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arXiv · 2605.03177

Understanding the effects of competing spin-pair dephasing pathways in molecular spins

Timothy J. Krogmeier·James Bradley·Anthony W. Schlimgen·Kade Head-Marsden
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Abstract

Molecular spins offer promise in emerging quantum technologies such as quantum sensing and computing. At low temperatures, nuclear spin-spin interactions affect electron spin coherence lifetimes through pure dephasing. Nuclear-spin noise can originate from spin pairs within a molecule itself, pairs in a surrounding environment system, or pairs in which one spin is on the molecule and the other in the environment. Improving coherence times requires detailed knowledge of the dominant sources of dephasing. Here, we analyze the decoherence behavior of two molecular qubit candidates with various ligands and in different nuclear-spin containing solvents. We apply an electronic-structure enhanced, non-Markovian perturbative theoretical method to connect experimentally comparable dephasing times to individual spin pairs. This analysis allows the development of a computational workflow to strategically improve coherence lifetimes in spin systems where decoherence is dominated by spin-spin dephasing.

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Timothy J. Krogmeier, James Bradley, Anthony W. Schlimgen, Kade Head-Marsden. 2026-05-04. Understanding the effects of competing spin-pair dephasing pathways in molecular spins. https://arxiv.org/abs/2605.03177

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