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arxiv: 2510.19598 · v3 · submitted 2025-10-22 · 🪐 quant-ph

Zero-field identification and control of hydrogen-related electron-nuclear spin registers in diamond

Alexander Ungar , Hao Tang , Andrew Stasiuk , Bo Xing , Boning Li , Ju Li , Alexandre Cooper , Paola Cappellaro This is my paper

Pith reviewed 2026-05-18 04:42 UTC · model grok-4.3

classification 🪐 quant-ph
keywords electron-nuclear spin defectsdiamondzero-field DEERhydrogen-related defectsnuclear spin qubitNEETR protocolab initio defect identificationquantum registers
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The pith

Zero-field resonance protocols identify a new hydrogen-related defect in diamond and enable coherent control of its nuclear spin qubit.

A machine-rendered reading of the paper's core claim, the machinery that carries it, and where it could break.

The paper develops two hybrid electron-nuclear control schemes to characterize unknown spin defects in diamond at the single-spin level. Zero-field double electron-electron resonance extracts hyperfine components while a nuclear-electron-electron triple resonance protocol uses the electronic spin to initialize and identify the nuclear spin. Comparing these measurements to ab initio calculations identifies a new hydrogen-related defect structure and confirms a previously known nitrogen-related one. The same NEETR protocol further demonstrates initialization, unitary control, and a coherence time of 1.0(3) ms for the hydrogen nuclear spin. This approach supplies a practical route to incorporating previously uncharacterized defects into multi-qubit quantum registers.

Core claim

Applying ZF-DEER extracts hyperfine components at zero field, and the NEETR protocol controls the nuclear spin through its interaction with the stronger electronic spin. These measurements, when matched to ab initio calculations, resolve a new hydrogen-related defect structure and accurately reproduce a known nitrogen-related defect. The NEETR sequence additionally achieves initialization, unitary control, and long-lived coherence of the hydrogen nuclear spin qubit with T2 = 1.0(3) ms.

What carries the argument

The ZF-DEER protocol for zero-field hyperfine extraction combined with the NEETR triple-resonance sequence that routes nuclear control through the electronic spin.

If this is right

  • The identified hydrogen-related defect can now be integrated as a controllable nuclear spin qubit in diamond-based quantum registers.
  • The NEETR protocol supplies a general route to initialization and unitary control of nuclear spins coupled to optically active electrons.
  • Zero-field hyperfine extraction plus ab initio matching supplies a template for characterizing other unknown electron-nuclear defects.
  • Millisecond nuclear coherence times support longer storage times in quantum sensing and networking protocols that use these registers.

Where Pith is reading between the lines

These are editorial extensions of the paper, not claims the author makes directly.

  • The zero-field approach may reduce the need for precise magnetic-field alignment when screening new defects in other wide-bandgap hosts.
  • Systematic application of the same workflow could map families of hydrogen-related defects across different diamond growth conditions.
  • Long nuclear coherence in these registers suggests they could serve as auxiliary memories in hybrid quantum devices that combine sensing and communication.

Load-bearing premise

The extracted hyperfine values and resonance signals match ab initio calculations to specific defect structures without significant overlap from other possible electron-nuclear configurations or experimental artifacts.

What would settle it

An independent measurement that yields hyperfine components inconsistent with the proposed hydrogen-related structure or a coherence time far below 1 ms on the same defect would undermine the identification and control claims.

Figures

Figures reproduced from arXiv: 2510.19598 by Alexander Ungar, Alexandre Cooper, Andrew Stasiuk, Boning Li, Bo Xing, Hao Tang, Ju Li, Paola Cappellaro.

Figure 1
Figure 1. Figure 1: FIG. 1. Hyperfine component identification for X1 and X2 defects. (a) Double electron-electron resonance (DEER) performed [PITH_FULL_IMAGE:figures/full_fig_p003_1.png] view at source ↗
Figure 2
Figure 2. Figure 2: FIG. 2. Nuclear spin identification for X1 and X2 defects. (a) Nuclear-electron-electron triple resonance (NEETR) pulse [PITH_FULL_IMAGE:figures/full_fig_p005_2.png] view at source ↗
Figure 3
Figure 3. Figure 3: FIG. 3. (a) Model of the V-CH-V [PITH_FULL_IMAGE:figures/full_fig_p006_3.png] view at source ↗
Figure 4
Figure 4. Figure 4: FIG. 4. Universal control and coherence of the X1 hydrogen nuclear spin. (a) Applying the NEETR sequence (Fig. [PITH_FULL_IMAGE:figures/full_fig_p008_4.png] view at source ↗
read the original abstract

Spin defects in diamond serve as powerful building blocks for quantum technologies, especially for applications in quantum sensing and quantum networking. Electron-nuclear defects formed in the environment of optically active spins, such as the nitrogen-vacancy (NV) center, provide a resource for multi-qubit quantum registers. However, many of these defects have yet to be characterized, limiting their control and integration in quantum devices. Here, we apply two hybrid electron-nuclear spin control schemes to self-consistently characterize unknown spin defects at the single-spin level. We perform double electron-electron resonance at zero field (ZF-DEER) to extract hyperfine components and introduce a nuclear-electron-electron triple resonance (NEETR) protocol to control and identify the nuclear spin through the stronger electronic spin interaction. These results provide a guide to resolving the defect structures using ab initio calculations, leading to the identification of a new hydrogen-related defect structure as well as an accurate match to a previously identified nitrogen-related defect. We further apply our NEETR protocol to demonstrate initialization, unitary control, and long-lived coherence of the hydrogen nuclear spin qubit with $T_2 = 1.0(3)\,\mathrm{ms}$. Together, these characterization and control tools establish a framework to harness previously unknown electron-nuclear defects for quantum register applications.

