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REVIEW 3 major objections 5 minor 30 references

Updated line list for the principal isotopologue of carbon monoxide

T0 review · 3 major / 5 minor · reviewed 2026-08-07 · deepseek-v4-flash

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Pith's one-line read The paper argues that the previously used 1-0 band measurements for CO are systematically wrong, removes them from the fit, and produces an updated line list with new predictions.

desk verdict A careful, reproducible update of the CO line list whose central 1-0 prediction is conditional on an unpublished HITRAN2024 result; worth reviewing, but not ready to adopt. read the letter →

arxiv 2506.12216 v1 pith:CEPANRHE submitted 2025-06-13 physics.chem-ph astro-ph.EPastro-ph.SRphysics.ao-ph

Vladimir G. Ushakov , Emile S. Medvedev This is my paper
classification physics.chem-phastro-ph.EPastro-ph.SRphysics.ao-ph
keywords carbonmonoxidelinelistdipole-momentfunctionovertoneintensities1-0band8-0predictionsHITRANNIDL
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 updates the line list for the principal isotopologue of carbon monoxide by arguing that the two older fundamental-band datasets are systematically wrong, because they conflict with new high-precision measurements of the 3-0 and 7-0 overtone bands. It re-fits the semi-empirical dipole-moment function after excluding all 1-0 band data, and computes a new line list that describes all remaining accepted experimental and theoretical data within uncertainties. A sympathetic reader would care because the 1-0 band is the strongest CO absorption used in atmospheric remote sensing, and the updated predictions move back toward HITRAN2016, calling into question the 2% downward revision adopted in HITRAN2020. The paper also provides explicit predictions for the still-unmeasured 8-0 band and for the 1-0 band, which the announced but not yet published HITRAN2024 fundamental-band data can test.

What carries the argument

The load-bearing object is the irregular dipole-moment function (DMF), a semi-empirical function $d(r)$ giving the electric dipole moment of CO as a function of internuclear distance; it is fitted to transition dipole moments converted from measured line intensities and constrained by ab initio points and by the limiting behavior $d(r)\propto r^3$ at $r\to 0$ and $d(r)\approx d_4 r^{-4}$ at $r\to\infty$. It carries the argument because line intensities are integrals of this function with vibrational wave functions, and high-overtone intensities are extremely sensitive to its analytic behavior. The paper fits three models with different analytical properties, including a rational DMF with five pairs of complex-conjugate poles, and selects the irregular DMF because it stays smooth in the complex plane and reproduces the NIDL, the overtone intensity-decay law, while the regular DMF does not.

What would settle it

A direct high-precision measurement of several CO fundamental-band line intensities at the 0.1-0.5% level would settle the question: if the measured values land about 2% below their HITRAN2016 values, near HITRAN2020, then excluding the older 1-0 data was unjustified. Publishing and comparing the announced HITRAN2024 cold- and hot-fundamental intensities to Table 2 would provide essentially the same test.

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Extended reading notes

Core claim

The authors claim that the new sub-permille 3-0 measurements and the first 7-0 measurements cannot be reconciled with the two fundamental-band datasets used in their previous fits. On that basis they remove all 1-0 data from the fitting set, sharply increase the uncertainties assigned to ab initio dipole-moment points, and re-fit three model dipole-moment functions to the remaining data. They conclude that the re-fit describes all accepted data well, that the irregular and rational dipole-moment functions give mutually consistent predictions, and that the irregular dipole-moment function yields a 1-0 band in agreement with HITRAN2016 to about 0.5%, meaning HITRAN2020's 1.02 scaling was driven by flawed measurements. The paper presents new 1-0 and 8-0 intensity tables and a full updated line list.

Load-bearing premise

The claim rests on treating the older 1-0 band measurements as systematically wrong and on trusting the announced but not yet published HITRAN2024 fundamental-band measurements; if those older data are actually right, or the new announcement follows HITRAN2020, the re-fitted dipole-moment function is biased and its 1-0 prediction fails.

Editorial extensions

If this is right

  • If the updated line list is correct, the 1-0 CO band intensities should match HITRAN2016 values within about 0.5%, and HITRAN2020's uniform 2% reduction should be reversed.
  • The still-unmeasured 8-0 band now comes with explicit intensity predictions, enabling a direct test when high-overtone measurements reach that band.
  • Because the irregular and rational DMFs agree within about 1% for the 7-0 band and about 2% for the 8-0 band far from anomalies, the predicted intensities are largely independent of the DMF parameterization.
  • The regular DMF, although it fits the measured low bands, violates the NIDL and behaves non-physically in the complex plane, so it should not be used for extrapolated overtone intensities.

