Exploring hyperfine coupling in molecular qubits

Abstract

Molecular qubits represent a promising avenue for advancing quantum sensing and computing technologies, yet significant challenges remain in optimising their performance. Hyperfine coupling has a critical influence on molecular qubit properties. While previous studies have exhaustively investigated this phenomenon, a comprehensive understanding of the underlying mechanisms across different systems remains elusive. A benchmark test was performed using DFT to assess which methodology worked best to accurately predict hyperfine coupling constants in molecular qubits predominantly composed of VIV and CuII. We systematically analysed the decomposition of hyperfine coupling and examined how variations in coordination sphere and molecular geometry impact dipolar, isotropic and spin–orbit contributions. By modelling diverse systems, we demonstrate how molecular design can fine-tune hyperfine coupling contributions, either minimising overall interaction or enhancing coupling along specific axes. This study provides useful insights into the structure–property relationships governing hyperfine coupling mechanisms and assesses the accuracy of different choices of density functional, basis sets and relativistic corrections in the prediction of hyperfine coupling constants.

Graphical abstract: Exploring hyperfine coupling in molecular qubits

Supplementary files

Article information

Article type
Edge Article
Submitted
03 Apr 2025
Accepted
22 May 2025
First published
23 May 2025
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY-NC license

Chem. Sci., 2025, Advance Article

Exploring hyperfine coupling in molecular qubits

J. Cardona, À. Solé, P. Mella, D. Aravena, J. Ruiz-Hidalgo, S. Gómez-Coca and E. Ruiz, Chem. Sci., 2025, Advance Article , DOI: 10.1039/D5SC02500A

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