Trigonal Bipyramidal V 3+ Complex as an Optically Addressable Molecular Qubit Candidate.

Autor: Fataftah MS; Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States., Bayliss SL; Pritzker School of Molecular Engineering, University of Chicago, Chicago, Illinois 60637, United States., Laorenza DW; Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States., Wang X; 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., Phelan BT; Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States.; The Institute for Sustainability and Energy at Northwestern, Northwestern University, Evanston, Illinois 60208, United States., Wilson CB; 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., Mintun PJ; Pritzker School of Molecular Engineering, University of Chicago, Chicago, Illinois 60637, United States., Kovos BD; Pritzker School of Molecular Engineering, University of Chicago, Chicago, Illinois 60637, United States., Wasielewski MR; Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States.; The Institute for Sustainability and Energy at Northwestern, Northwestern University, Evanston, Illinois 60208, United States., Han S; 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.; Institute for Terahertz Science and Technology, University of California, Santa Barbara, Santa Barbara, California 93106, United States., Sherwin MS; 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., Awschalom DD; Pritzker School of Molecular Engineering, University of Chicago, Chicago, Illinois 60637, 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., Freedman DE; Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States.
Jazyk: angličtina
Zdroj: Journal of the American Chemical Society [J Am Chem Soc] 2020 Nov 19. Date of Electronic Publication: 2020 Nov 19.
DOI: 10.1021/jacs.0c08986
Abstrakt: 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, V 3+ complex, (C 6 F 5 ) 3 trenVCN 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 V 3+ complexes are candidates for optical spin addressability.
Databáze: MEDLINE
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