Reading between the lines

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

  • If the 1-0 exclusion survives the publication of the HITRAN2024 fundamental-band data, databases that adopted the 2% downward scaling in HITRAN2020 would need revision, which would propagate into atmospheric retrievals that use CO columns.
  • The agreement of two analytically very different DMFs after the new constraints suggests a practical validation recipe for overtone line lists: predictive reliability is indicated when structurally unrelated fitting functions agree outside the fitted region.
  • A natural extension is to repeat the fit with the announced hot-fundamental-band measurements, which would test whether the same dipole-moment function also works for vibrationally excited lower states.
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Editorial analysis

A structured set of objections, weighed in public.

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

Referee Report

3 major / 5 minor

Summary. The paper updates the authors' 2022 CO line list by refitting the semi-empirical irregular dipole-moment function (DMF) to a data set that includes new high-precision measurements of the 3-0 (Hodges25, Bielska22) and 7-0 (Balashov23) bands, while excluding all previously used 1-0 band intensity data (Zou02, Devi18). The authors report that the new 3-0 and 7-0 data cannot be fitted simultaneously with the old 1-0 data, and after 'try[ing] them one by one' they conclude that the 1-0 data are systematically wrong. The final Fit 2 uses three model DMFs (irregular, rational, and regular) with increased ab initio uncertainty bars; the irregular and rational DMFs give consistent predictions for the unobserved 1-0 and 8-0 bands. The paper claims excellent agreement with independent high-level ab initio calculations for the 3-0 band and predicts 1-0 intensities close to HITRAN2016, with a full line list and code provided as supplementary material.

Significance. If the central claim is correct, the updated line list represents a meaningful improvement over the authors' previous Medvedev&Ushakov22 list: the 1-0 band intensities would be ~2% higher than HITRAN2020, reverting toward HITRAN2016, and the new 3-0 and 7-0 data would be reproduced within experimental uncertainties. The paper is also of practical value to the spectroscopic database community because it provides concrete predictions for the 1-0 and 8-0 bands that can be tested once the announced HITRAN2024 fundamental-band measurements are published. The authors are to be credited for releasing the FORTRAN code and full line list, and for comparing against independent high-level ab initio calculations (SUCL) for the 3-0 band, which shows agreement to ~0.05%. However, the significance of the work is tempered by the fact that the load-bearing exclusion of all 1-0 data rests on an unpublished announcement (Ref. [9]) and on a data-dependent fitting decision, rather than on a robust outlier or systematic-error analysis.

major comments (3)
  1. [Section 3, final Fit 2] The exclusion of all 1-0 band data (both Zou02 and Devi18) is the central decision of the paper, yet the justification is essentially a one-by-one trial ('we tried them one by one and found that these were the data of Zou02') supplemented by an unpublished HITRAN2024 announcement (Ref. [9], 'in preparation'). The reasoning is circular in a practical sense: the 1-0 data are removed because they cannot be fitted simultaneously with the 3-0/7-0 data, and the resulting fit is then used (Table 1, Fig. 12) to assert that the removed data are systematically wrong. To make this load-bearing claim credible, the paper should provide a quantitative outlier analysis (e.g., standardized residuals, influence diagnostics, or a test of consistency with the 2-0 and other low-overtone bands), and a sensitivity analysis showing how the fitted DMF and 1-0 prediction change when subsets of the 1-0 data are retained. The paper should also explicitly discuss the status of Ref. [9] as unpublished and explain what independent information it provides beyond the raw statement of agreement with HITRAN2016.
  2. [Section 5, Table 2] The predicted 1-0 and 8-0 band intensities are quoted to five or more significant digits (e.g., S1-0 = 9.6582E-20 cm/molecule) without any uncertainty estimate. Given that the DMF parameters are fitted with finite precision and that the exclusion of the 1-0 data is contested, the headline predictions need an error budget. The consistency between the irregular and rational DMFs (within ~1% for 7-0 and ~2% for 8-0) is useful but does not capture systematic errors from the data-selection decision or from the ad hoc inflation of ab initio uncertainties. The authors should report at least a conservative uncertainty on the tabulated S1-0 and S8-0 values, ideally propagating fit uncertainties and showing the spread among acceptable DMF models.
  3. [Section 3, Fit 1] The treatment of ab initio uncertainty is ad hoc: the original uncertainties are multiplied by 200 for r < 0.5 Å and by max(0.3 D, 10σ_orig) for r > 0.5 Å. The choice of these inflation factors is not justified, and no sensitivity test is performed. Since the weight of the theoretical DMF in the fit directly affects the final intensities (the authors themselves show that Fit 0 without such inflation fails to reproduce the 7-0 band), the paper should demonstrate that the final 1-0 and 8-0 predictions are robust to reasonable variations of these inflation factors, e.g., by repeating the fit with σ multiplied by 5, 10, 50, and 200.
minor comments (5)
  1. [Abstract] The abstract states that the line list was 'calculated earlier by the present authors [1, 2] with the irregular dipole-moment function', but the paper actually fits three different model DMFs and only later selects the irregular one; this is slightly misleading.
  2. [Section 2] The sentence 'Both these measurements gave the intensities ... weaker by about 2% than in HITRAN2016' is grammatically awkward and could be clarified, especially regarding the abundance recalculation of the Zou02 data.
  3. [Figure 13] The abbreviation 'SUCL' is used in the caption and text but never explicitly defined; please provide the full name (e.g., 'Semiempirical Universal Carbon monoxide Line list' or similar) at first use.
  4. [Table 1] The footnote 'Possible misprints in the experimental uncertainties of individual lines, e.g. 0.03% for line P11' is vague; please specify which data set this refers to and what action was taken (e.g., were those lines given reduced weight or excluded?).
  5. [Throughout] The acronym 'NIDL' is used without expansion at first occurrence (Figure 14 and text); consider defining it as, e.g., 'nonlinear intensity decay law' to aid the reader.

