl)₄ systems illustrates the impact of the ligand field on both the ground state spin structure and excited state manifold, laying the groundwork for the design of structurally precise optically addressable molecular qubits.

中文翻译：

可调 Cr4+ 分子色心

合成化学固有的原子精度使量子技术能够对量子比特或量子比特进行自下而上的结构控制。调整具有光学自旋初始化和读出功能的顺磁性分子量子位是设计用于量子传感、网络和计算应用的定制量子位的关键一步。在这里，我们证明了能够实现S = 1、Cr(aryl) ₄的光学自旋初始化和读出的电子结构，其中芳基 = 2,4-二甲基苯基 ( 1 )、邻甲苯基 ( 2 ) 和 2,3 -二甲基苯基 ( 3 ) 很容易转化为 Cr(烷基) ₄化合物，其中烷基 = 2,2,2-三苯乙基 ( 4)、(三甲基甲硅烷基)甲基( 5 )和环己基( 6 )。1 – 6的小基态零场分裂值 (<5 GHz)允许在 X 波段微波频率下进行相干自旋操作，从而能够对自旋动力学进行温度、浓度和方向相关的研究。电子吸收和发射光谱证实了4 – 6所需的电子结构，其表现出 897 至 923 nm 的光致发光，而理论计算阐明了芳基和烷基 Cr ⁴⁺化合物的不同键合相互作用。_{Cr(aryl) 4}和 Cr(alkyl)的组合实验和理论比较_图4系统说明了配体场对基态自旋结构和激发态流形的影响，为设计结构精确的光学可寻址分子量子比特奠定了基础。

更新日期：2021-12-22

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