High-Efficiency, High-Fidelity Charge Initialization of Shallow Nitrogen Vacancy Centers in Diamond

Artur Lozovoi; Carlos A. Meriles; Jared Rovny; Marjana Mahdia; Nathalie P. de Leon; Zhiyang Yuan

REVIEW 3 major objections 6 minor 28 references

High-Efficiency, High-Fidelity Charge Initialization of Shallow Nitrogen Vacancy Centers in Diamond

T0 review · 3 major / 6 minor · reviewed 2026-08-07 · deepseek-v4-flash

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Pith's one-line read Shallow NV centers can be pushed into their negative charge state with 95% fidelity in about 300 μs using simultaneous green and near-infrared light, and to 90% in 10 μs.

desk verdict A useful and mostly careful NV charge-initialization study, but the 10-μs headline is a model extrapolation to an unmeasured power point, not a direct measurement. read the letter →

arxiv 2506.00707 v1 pith:EO6T6QO7 submitted 2025-05-31 cond-mat.mtrl-sci quant-ph

Marjana Mahdia , Artur Lozovoi , Jared Rovny , Zhiyang Yuan , Carlos A. Meriles , Nathalie P. de Leon This is my paper · ORCID

classification cond-mat.mtrl-sciquant-ph

keywords nitrogen-vacancycenterschargestateinitializationmulticolorexcitationnear-infraredquantumsensingrate-equationmodelcovariancemagnetometryshallowNV

verification ladder T0 review T1 audit T2 compute T3 formal

The pith

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

The reading

The paper sets out to show that a simple two-color optical pulse—simultaneous 520 nm green and 905 nm near-infrared illumination—can initialize shallow nitrogen-vacancy (NV) centers, sitting 5–15 nm below a diamond surface, into their negative charge state with near-unity fidelity at low power and short time. This matters because the conventional green-only initialization leaves about 30% of the population in the wrong (neutral) charge state, and that preparation error is the dominant limit on nanoscale quantum sensing. By fitting a two-state rate-equation model to single-NV charge dynamics, the authors identify a parameter region where 95% initialization is reached within 300 μs (1 mW NIR, 10 μW green) and 90% within 10 μs (4 mW NIR, 39 μW green).

What carries the argument

The central object is the two-state rate-equation model of NV charge cycling, $d/dt[NV^-; NV^0] = [[-\gamma_i, \gamma_r], [\gamma_i, -\gamma_r]][NV^-; NV^0]$, with solution $[NV^-](t) = \gamma_r/\gamma_{tot} + (\rho_0 - \gamma_r/\gamma_{tot})e^{-\gamma_{tot} t}$. The rates $\gamma_i$ and $\gamma_r$ depend on green and NIR powers through multi-photon ionization and recombination channels, including two-photon green ionization, combined green-NIR pathways, and singlet-mediated three-photon processes. The paper fits these rates to measured $[NV^-]$ versus time curves at several powers, validates the model on power combinations not used during fitting, and then uses the fitted model to map the power-time parameter space and identify the region where $[NV^-] \ge 0.90$ within 10 μs.

What would settle it

Measure the NV− population, using the same zero-readout-time extrapolation, after exactly 10 μs of simultaneous 4 mW NIR and 39 μW green illumination on a shallow NV center (5–15 nm deep) with the same surface treatment; if the fidelity falls below 90%, the model's extrapolation is optimistic and the headline speed does not hold.

Watch

Extended reading notes

Core claim

The central discovery is that shallow NV centers, when prepared with the right oxygen surface termination, exhibit charge interconversion rates several times higher than bulk NVs under combined green and NIR excitation, which converts the previously slow (millisecond) bulk multicolor initialization into a microsecond-scale, low-power protocol. The paper reports 95% NV− initialization within 300 μs at sub-milliwatt NIR and microwatt green powers, and its fitted model identifies a parameter region where 90% initialization is reached in 10 μs at 4 mW NIR and 39 μW green. It further shows that the multicolor pulse preserves optical spin polarization, increases spin contrast by 12.5%, and reduces readout noise by about 10%, and calculates that the reduced SPAM error shortens the total time for three-point covariance magnetometry by a factor of five.

