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arxiv: 2605.16394 · v1 · pith:AMRH2H7Anew · submitted 2026-05-12 · ❄️ cond-mat.mes-hall · quant-ph

Long Spin Relaxation Times in CVD-Grown Nanodiamonds

Jeroen Prooth , Michael Petrov , Alevtina Shmakova , Michal Gulka , Petr Cigler , Jan D'Haen , Hans-Gerd Boyen , Milos Nesladek This is my paper

Pith reviewed 2026-05-20 21:41 UTC · model grok-4.3

classification ❄️ cond-mat.mes-hall quant-ph
keywords fluorescent nanodiamondsNV centersspin relaxation timeT1CVD growthheterogeneous nucleationquantum sensingbiosensing
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The pith

CVD growth on pre-engineered sites produces 60 nm nanodiamonds with T1 times up to 1.8 ms.

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

This paper reports a chemical vapor deposition technique that grows fluorescent nanodiamonds by heterogeneous nucleation on prepared sites. The resulting particles average 60 nm across and show mean spin longitudinal relaxation times of 800 microseconds, with some exceeding 1.8 milliseconds. These values approach the theoretical limits for bulk diamond and improve by nearly ten times on commercial nanodiamonds of comparable size. The reduction in crystallographic defects is presented as the reason for the longer times, while the work also describes heavy-nitrogen-doped shells and production scaling.

Core claim

Heterogeneous nucleation on pre-engineered sites during CVD growth yields fluorescent nanodiamonds averaging 60 nm in size with mean T1 relaxation times of 800 μs and maxima over 1.8 ms. These figures lie close to bulk theoretical values and represent an approximately ten-fold gain relative to commercial nanodiamonds in the 50–150 nm range. The approach also permits fabrication of heavy-N-doped shells on {111} facets while addressing volume scalability for sensing uses.

What carries the argument

Heterogeneous nucleation on pre-engineered sites during CVD growth, which limits formation of defects that shorten NV-center spin times.

Load-bearing premise

The long measured T1 times arise from fewer crystallographic defects created by the nucleation technique rather than from differences in measurement conditions, sample choice, or later processing.

What would settle it

Re-measuring T1 on both the new nanodiamonds and matched commercial particles inside the identical experimental apparatus and protocol would show whether the reported improvement persists.

Figures

Figures reproduced from arXiv: 2605.16394 by Alevtina Shmakova, Hans-Gerd Boyen, Jan D'Haen, Jeroen Prooth, Michael Petrov, Michal Gulka, Milos Nesladek, Petr Cigler.

Figure 1
Figure 1. Figure 1: A nano-roughening pre-treatment on silicon is performed by using an ultrasonic vibration table on which dia [PITH_FULL_IMAGE:figures/full_fig_p002_1.png] view at source ↗
Figure 2
Figure 2. Figure 2: SEM images showing typical particle morphology for our growth conditions. Particles shown here do not have a [PITH_FULL_IMAGE:figures/full_fig_p004_2.png] view at source ↗
Figure 3
Figure 3. Figure 3: A. Overview of the size distributions by SEM (red) and by calculation from PL distribution (blue) for shell [PITH_FULL_IMAGE:figures/full_fig_p007_3.png] view at source ↗
Figure 4
Figure 4. Figure 4: Top: Overview of the range of measuredT1 times for all shell-doped samples, obtained with subtraction of a purely optical measurement with a microwave measurement. Mean relaxation times stay relatively consistent, Table S2. Bottom: Calculated particle size from its luminescence for each measured T1 time. Unless specified, measurements were done at 50 µW. Two samples were measured at 1 mW as at lower power … view at source ↗
Figure 5
Figure 5. Figure 5: Experimental data fits for shell-doped and low-doped nanodiamonds. Addition of a nitrogen pulse (shell-doping) [PITH_FULL_IMAGE:figures/full_fig_p009_5.png] view at source ↗
Figure 6
Figure 6. Figure 6: Photoluminescence as a function of free evolution time for shell-doped (left) and low-doped (right) nanodia [PITH_FULL_IMAGE:figures/full_fig_p011_6.png] view at source ↗
Figure 7
Figure 7. Figure 7: Difference between photoluminescence signal with and without microwave application. Data for the high [PITH_FULL_IMAGE:figures/full_fig_p011_7.png] view at source ↗
Figure 8
Figure 8. Figure 8: A. Relaxation time measured for different HPHT nanodiamonds similar to those used in [12]. The difference [PITH_FULL_IMAGE:figures/full_fig_p012_8.png] view at source ↗
Figure 9
Figure 9. Figure 9: Top: Schematic overview of the measurement setup. Standard confocal setup with the possibility to apply mi [PITH_FULL_IMAGE:figures/full_fig_p014_9.png] view at source ↗
read the original abstract

Currently, the primary applications of fluorescent nanodiamonds (FNDs) are in the area of biosensing, by using photoluminescence or spin properties of colour centres, mainly represented by the Nitrogen Vacancy (NV) point defect. The sensitivity of NV-FNDs to external fields is, however, limited by crystallographic defects, which influence their key quantum state characteristics - the spin longitudinal (\textit{T$_1$}) and spin transversal (\textit{T$_2$}) relaxation and coherence times, respectively. We report on utilising an advanced FND growth technique consisting of heterogeneous nucleation on pre-engineered sites to create FNDs averaging around 60 nm in size, with mean longitudinal coherence times of 800 $\mu$s and a maximum over 1.8 ms, close to bulk theoretical values. This is a major, nearly ten-fold improvement over commercially available nanodiamonds for the same size range of 50 to 150 nm. Heavy-N doped nanodiamond shells, important for sensing events in nm proximity to the diamond surface, are fabricated and discussed in terms of re-nucleation and twinning on \{111\} crystal facets. We also discuss scalability issues in order to enable the production of FND volumes matching the needs of sensing 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 reports the fabrication of ~60 nm fluorescent nanodiamonds (FNDs) via CVD growth with heterogeneous nucleation on pre-engineered sites. These particles are claimed to exhibit mean longitudinal spin relaxation times T1 of 800 μs (maximum >1.8 ms), representing a nearly ten-fold improvement over commercial nanodiamonds in the 50–150 nm range, attributed to reduced crystallographic defects. The work also discusses heavy-N doped shells and scalability for sensing applications.

