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

Majed S. Fataftah; Sam L. Bayliss; Daniel W. Laorenza; Xiaoling Wang; Brian T. Phelan; C. Blake Wilson; Peter J. Mintun; Berk D. Kovos; Michael R. Wasielewski; Songi Han; Mark S. Sherwin; David D. Awschalom; Danna E. Freedman

doi:10.1021/jacs.0c08986

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

Majed S. Fataftah, Sam L. Bayliss, Daniel W. Laorenza, Xiaoling Wang, Brian T. Phelan, C. Blake Wilson, Peter J. Mintun, Berk D. Kovos, Michael R. Wasielewski^*, Songi Han^*, Mark S. Sherwin^*, David D. Awschalom^*, Danna E. Freedman^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

54 Scopus citations

Abstract

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.

Original language	English (US)
Pages (from-to)	20400-20408
Number of pages	9
Journal	Journal of the American Chemical Society
Volume	142
Issue number	48
DOIs	https://doi.org/10.1021/jacs.0c08986
State	Published - Dec 2 2020

Funding

The authors thank Dr. Johan van Tol and Rebecca Sponenburg for experimental assistance. The authors acknowledge David Enyeart and Nickolay Agladze for maintaining, repairing, and assisting with operation of the UCSB FEL. This project was initiated with support for M.S.F. from National Science Foundation CAREER Award No. CHE-1455017 to investigate fundamentals of coherence time and continued through support from DE-SC0019356 (D.E.F., D.W.L., B.T.P., and M.R.W) to develop molecules that interface with existing quantum infrastructure. We acknowledge funding from ONR N00014-17-1-3026, the MRSEC Shared User Facilities at the University of Chicago (NSF DMR-1420709), NSF-DMR-1906325, 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 DMR-1126894 and NSF-DMR-1626681. Experimental work was supported by the MRSEC Shared User Facilities at the University of Chicago (NSF DMR-1420709), IMSERC at Northwestern University, which has received support from Northwestern University, the State of Illinois, and the Int. Institute of Nanotechnology. A portion of this work was performed at the National High Magnetic Field Laboratory, which is supported by the National Science Foundation Cooperative Agreement No. DMR-1644779 and the State of Florida.

ASJC Scopus subject areas

General Chemistry
Biochemistry
Catalysis
Colloid and Surface Chemistry

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10.1021/jacs.0c08986

Cite this

Fataftah, M. S., Bayliss, S. L., Laorenza, D. W., Wang, X., Phelan, B. T., Wilson, C. B., Mintun, P. J., Kovos, B. D., Wasielewski, M. R., Han, S., Sherwin, M. S., Awschalom, D. D., & Freedman, D. E. (2020). Trigonal Bipyramidal V³⁺Complex as an Optically Addressable Molecular Qubit Candidate. Journal of the American Chemical Society, 142(48), 20400-20408. https://doi.org/10.1021/jacs.0c08986

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title = "Trigonal Bipyramidal V3+Complex as an Optically Addressable Molecular Qubit Candidate",

abstract = "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.",

author = "Fataftah, {Majed S.} and Bayliss, {Sam L.} and Laorenza, {Daniel W.} and Xiaoling Wang and Phelan, {Brian T.} and Wilson, {C. Blake} and Mintun, {Peter J.} and Kovos, {Berk D.} and Wasielewski, {Michael R.} and Songi Han and Sherwin, {Mark S.} and Awschalom, {David D.} and Freedman, {Danna E.}",

note = "Funding Information: The authors thank Dr. Johan van Tol and Rebecca Sponenburg for experimental assistance. The authors acknowledge David Enyeart and Nickolay Agladze for maintaining, repairing, and assisting with operation of the UCSB FEL. This project was initiated with support for M.S.F. from National Science Foundation CAREER Award No. CHE-1455017 to investigate fundamentals of coherence time and continued through support from DE-SC0019356 (D.E.F., D.W.L., B.T.P., and M.R.W) to develop molecules that interface with existing quantum infrastructure. We acknowledge funding from ONR N00014-17-1-3026, the MRSEC Shared User Facilities at the University of Chicago (NSF DMR-1420709), NSF-DMR-1906325, 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 DMR-1126894 and NSF-DMR-1626681. Experimental work was supported by the MRSEC Shared User Facilities at the University of Chicago (NSF DMR-1420709), IMSERC at Northwestern University, which has received support from Northwestern University, the State of Illinois, and the Int. Institute of Nanotechnology. A portion of this work was performed at the National High Magnetic Field Laboratory, which is supported by the National Science Foundation Cooperative Agreement No. DMR-1644779 and the State of Florida. Publisher Copyright: {\textcopyright} ",

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Fataftah, MS, Bayliss, SL, Laorenza, DW, Wang, X, Phelan, BT, Wilson, CB, Mintun, PJ, Kovos, BD, Wasielewski, MR , Han, S, Sherwin, MS, Awschalom, DD & Freedman, DE 2020, 'Trigonal Bipyramidal V³⁺Complex as an Optically Addressable Molecular Qubit Candidate', Journal of the American Chemical Society, vol. 142, no. 48, pp. 20400-20408. https://doi.org/10.1021/jacs.0c08986

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T1 - Trigonal Bipyramidal V3+Complex as an Optically Addressable Molecular Qubit Candidate

AU - Fataftah, Majed S.

AU - Bayliss, Sam L.

AU - Laorenza, Daniel W.

AU - Wang, Xiaoling

AU - Phelan, Brian T.

AU - Wilson, C. Blake

AU - Mintun, Peter J.

AU - Kovos, Berk D.

AU - Wasielewski, Michael R.

AU - Han, Songi

AU - Sherwin, Mark S.

AU - Awschalom, David D.

AU - Freedman, Danna E.

N1 - Funding Information: The authors thank Dr. Johan van Tol and Rebecca Sponenburg for experimental assistance. The authors acknowledge David Enyeart and Nickolay Agladze for maintaining, repairing, and assisting with operation of the UCSB FEL. This project was initiated with support for M.S.F. from National Science Foundation CAREER Award No. CHE-1455017 to investigate fundamentals of coherence time and continued through support from DE-SC0019356 (D.E.F., D.W.L., B.T.P., and M.R.W) to develop molecules that interface with existing quantum infrastructure. We acknowledge funding from ONR N00014-17-1-3026, the MRSEC Shared User Facilities at the University of Chicago (NSF DMR-1420709), NSF-DMR-1906325, 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 DMR-1126894 and NSF-DMR-1626681. Experimental work was supported by the MRSEC Shared User Facilities at the University of Chicago (NSF DMR-1420709), IMSERC at Northwestern University, which has received support from Northwestern University, the State of Illinois, and the Int. Institute of Nanotechnology. A portion of this work was performed at the National High Magnetic Field Laboratory, which is supported by the National Science Foundation Cooperative Agreement No. DMR-1644779 and the State of Florida. Publisher Copyright: ©

PY - 2020/12/2

Y1 - 2020/12/2

N2 - 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.

AB - 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.

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

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CCDC 2046226: Experimental Crystal Structure Determination

CCDC 2046227: Experimental Crystal Structure Determination

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

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CCDC 2046226: Experimental Crystal Structure Determination

CCDC 2046227: Experimental Crystal Structure Determination

Cite this

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