Load-bearing premise

The load-bearing premise is that the two-state rate-equation model, fit at a few power combinations, extrapolates accurately across the power-time parameter space—in particular, the claim that 90% initialization can be reached in 10 μs at 4 mW NIR and 39 μW green rests on the fitted model rather than on directly measured data at those exact settings.

Editorial extensions

If this is right

The protocol can replace green-only initialization in single-NV and wide-field setups without new hardware, needing only microwatts of green and a few milliwatts of near-infrared light.
The reduced state-preparation and measurement error directly increases magnetometer sensitivity, since spin contrast rises and readout noise falls.
The 10 μs initialization time is comparable to typical sensing sequence lengths, so the added overhead is negligible in ordinary NV sensing experiments.
In covariance magnetometry, the reduced readout noise shortens total experiment time fivefold for three-point correlations, making higher-order multipoint correlators practical.
The scheme scales to wide-field multiplexed excitation: 300 μs of 70 mW green and 800 mW NIR over a 10×10 μm² area reaches 95% NV− population.

Reading between the lines

Editorial extensions of the paper, not claims the author makes directly.

The higher rates measured here versus bulk NVs likely stem from the oxygen surface termination; if so, the same termination may accelerate charge initialization for other shallow color centers in diamond.
The parameter-space map shows an optimal NIR power beyond which three-photon ionization degrades fidelity; this trade-off should be re-examined for other wavelengths and diamond surface chemistries.
The 10 μs claim at 4 mW NIR and 39 μW green rests on model extrapolation, so a direct measurement at those exact settings would be the cleanest test of whether the fitted rates hold beyond the training data.

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Editorial analysis

A structured set of objections, weighed in public.

Desk editor's note, referee report, and a circularity audit.

Desk Editor's Note

read the letter

Short version: this is a useful, mostly careful experimental paper, but the flashiest number in the abstract—90% in 10 μs—is a model extrapolation to an unmeasured power point, not a direct measurement. The 95% in 300 μs is on firmer ground but carries the same readout-correction assumptions.

What's genuinely new: for shallow NVs (5–15 nm), the authors show that simultaneous green and NIR light prepares NV− to ~95% in a few hundred microseconds, far faster than the millisecond-scale times Hopper et al. reported for bulk NVs. They fit a two-state rate model to their transients, then validate it on two held-out power combinations (Fig. 2c). That out-of-sample check is good practice and gives me real confidence in the model's basic form. The measured spin contrast and readout-noise improvements are solid, not modeled. The parameter maps in Fig. 3 will be practically useful for people choosing operating conditions.

Soft spots, in proportion. The 90%-in-10-μs claim comes from the model colormap at 4 mW NIR and 39 μW green, a point that never appears in the fitted or verified datasets. If the ionization/recombination rates have a power dependence not captured by the model—say, a process turning on above the fitted NIR range—that point could shift. The same exponential readout extrapolation to t_intg=0 and the assumed initial state ρ0≈0.72 underlie both headline numbers; starting from NV0 would lengthen the time to threshold. The 300 μs/95% claim is less exposed because it sits near measured 181 μs data, but it's still read off the model. There's also a small internal inconsistency: the abstract says 1 mW NIR for the 300 μs point, while the intro says 0.75 mW. Finally, no data or code are deposited, so the fitted rates can't be independently re-evaluated. These are fixable issues, not fundamental flaws.

Who's this for? Experimental NV-sensing groups, especially those doing shallow-NV work and multi-point covariance magnetometry. It's a practical improvement, not a new mechanism. The modeling is transparent and the validation step is more than most papers in this area do. The main weakness is that the abstract oversells a model prediction as a demonstrated result.

Recommendation: send it to peer review. A good referee should ask for the 10 μs point to be measured directly, or the claim softened to "model predicts," and should push for data deposition. With those changes this becomes a solid, citable paper.