Circularity Check

0 steps flagged · score 2.0 of 10

No formal circularity: the 1-0 and 8-0 intensities are genuine predictions outside the fit set, though the headline 1-0 result is contingent on excluding the old 1-0 data.

full rationale

The derivation chain is not circular in the formal sense. The DMF parameters are fitted to a dataset that includes the new 3-0 (Hodges25, Bielska22) and 7-0 (Balashov23) intensities and excludes the 1-0 band, so the 3-0/7-0 agreement is a fit result rather than an independent validation. However, the 1-0 and 8-0 predictions are not fit targets, so they are not forced by construction. The exclusion of the 1-0 data is motivated by an internal consistency check ('we tried them one by one and found that these were the data of Zou02') and by the announced but unpublished HITRAN2024 update; this is a data-selection and robustness concern, not a self-referential reduction. No equation defines a predicted quantity in terms of the fitted quantity. The irregular DMF is taken from the authors' prior work, but it is re-fit here against external measurements and cross-checked against the rational DMF and independent ab initio calculations, so the central claim does not reduce to a self-citation. The main caveat is epistemic: the paper's 1-0 prediction depends on the assumption that the old 1-0 measurements are systematically wrong, which is supported only by internal fit residuals and by an as-yet-unpublished database update, not by an independent published measurement. This lowers confidence but does not constitute circularity under the specified patterns.

Assumptions & free parameters 5 free parameters · 4 assumptions · 0 invented entities

The model DMFs carry several fitted parameters not reported in the text, plus an ad hoc inflation of ab initio uncertainties. No new physical entities are introduced. The main assumptions are the validity of the model forms and of the unpublished HITRAN2024 fundamental-band data.

free parameters (5)
  • Irregular DMF parameters = not reported in text
    The irregular dipole-moment function from Refs. [1,2] is refitted in Fit 2 to the modified data set; parameter values are only in the supplementary material.
  • Rational DMF parameters = not reported in text
    Used as a cross-check model, fitted with fixed and floating d4; predicts 1-0 and 8-0 within 2% of the irregular DMF.
  • Regular DMF parameters = not reported in text
    Refitted but rejected for predictions because it violates complex-plane smoothness and the NIDL.
  • d4 asymptotic coefficient = -5.1 DÅ4 fixed; -3.9 DÅ4 when floated for rational DMF
    Asymptotic dipole coefficient at large r; fixed for irregular and regular models, floated for the rational model in Fit 0.
  • Ab initio uncertainty inflation factors = 200 at r<0.5 Å; max(0.3 D, 10 sigma_orig) at r>0.5 Å
    Hand-chosen in Fit 1 to reduce the weight of ab initio DMF points; directly affects the fitted DMF and high-overtone intensities.
assumptions (4)
  • domain assumption The CO potential energy curve from previous work is accurate enough not to be refitted.
    Intensities are computed using the potential from prior studies in the Meshkov22 context; line-list accuracy depends on it, but the paper does not re-evaluate the potential.
  • domain assumption The true dipole-moment function is well represented by one of the three model forms (irregular, regular, rational) with specified asymptotic behavior and no singularities near the integration path.
    The model DMF forms and analyticity requirements are the basis of the fit and of the predictions, introduced in Sections 3 and 4.
  • standard math Quantum mechanical transition dipole moment integrals computed within the Born-Oppenheimer separation give reliable line intensities.
    Standard quantum chemistry applied without proof in the intensity calculations.
  • ad hoc to paper The new HITRAN2024 fundamental-band measurements, announced but not yet published, are correct and agree with HITRAN2016, supporting the exclusion of the 1-0 data.
    This is an unpublished supporting result cited as Ref. [9] 'in preparation'; the paper's 1-0 prediction relies on it.