Editorial analysis

A structured set of objections, weighed in public.

Desk editor's note, referee report, simulated authors' rebuttal, and a circularity audit. Tearing a paper down is the easy half of reading it; the pith above is the substance, this is the friction.

Referee Report

2 major / 2 minor

Summary. The manuscript introduces zero-field double electron-electron resonance (ZF-DEER) and nuclear-electron-electron triple resonance (NEETR) protocols for self-consistent characterization of unknown electron-nuclear spin defects in diamond at the single-spin level. Hyperfine components extracted via ZF-DEER are matched to ab initio calculations to identify a new hydrogen-related defect structure and confirm a previously known nitrogen-related defect; the NEETR protocol is then used to demonstrate initialization, unitary control, and coherence of the hydrogen nuclear spin qubit with T2 = 1.0(3) ms.

Significance. If the central identification holds, the work supplies practical experimental tools for resolving defect structures that can serve as multi-qubit registers, together with a concrete demonstration of long nuclear-spin coherence. The hybrid experimental-theoretical approach and the reported T2 value are strengths that would be useful for quantum sensing and networking applications.

major comments (2)
  1. [§4] §4 (defect identification): the assignment of the new hydrogen-related defect rests on matching the ZF-DEER-extracted hyperfine tensor components to a single ab initio candidate. No systematic scan over alternative H placements, charge states, or nearby impurities is shown, and no quantitative metric (RMS deviation, likelihood ratio, or similar) is provided to demonstrate that no other plausible configuration lies within the experimental uncertainty of the measured A-tensor.
  2. [Methods and §5] Methods and §5 (NEETR results): the reported T2 = 1.0(3) ms and the uniqueness of the nuclear-spin identification via NEETR signals are central to the control claim, yet the manuscript does not include the full pulse sequences, raw time traces, or detailed error-propagation analysis that would allow independent assessment of the quoted uncertainty.
minor comments (2)
  1. [Figures 3-5] Figure captions and axis labels in the ZF-DEER and NEETR data panels could be expanded to include the precise fitting ranges and the number of averaged shots.
  2. [Table 1 or new table] A short table comparing the measured hyperfine components with the ab initio values for both the H and N defects would improve readability.

Simulated Author's Rebuttal

2 responses · 0 unresolved

We thank the referee for the careful reading and constructive comments on our manuscript. We address each major point below and indicate the revisions made to strengthen the presentation of the defect identification and the NEETR results.

read point-by-point responses

  1. Referee: [§4] §4 (defect identification): the assignment of the new hydrogen-related defect rests on matching the ZF-DEER-extracted hyperfine tensor components to a single ab initio candidate. No systematic scan over alternative H placements, charge states, or nearby impurities is shown, and no quantitative metric (RMS deviation, likelihood ratio, or similar) is provided to demonstrate that no other plausible configuration lies within the experimental uncertainty of the measured A-tensor.

    Authors: We agree that the identification would be strengthened by a more systematic comparison. The selected candidate was chosen on the basis of the known incorporation of hydrogen during the CVD growth process used for the sample and the close numerical agreement with the measured hyperfine tensor. In the revised manuscript we have added a supplementary note that reports the RMS deviation between the experimental A-tensor and the ab initio values for the identified structure, together with a brief discussion of why alternative common placements and charge states produce tensors that fall outside the experimental uncertainty. A fully exhaustive computational scan over all conceivable configurations is computationally intensive and lies beyond the scope of the present work; we have noted this limitation explicitly. revision: partial

  2. Referee: [Methods and §5] Methods and §5 (NEETR results): the reported T2 = 1.0(3) ms and the uniqueness of the nuclear-spin identification via NEETR signals are central to the control claim, yet the manuscript does not include the full pulse sequences, raw time traces, or detailed error-propagation analysis that would allow independent assessment of the quoted uncertainty.

    Authors: We accept that additional experimental detail is required for independent verification. The revised manuscript now contains the complete NEETR pulse sequences in the Methods section, includes the raw coherence time traces as a new supplementary figure, and provides an expanded description of the fitting procedure together with the error-propagation analysis used to arrive at the quoted uncertainty of T2 = 1.0(3) ms. revision: yes

Circularity Check

0 steps flagged

No circularity: experimental extraction matched to independent ab initio calculations

full rationale

The paper extracts hyperfine components via ZF-DEER and applies NEETR for control and identification, then matches results to separate ab initio calculations to assign defect structures. This chain does not reduce by construction to self-definition, fitted inputs renamed as predictions, or load-bearing self-citations; the ab initio component is external and the experimental protocols operate on measured signals without circular re-use of the target identification. Uniqueness of the match is an evidential question outside the scope of circularity analysis.

Axiom & Free-Parameter Ledger

0 free parameters · 2 axioms · 0 invented entities

The central claim rests on standard assumptions from quantum spin resonance and the accuracy of ab initio defect modeling; no explicit free parameters or new invented entities are introduced in the abstract.

axioms (2)
  • domain assumption Hyperfine components extracted from ZF-DEER at zero field accurately reflect the electron-nuclear spin interactions of the target defects.
    Invoked when applying ZF-DEER to extract components for structure resolution.
  • domain assumption Ab initio calculations provide reliable guidance for matching experimental hyperfine data to specific defect structures.
    Used to identify the hydrogen-related and nitrogen-related defects.

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