Trigonal Bipyramidal V3+ Complex as an Optically Addressable Molecular Qubit Candidate

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 initializati...

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Bibliographic Details
Published in:Journal of the American Chemical Society 2020-12, Vol.142 (48), p.20400-20408
Main Authors: Fataftah, Majed S, Bayliss, Sam L, Laorenza, Daniel W, Wang, Xiaoling, Phelan, Brian T, Wilson, C. Blake, Mintun, Peter J, Kovos, Berk D, Wasielewski, Michael R, Han, Songi, Sherwin, Mark S, Awschalom, David D, Freedman, Danna E
Format: Article
Language:English
Subjects:
30 DIRECT ENERGY CONVERSION
defects
electron paramagnetic resonance spectroscopy
ligands
magnetic properties
PHYSICS OF ELEMENTARY PARTICLES AND FIELDS
quantum information science
quantum mechanics
spin qubits
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Summary: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)3trenVCN t Bu (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.
ISSN:0002-7863
1520-5126
DOI:10.1021/jacs.0c08986