Trigonal Bipyramidal V3+ Complex as an Optically Addressable Molecular Qubit Candidate,Journal of the American Chemical Society

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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

Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States.
Pritzker School of Molecular Engineering, University of Chicago, Chicago, Illinois 60637, United States.
Institute for Terahertz Science and Technology, University of California, Santa Barbara, Santa Barbara, California 93106, United States.
Department of Physics, University of California, Santa Barbara, Santa Barbara, California 93106, United States.
The Institute for Sustainability and Energy at Northwestern, Northwestern University, Evanston, Illinois 60208, United States.
Department of Chemical Engineering, University of California, Santa Barbara, Santa Barbara, California 93106, United States.
Department of Chemistry and Biochemistry, University of California, Santa Barbara, Santa Barbara, California 93106, United States.
Department of Physics, University of Chicago, Chicago, Illinois 60637, United States.
Center for Molecular Engineering and Materials Science Division, Argonne National Laboratory, Lemont, Illinois 60439, United States.

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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