Trigonal bipyramidal V3+ complex as an optically addressable molecular qubit candidate

Fataftah, M. S. et al. (2020) Trigonal bipyramidal V3+ complex as an optically addressable molecular qubit candidate. Journal of the American Chemical Society, 142(48), pp. 20400-20408. (doi: 10.1021/jacs.0c08986) (PMID:33210910)

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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.

Item Type:Articles
Additional Information:We acknowledge funding from ONR N00014-17-1-3026, the MRSEC Shared User Facilities at the University of Chicago (NSF DMR-1420709), NSF-DMR1906325, and the University of California Office of the President Multicampus Research Programs and Initiatives under Grant MRI-19-601107 for the ITST Terahertz Facilities, which have been upgraded with funds from NSF DMR1126894 and NSF-DMR-1626681.
Glasgow Author(s) Enlighten ID:Bayliss, Dr Sam
Authors: Fataftah, M. S., Bayliss, S. L., Laorenza, D. W., Wang, X., Phelan, B. T., Blake Wilson, C., Mintun, P. J., Kovos, B. D., Wasielewski, M. R., Han, S., Sherwin, M. S., Awschalom, D. D., and Freedman, D. E.
College/School:College of Science and Engineering > School of Engineering > Electronics and Nanoscale Engineering
Journal Name:Journal of the American Chemical Society
Publisher:American Chemical Society
ISSN (Online):1520-5126
Published Online:19 November 2020

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