Referee Report

3 major / 6 minor

Summary. This paper reports a protocol for charge-state initialization of shallow nitrogen-vacancy (NV) centers using simultaneous green (520 nm) and near-infrared (905 nm) illumination. By measuring charge-state populations after multicolor initialization and fitting a two-state rate-equation model, the authors identify parameter regimes where the negative charge population reaches 95% within 300 μs at modest powers (1 mW NIR, 10 μW green) and predict 90% initialization in as little as 10 μs at higher NIR power (4 mW, 39 μW green). The model is validated on two independent power combinations in Fig. 2(c), and the authors further demonstrate a 12.5% increase in spin contrast and a reduction in readout noise. Sensitivity calculations for covariance magnetometry show that the protocol could shorten total experiment times for multi-point correlator measurements.

Significance. If the results hold, this is a practically useful advance: it offers a fast, low-power route to near-unity charge initialization of shallow NV centers, directly addressing a dominant SPAM error source in nanoscale sensing. The out-of-sample validation in Fig. 2(c) is a notable strength, and the sensitivity analysis connects the charge fidelity to a concrete metrological benefit. However, the headline speed claims—especially the 10 μs / 90% point—are model extrapolations to power combinations not directly measured, and the readout correction relies on an exponential extrapolation whose validity across the full parameter space is not fully demonstrated. The absence of deposited data and code further limits independent verification.

major comments (3)

[Abstract, Section II.B, Fig. 3] The claim that 'the time to 90% charge initialization can be as fast as 10 μs for 4 mW of near-infrared and 39 μW of green illumination' is not directly supported by any displayed measurement at that parameter combination. The model in Eq. (2) is fitted to data at fixed powers in Fig. 2(a,b) and validated only at two new points in Fig. 2(c); the specific point (n=4 mW, g=39 μW) is not among them and appears to be outside the fitted range. Since this is a central headline claim, the authors should either provide a direct measurement at (or near) this point or explicitly label the 10 μs value as a model prediction and temper the abstract and conclusion accordingly.
[Section II.A, Fig. 1(e)] The true initialization fidelity is obtained by extrapolating the measured [NV-] to t_intg=0 using an exponential fit to the destructive-readout decay. This correction is applied to all subsequent data, including the values used to fit the rate model and the values shown in Figs. 2 and 3. However, the manuscript does not demonstrate that the decay is single-exponential for all initialization conditions, nor that the decay rate is independent of the green and NIR powers used. If, for example, the multicolor initialization leaves the NV in a different internal state that alters the two-photon ionization rate during readout, the extrapolation could systematically bias the reported fidelities. Please provide evidence that the exponential extrapolation is robust across the parameter range studied, or quantify the sensitivity of the headline claims to the assumed decay form.
[Data and Code Availability, Supplementary Material] The central quantitative results—the fitted rates γ_i and γ_r and the parameter maps in Fig. 3—depend on the full rate expressions, which are only in the Supplementary Material, and the data are available only 'upon reasonable request'. No data or code are deposited. Because the 95%-in-300 μs and 90%-in-10 μs claims are model extrapolations, independent re-evaluation of the fitting and validation procedure is essential. I ask that the authors deposit the raw charge-population datasets and the fitting code, or at minimum include the full rate expressions and fitting procedure in the main text so that the extrapolation can be scrutinized without correspondence with the authors.

minor comments (6)

[Acknowledgements] There is a typo in the acknowledgment: 'Contract Nop.' should read 'Contract No.'.
[Throughout] The notation for the integration time is inconsistent: the text uses both t_intg and tintg. Please unify to a single symbol.
[Fig. 1(e)] The axes of Fig. 1(e) are not described in the caption; please include axis labels and units.
[Section II.B] The statement that 5–10 μs initialization is 'comparable to the sequence length for conventional NV center sensing protocols' would benefit from a specific reference to the typical green-pulse duration used in such protocols, rather than a general citation.
[Section II.D, Fig. 5] The claim of 'a 5-fold decrease in overall time' should specify whether this refers to the 3-point correlator at a particular target field amplitude, and should state the comparison conditions (e.g., same target σ_B,min).
[Conclusion] The conclusion restates the 10 μs / 90% figure without the qualifier that it is a model prediction; this should be revised for consistency with the requested reframing in the major comments.

