Enhancing spin coherence in optically addressable molecular qubits through host-matrix control

Bayliss, S. L. , Deb, P., Laorenza, D. W., Onizhuk, M., Galli, G., Freedman, D. E. and Awschalom, D. D. (2022) Enhancing spin coherence in optically addressable molecular qubits through host-matrix control. Physical Review X, 12(3), 031028. (doi: 10.1103/PhysRevX.12.031028)

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Abstract

Optically addressable spins are a promising platform for quantum information science due to their combination of a long-lived qubit with a spin-optical interface for external qubit control and read out. The ability to chemically synthesize such systems—to generate optically addressable molecular spins—offers a modular qubit architecture which can be transported across different environments, and atomistically tailored for targeted applications through bottom-up design and synthesis. Here we demonstrate how the spin coherence in such optically addressable molecular qubits can be controlled through engineering their host environment. By inserting chromium (IV)-based molecular qubits into a non-isostructural host matrix, we generate noise-insensitive clock transitions, through a transverse zero-field splitting, that are not present when using an isostructural host. This host-matrix engineering leads to spin-coherence times of more than 10 µs for optically addressable molecular spin qubits in a nuclear and electron-spin rich environment. We model the dependence of spin coherence on transverse zero-field splitting from first principles and experimentally verify the theoretical predictions with four distinct molecular systems. Finally, we explore how to further enhance optical-spin interfaces in molecular qubits by investigating the key parameters of optical linewidth and spin-lattice relaxation time. Our results demonstrate the ability to test qubit structure-function relationships through a tunable molecular platform and highlight opportunities for using molecular qubits for nanoscale quantum sensing in noisy environments.

Item Type:Articles
Status:Published
Refereed:Yes
Glasgow Author(s) Enlighten ID:Bayliss, Dr Sam
Authors: Bayliss, S. L., Deb, P., Laorenza, D. W., Onizhuk, M., Galli, G., Freedman, D. E., and Awschalom, D. D.
College/School:College of Science and Engineering > School of Engineering > Electronics and Nanoscale Engineering
Journal Name:Physical Review X
Publisher:American Physical Society
ISSN:2160-3308
ISSN (Online):2160-3308
Published Online:18 August 2022
Copyright Holders:Copyright © 2022 American Physical Society
First Published:First published in Physical Review X 12(3): 031028
Publisher Policy:Reproduced under a Creative Commons License
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