Title: Enhancing Spin Coherence in Optically Addressable Molecular Qubits through Host-Matrix Control

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 readout. 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 nonisostructural 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 structurefunction relationships through a tunablemore » molecular platform and highlight opportunities for using molecular qubits for nanoscale quantum sensing in noisy environments.« less

Authors:

Bayliss, S. L. ;

• Search DOE PAGES for author "Bayliss, S. L."
• Search DOE PAGES for ORCID "0000-0002-1156-7243"

Deb, P. ;

• Search DOE PAGES for author "Deb, P."
• Search DOE PAGES for ORCID "0000-0001-6269-9054"

Laorenza, D. W. ;

• Search DOE PAGES for author "Laorenza, D. W."
• Search DOE PAGES for ORCID "0000-0003-1566-6932"

Onizhuk, M. ;

• Search DOE PAGES for author "Onizhuk, M."
• Search DOE PAGES for ORCID "0000-0003-0434-4575"

Galli, G. ;

• Search DOE PAGES for author "Galli, G."
• Search DOE PAGES for ORCID "0000-0002-8001-5290"

Freedman, D. E. ;

• Search DOE PAGES for author "Freedman, D. E."
• Search DOE PAGES for ORCID "0000-0002-2579-8835"

Awschalom, D. D.

• Search DOE PAGES for author "Awschalom, D. D."
• Search DOE PAGES for ORCID "0000-0002-8591-2687"

Publication Date:

Thu Aug 18 00:00:00 EDT 2022

Research Org.:

Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Univ. of Chicago, IL (United States)

Sponsoring Org.:

USDOE; US Department of the Navy, Office of Naval Research (ONR); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

OSTI Identifier:

1882435

Alternate Identifier(s):

OSTI ID: 1903595

Grant/Contract Number:  

SC0019356; N00014-17-1-3026

Resource Type:

Published Article

Journal Name:

Physical Review. X

Additional Journal Information:

Journal Name: Physical Review. X Journal Volume: 12 Journal Issue: 3; Journal ID: ISSN 2160-3308

Publisher:

American Physical Society

Country of Publication:

United States

Language:

English

Subject:

74 ATOMIC AND MOLECULAR PHYSICS