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Cite this review

Pith. "Pith review of Updated line list for the principal isotopologue of carbon monoxide." pith.science (2026). https://pith.science/paper/CEPANRHE

@misc{pith2026250612216,
  author       = {Pith},
  title        = {Pith review of: Updated line list for the principal isotopologue of carbon monoxide},
  year         = {2026},
  howpublished = {\url{https://pith.science/paper/CEPANRHE}},
  note         = {Machine review of arXiv:2506.12216}
}
read the original abstract

The line list for the principal isotopologue of CO calculated earlier by the present authors [1, 2] with the irregular dipole-moment function (DMF) is updated with use of the recent high-precision measurements in the 3-0 [3, 4] (Bielska et al. 2022, Hodges et al. 2025) and 7-0 [5] (Balashov et al. 2023) bands. The new data came in contradiction with the experimental data on the 1-0 band [6, 7]. Therefore, we performed fitting several model DMFs to the modified original data set of Meshkov et al. [8] by including the new above-referenced data and by excluding the data for the 1-0 band. The updated line list is calculated with the irregular DMF. In particular, excellent agreement with recent high-level ab initio calculations on the 3-0 band [3] is emphasized and predictions for the 1-0 and 8-0 bands are outlined. In the new update of the HITRAN database [9], new high-precision measurements in the cold and hot fundamental bands are announced. When these data are published, they will be compared with the predictions of our new line list.

Figures

Figures reproduced from arXiv: 2506.12216 by the authors.

Figure 1
Figure 1. The DMFs obtained in Fit 0. Solid line, the irregula [PITH_FULL_IMAGE:figures/full_fig_p003_1.png] view at source ↗
Figure 2
Figure 2. Comparison of the calculated (Fit 0) and measured ( [PITH_FULL_IMAGE:figures/full_fig_p004_2.png] view at source ↗
Figure 3
Figure 3. Comparison of the calculated (Fit 0) and measured ( [PITH_FULL_IMAGE:figures/full_fig_p004_3.png] view at source ↗
Figures from the paper (16 more)
Figure 4
Figure 4. Figure 4: Comparison of the calculated (Fit 0) intensities i [PITH_FULL_IMAGE:figures/full_fig_p005_4.png]
Figure 5
Figure 5. Figure 5: The DMFs obtained in Fit 1. Crosses and pluses show t [PITH_FULL_IMAGE:figures/full_fig_p005_5.png]
Figure 6
Figure 6. Figure 6: Comparison of the calculated (Fit 1) and measured i [PITH_FULL_IMAGE:figures/full_fig_p006_6.png]
Figure 7
Figure 7. Figure 7: Comparison of the calculated (Fit 1) and measured i [PITH_FULL_IMAGE:figures/full_fig_p006_7.png]
Figure 8
Figure 8. Figure 8: Comparison of the calculated (Fit 1) intensities i [PITH_FULL_IMAGE:figures/full_fig_p007_8.png]
Figure 9
Figure 9. Figure 9: The DMFs obtained in Fit 2. Notations are the same as [PITH_FULL_IMAGE:figures/full_fig_p008_9.png]
Figure 10
Figure 10. Figure 10: Comparison of the calculated (Fit 2) and measured [PITH_FULL_IMAGE:figures/full_fig_p008_10.png]
Figure 11
Figure 11. Figure 11: Comparison of the calculated (Fit 2) and measured [PITH_FULL_IMAGE:figures/full_fig_p008_11.png]
Figure 12
Figure 12. Figure 12: The 1-0 band predicted by Fit 2. The results for all [PITH_FULL_IMAGE:figures/full_fig_p009_12.png]
Figure 13
Figure 13. Figure 13: Difference between the 3-0 band intensities calcu [PITH_FULL_IMAGE:figures/full_fig_p009_13.png]
Figure 14
Figure 14. Figure 14: Intensities of the v-0 (v = 1,...,40) transitions in the P and R branches in the NIDL coordinates: decimal logarithm of the Einstein-A coefficient vs square root of the upper-state energy, E′ , in units of the vibrational frequency, ω = 2143 cm−1 . The NIDL lines are …
Figure 15
Figure 15. Figure 15: Real and imaginary parts of the DMFs in the complex [PITH_FULL_IMAGE:figures/full_fig_p014_15.png]
Figure 16
Figure 16. Figure 16: Comparison of the 1-0 band intensities calculate [PITH_FULL_IMAGE:figures/full_fig_p014_16.png]
Figure 17
Figure 17. Figure 17: Comparison of the 7-0 band intensities calculate [PITH_FULL_IMAGE:figures/full_fig_p015_17.png]
Figure 18
Figure 18. Figure 18: Comparison of the 8-0 band intensities calculate [PITH_FULL_IMAGE:figures/full_fig_p016_18.png]
Figure 19
Figure 19. Figure 19: The intensities of the 8-0 band predicted with the [PITH_FULL_IMAGE:figures/full_fig_p016_19.png]

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Pith tools

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