Circularity Check

0 steps flagged · score 0.0 of 10

No significant circularity: the two-state model is fit to training data, verified out-of-sample, and the 10 μs headline is a disclosed model extrapolation, not a fitted parameter presented as an independent prediction.

full rationale

Walking the derivation chain: the rate-equation model (Eqs. 1-2) is fit to [NV−](tON) curves in Fig. 2(a,b). The model is then checked against two new power combinations in Fig. 2(c) that were not used in the fit. The parameter-space maps in Fig. 3 and the '10 μs / 90%' statement follow from the same fitted model, so they are extrapolations rather than direct measurements. This is a validation gap, but not circularity: the paper does not use the 10 μs point to justify the model, does not fit a parameter to that point, and does not claim the point was measured; it explicitly says the model is 'used' to make the map. The out-of-sample agreement is independent evidence for the model's power dependence. The 95%/300 μs claim sits close to a measured 0.95 at 181 μs. The exponential t_intg→0 readout correction and assumed ρ0=0.72 could bias absolute fidelities, but they are not inputs to the claimed prediction by construction. Self-citations (Refs. 11, 12, 21, 23) support sample preparation, sensitivity formulas, and applications; none is load-bearing for the charge-initialization result. No circular step can be exhibited.

Assumptions & free parameters 2 free parameters · 4 assumptions · 0 invented entities

The paper introduces no new physical entities. Its quantitative claims rest on a two-state rate model with parameters fitted to experimental data; the headline '10 μs' value is a model extrapolation.

free parameters (2)

Effective ionization and recombination rates γ_i, γ_r (or γ_r/γ_tot and γ_tot) = Not numerically reported; fitted per power level
These are solved by fitting the two-state model to the population data in Fig. 2(a,b). They directly determine the model maps in Fig. 3, including the '10 μs to 90%' prediction.
Initial negative-charge population ρ0 = 0.72 (measured from green-only initialization)
Used as the starting population in the model fits; it is measured, not chosen freely, but still an input to the model that could influence the fitted rates.

assumptions (4)

domain assumption The two-state rate-equation model (Eq. 1-2) captures NV charge cycling under multicolor illumination.
Adopted from Hopper et al. [8] and used throughout Section II.B; no validation of the two-state truncation is provided.
domain assumption Charge readout under orange illumination is destructive and follows an exponential decay due to two-photon ionization.
Used to extrapolate [NV-] to t_intg=0 (Fig. 1e); the exponential form is assumed, not derived.
domain assumption The fitted rates are constant for a given power combination and do not change during the illumination pulse.
Required for the closed-form solution in Eq. 2 and for extrapolation across the parameter space in Fig. 3.
standard math The NV centers are single, isolated emitters and the ensemble statistics are described by Poisson distributions of photon counts.
Used for the double-Poisson fits in Fig. 1(d) to extract [NV-].

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Cite this review

Pith. "Pith review of High-Efficiency, High-Fidelity Charge Initialization of Shallow Nitrogen Vacancy Centers in Diamond." pith.science (2026). https://pith.science/paper/EO6T6QO7

@misc{pith2026250600707,
  author       = {Pith},
  title        = {Pith review of: High-Efficiency, High-Fidelity Charge Initialization of Shallow Nitrogen Vacancy Centers in Diamond},
  year         = {2026},
  howpublished = {\url{https://pith.science/paper/EO6T6QO7}},
  note         = {Machine review of arXiv:2506.00707}
}

