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 of1demonstrating coherent control of this spin qubit with a 240 GHz electron paramagnetic resonance spectrometer powered by a free electron laser. We found that1exhibited 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.
- Authors:
-
[2];
[1];
[2];
[2];
[1];
[3];
[4];
[1]
- Northwestern Univ., Evanston, IL (United States)
- Univ. of Chicago, IL (United States)
- Univ. of California, Santa Barbara, CA (United States)
- Univ. of Chicago, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States)
- Publication Date:
- Research Org.:
- Univ. of California, Santa Barbara, CA (United States); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Northwestern Univ., Evanston, IL (United States); Univ. of Chicago, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); US Department of the Navy, Office of Naval Research (ONR); National Science Foundation (NSF)
- OSTI Identifier:
- 1905082
- Alternate Identifier(s):
- OSTI ID: 1773826
- Grant/Contract Number:
- SC0019356; N00014-17-1-3026; NSF DMR-1420709; NSF-DMR-1906325; MRI-19-601107; DMR-1126894; NSF-DMR-1626681
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 142; Journal Issue: 48; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 30 DIRECT ENERGY CONVERSION; 72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS; spin qubits; quantum information science; ligands; magnetic properties; electron paramagnetic resonance spectroscopy; quantum mechanics; defects
Citation Formats
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., and Freedman, Danna E. Trigonal Bipyramidal V3+ Complex as an Optically Addressable Molecular Qubit Candidate. United States: N. p., 2020.
Web. doi:10.1021/jacs.0c08986.
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. Trigonal Bipyramidal V3+ Complex as an Optically Addressable Molecular Qubit Candidate. United States. https://doi.org/10.1021/jacs.0c08986
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., and Freedman, Danna E. Thu .
"Trigonal Bipyramidal V3+ Complex as an Optically Addressable Molecular Qubit Candidate". United States. https://doi.org/10.1021/jacs.0c08986. https://www.osti.gov/servlets/purl/1905082.
@article{osti_1905082,
title = {Trigonal Bipyramidal V3+ Complex as an Optically Addressable Molecular Qubit Candidate},
author = {Fataftah, Majed S. and Bayliss, Sam L. and Laorenza, Daniel W. and Wang, Xiaoling and Phelan, Brian T. and Wilson, C. Blake and Mintun, Peter J. and Kovos, Berk D. and Wasielewski, Michael R. and Han, Songi and Sherwin, Mark S. and Awschalom, David D. and Freedman, Danna E.},
abstractNote = {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 of1demonstrating coherent control of this spin qubit with a 240 GHz electron paramagnetic resonance spectrometer powered by a free electron laser. We found that1exhibited 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.},
doi = {10.1021/jacs.0c08986},
journal = {Journal of the American Chemical Society},
number = 48,
volume = 142,
place = {United States},
year = {Thu Nov 19 00:00:00 EST 2020},
month = {Thu Nov 19 00:00:00 EST 2020}
}
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