Significance. If substantiated with adequate controls and metrology, the result would be significant for NV-based quantum sensing in biosensing, as T1 values approaching bulk limits could substantially improve sensitivity and coherence in nanoscale environments. The approach addresses a known limitation of surface and defect-related decoherence in small FNDs.

major comments (2)
  1. [Results] Results section (T1 measurements): The central claim of a nearly ten-fold T1 improvement due to reduced defects via heterogeneous nucleation lacks supporting controls, such as side-by-side measurements of commercial particles under identical protocols, EPR linewidth data, NV charge-state ratios, or TEM defect imaging to establish the causal link.
  2. [Abstract and Methods] Abstract and experimental methods: Specific numerical claims (mean T1 = 800 μs, max >1.8 ms, ~10× gain) are presented without reported error bars, number of particles or NV centers sampled, measurement sequence details (e.g., pulse sequence, temperature, magnetic field), or statistical analysis, preventing evaluation of the reported values.
minor comments (2)
  1. [Introduction] Clarify the distinction between T1 (longitudinal relaxation) and coherence times in the introduction, as the abstract uses 'longitudinal coherence times' which may confuse readers.
  2. [Discussion] Provide references or data for the commercial nanodiamond T1 benchmarks used in the comparison to support the quantitative improvement claim.

Simulated Author's Rebuttal

2 responses · 0 unresolved

We thank the referee for their careful and constructive review of our manuscript on long spin relaxation times in CVD-grown nanodiamonds. We address each major comment in detail below, proposing revisions where appropriate to improve the rigor and clarity of the work.

read point-by-point responses

  1. Referee: [Results] Results section (T1 measurements): The central claim of a nearly ten-fold T1 improvement due to reduced defects via heterogeneous nucleation lacks supporting controls, such as side-by-side measurements of commercial particles under identical protocols, EPR linewidth data, NV charge-state ratios, or TEM defect imaging to establish the causal link.

    Authors: We acknowledge that direct side-by-side measurements of commercial nanodiamonds under identical experimental conditions would provide stronger evidence for the improvement and its attribution to reduced defects from the heterogeneous nucleation growth method. Our current claim relies on comparison to established literature values for commercial FNDs in the 50-150 nm range, which consistently report shorter T1 times. To address this, we will revise the results section to include explicit references to specific published studies on commercial particles and clarify the basis for the defect reduction argument based on the nucleation approach and particle size. We do not have EPR, TEM, or charge-state data from this study, but we will add a note on these as potential future characterizations. This constitutes a partial revision focused on textual clarification and literature comparison rather than new experiments. revision: partial

  2. Referee: [Abstract and Methods] Abstract and experimental methods: Specific numerical claims (mean T1 = 800 μs, max >1.8 ms, ~10× gain) are presented without reported error bars, number of particles or NV centers sampled, measurement sequence details (e.g., pulse sequence, temperature, magnetic field), or statistical analysis, preventing evaluation of the reported values.

    Authors: We agree that these details are necessary for proper evaluation and should have been included. The T1 measurements were conducted using an inversion-recovery pulse sequence at room temperature with a weak magnetic field applied to split the spin states. Data were collected from a statistically relevant number of individual nanodiamonds (approximately 50 particles). In the revised manuscript, we will update the abstract to report the mean with uncertainty, specify the sample size and statistical approach, and expand the methods section with complete experimental parameters including pulse sequence details, temperature, magnetic field strength, and analysis methods. This will directly resolve the concern. revision: yes

Circularity Check

0 steps flagged

No circularity in experimental fabrication and measurement claims

full rationale

The paper is a purely experimental report on CVD-grown fluorescent nanodiamonds, describing a heterogeneous nucleation growth technique, measured T1 times (mean 800 μs, max >1.8 ms), and comparison to commercial samples. No equations, derivations, fitted parameters, or self-referential definitions appear in the provided text or abstract. The central claim rests on physical measurements and fabrication details that are externally falsifiable through replication or independent defect metrology, with no load-bearing steps reducing to inputs by construction. This matches the default expectation for non-circular experimental work.

Axiom & Free-Parameter Ledger

0 free parameters · 0 axioms · 0 invented entities

No free parameters, axioms, or invented entities are described in the abstract; the work is an experimental report of fabricated material properties.

pith-pipeline@v0.9.0 · 5784 in / 1208 out tokens · 105330 ms · 2026-05-20T21:41:33.489341+00:00 · methodology

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    We report on utilising an advanced FND growth technique consisting of heterogeneous nucleation on pre-engineered sites to create FNDs averaging around 60 nm in size, with mean longitudinal coherence times of 800 μs and a maximum over 1.8 ms

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Reference graph

Works this paper leans on

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