read the original abstract

Nitrogen vacancy (NV) centers in diamond exhibit long spin coherence times, optical initialization, and optical spin readout under ambient conditions, making them excellent quantum sensors. However, the conventional scheme for charge state initialization based on off-resonant green excitation results in significant state preparation errors, typically around 30%. One method for improving charge state initialization fidelity is to use multicolor excitation, which has been demonstrated to achieve a near-unity preparation fidelity for bulk NV centers by using a few milliseconds of near-infrared (5 mW) and green (10 {\mu}W) excitation. The translation of such schemes to NV centers near the diamond surface with higher efficiency optical pumping would enable myriad tasks in nanoscale sensing. Here, we demonstrate a protocol for efficient charge initialization of shallow NV centers between 5 nm and 15 nm from the diamond surface. By carefully studying the charge dynamics of shallow NV centers, we identify a region of parameter space that allows for near-unity (95%) charge initialization within 300 {\mu}s of near-infrared (1 mW) and green (10 {\mu}W) excitation. The time to 90% charge initialization can be as fast as 10 {\mu}s for 4 mW of near-infrared and 39 {\mu}W of green illumination. This fast, efficient charge initialization protocol will enable nanoscale sensing applications where state preparation errors currently prohibit scaling, such as measuring higher-order multi-point correlators.

Figures

Figures reproduced from arXiv: 2506.00707 by the authors.

**Figure 2.** FIG. 2 [PITH_FULL_IMAGE:figures/full_fig_p003_2.png] view at source ↗

**Figure 4.** FIG. 4 [PITH_FULL_IMAGE:figures/full_fig_p004_4.png] view at source ↗

Figures from the paper (2 more)

**Figure 3.** Figure 3: FIG. 3 [PITH_FULL_IMAGE:figures/full_fig_p004_3.png]

**Figure 5.** Figure 5: FIG. 5 [PITH_FULL_IMAGE:figures/full_fig_p004_5.png]

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Reference graph

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Pith tools

Reviewed August 7, 2026 · model on record in the stance chip above.

[1] [1]

Childress and R

L. Childress and R. Hanson, Diamond nv centers for quan- tum computing and quantum networks, MRS bulletin38, 134 (2013)

work page 2013

[2] [2]

M. W. Doherty, N. B. Manson, P. Delaney, F. Jelezko, J. Wrachtrup, and L. C. Hollenberg, The nitrogen-vacancy colour centre in diamond, Physics Reports528, 1 (2013)

2013

[3] [3]

Schirhagl, K

R. Schirhagl, K. Chang, M. Loretz, and C. L. Degen, Nitrogen- vacancy centers in diamond: nanoscale sensors for physics and biology, Annual review of physical chemistry65, 83 (2014)

work page 2014

[4] [4]

Aslam, G

N. Aslam, G. Waldherr, P. Neumann, F. Jelezko, and J. Wrachtrup, Photo-induced ionization dynamics of the ni- trogen vacancy defect in diamond investigated by single-shot charge state detection, New Journal of Physics15, 013064 (2013)

work page 2013

[5] [5]

Mahdia, J

M. Mahdia, J. Allred, Z. Yuan, J. Rovny, and N. P. De Leon, Probing itinerant carrier dynamics at the diamond surface using single nitrogen vacancy centers, Applied Physics Letters122 (2023)

work page 2023

[6] [6]

A. Wood, A. Lozovoi, R. Goldblatt, C. Meriles, and A. Mar- tin, Wavelength dependence of nitrogen vacancy center charge cycling, Physical Review B109, 134106 (2024)

work page 2024

[7] [7]

Wirtitsch, G

D. Wirtitsch, G. Wachter, S. Reisenbauer, M. Gulka, V . Ivády, F. Jelezko, A. Gali, M. Nesladek, and M. Trupke, Exploiting ionization dynamics in the nitrogen vacancy center for rapid, high-contrast spin, and charge state initialization, Physical Re- view Research5, 013014 (2023)

work page 2023

[8] [8]

D. A. Hopper, R. R. Grote, A. L. Exarhos, and L. C. Bas- sett, Near-infrared-assisted charge control and spin readout of the nitrogen-vacancy center in diamond, Physical Review B94, 241201 (2016)

work page 2016