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Trigonal Bipyramidal V3+ Complex as an Optically Addressable Molecular Qubit Candidate
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-11-19 , DOI: 10.1021/jacs.0c08986
Majed S Fataftah 1 , Sam L Bayliss 2 , Daniel W Laorenza 1 , Xiaoling Wang 3, 4 , Brian T Phelan 1, 5 , C Blake Wilson 3, 4 , Peter J Mintun 2 , Berk D Kovos 2 , Michael R Wasielewski 1, 5 , Songi Han 3, 6, 7 , Mark S Sherwin 3, 4 , David D Awschalom 2, 8, 9 , Danna E Freedman 1
Affiliation  

Synthetic chemistry enables a bottom-up approach to quantum information science, where atoms can be deterministically positioned in a quantum bit or qubit. Two key requirements to realize quantum technologies are qubit initialization and read-out. By imbuing molecular spins with optical initialization and readout mechanisms, analogous to solid-state defects, molecules could be integrated into existing quantum infrastructure. To mimic the electronic structure of optically addressable defect sites, we designed the spin-triplet, V3+ complex, (C6F5)3trenVCNtBu (1). We measured the static spin properties as well as the spin coherence time of 1 demonstrating coherent control of this spin qubit with a 240 GHz electron paramagnetic resonance spectrometer powered by a free electron laser. We found that 1 exhibited narrow, near-infrared photoluminescence (PL) from a spin-singlet excited state. Using variable magnetic field PL spectroscopy, we resolved emission into each of the ground-state spin sublevels, a crucial component for spin-selective optical initialization and readout. This work demonstrates that trigonally symmetric, heteroleptic V3+ complexes are candidates for optical spin addressability.

中文翻译:


三角双锥 V3+ 复合物作为光学可寻址分子量子位候选者



合成化学为量子信息科学提供了一种自下而上的方法,其中原子可以确定地定位在量子位或量子位中。实现量子技术的两个关键要求是量子位初始化和读出。通过为分子自旋注入光学初始化和读出机制(类似于固态缺陷),分子可以集成到现有的量子基础设施中。为了模拟光学可寻址缺陷位点的电子结构,我们设计了自旋三重态 V3+ 复合物 (C6F5)3trenVCNtBu (1)。我们测量了静态自旋特性以及 1 的自旋相干时间,证明了使用由自由电子激光器供电的 240 GHz 电子顺磁共振波谱仪对该自旋量子位的相干控制。我们发现1表现出来自自旋单重激发态的窄近红外光致发光(PL)。使用可变磁场 PL 光谱,我们将发射解析为每个基态自旋子能级,这是自旋选择性光学初始化和读出的关键组成部分。这项工作表明,三角对称杂配 V3+ 配合物是光学自旋寻址能力的候选者。
更新日期:2020-11-19
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