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Engineering Clock Transitions in Molecular Lanthanide Complexes
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DOI：10.1021/jacs.3c09353.png)
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Molecular lanthanide (Ln) complexes are promising candidates for the development of next-generation quantum technologies. High-symmetry structures incorporating integer spin Ln ions can give rise to well-isolated crystal field quasi-doublet ground states, i.e., quantum two-level systems that may serve as the basis for magnetic qubits. Recent work has shown that symmetry lowering of the coordination environment around the Ln ion can produce an avoided crossing or clock transition within the ground doublet, leading to significantly enhanced coherence. Here, we employ single-crystal high-frequency electron paramagnetic resonance spectroscopy and high-level ab initio calculations to carry out a detailed investigation of the nine-coordinate complexes, [(HoL1L2)-L-III], where L-1 = 1,4,7,10-tetrakis(2-pyridylmethyl)-1,4,7,10-tetraaza-cyclododecane and L-2 = F- (1) or [MeCN](0) (2). The pseudo-4-fold symmetry imposed by the neutral organic ligand scaffold (L-1) and the apical anionic fluoride ion generates a strong axial anisotropy with an m(J) = +/- 8 ground-state quasi-doublet in 1, where m J denotes the projection of the J = 8 spin-orbital moment onto the similar to C-4 axis. Meanwhile, off-diagonal crystal field interactions give rise to a giant 116.4 +/- 1.0 GHz clock transition within this doublet. We then demonstrate targeted crystal field engineering of the clock transition by replacing F- with neutral MeCN (2), resulting in an increase in the clock transition frequency by a factor of 2.2. The experimental results are in broad agreement with quantum chemical calculations. This tunability is highly desirable because decoherence caused by second-order sensitivity to magnetic noise scales inversely with the clock transition frequency.
Keyword:
STATE PERTURBATION-THEORY
BASIS-SETS
HIGH-SYMMETRY
QUANTUM
VALENCE
MAGNETS
IMPLEMENTATION
DESIGN
FAMILY
EPR
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15.6
论文数:
20.0W
被引数:
60.2W
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