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Small Energy Gap Revealed in CrBr3 by Scanning Tunneling Spectroscopy

T0 review · 5 major / 5 minor · reviewed 2026-08-14 · deepseek-v4-flash

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Pith's one-line read CrBr3's real band gap is 0.57 eV, not the 1.68–2.1 eV value assumed for decades.

desk verdict A plausible direct STS measurement of a small gap in CrBr3 that overclaims certainty; the qualitative finding is likely right but the exact value and the 'unambiguous' framing need more controls. read the letter →

arxiv 1909.00074 v2 pith:4KDLA3XH submitted 2019-08-30 cond-mat.mtrl-sci

Dinesh Baral , Zhuangen Fu , Andrei S. Zadorozhnyi , Rabindra Dulal , Aaron Wang , Narendra Shrestha , Uppalaiah Erugu , Jinke Tang
show 3 more authors
Yuri Dahnovsky Jifa Tian TeYu Chien
This is my paper · ORCID
classification cond-mat.mtrl-sci
keywords CrBr3scanningtunnelingspectroscopybandgapvanderWaalsmagnetdI/dVDFT+U2Dferromagnetismlayeredsemiconductor
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

This paper claims that the layered magnetic semiconductor CrBr3 has a far smaller electronic energy gap than the 1.68–2.1 eV range assumed from optical absorption for decades. Using scanning tunneling spectroscopy on exfoliated flakes at 77 K, the authors find two intrinsic peaks flanking the Fermi level, one in the conduction band at 0.25 eV and one in the valence band at −0.31 eV, giving a peak-to-peak gap of 0.57 ± 0.04 eV and an onset gap of 0.29 ± 0.05 eV. If correct, the result settles a controversy opened by a 1.35 eV photoluminescence feature and changes how the material's optical, magnetic, and transport data are interpreted. The paper also proposes a DFT+U parameter set (U = 5 eV, J = 3 eV) that reproduces the small gap.

What carries the argument

The load-bearing measurement is the normalized differential conductance spectrum dI/dV, which is proportional to the local density of states, taken with a lock-in amplifier on thick exfoliated CrBr3 flakes on HOPG at 77 K. The normalization follows a broadening formula (Eq. 1) that suppresses noise without shifting peak positions. The argument is carried by the multi-peak spectrum: nine reproducible peaks, four on the conduction side and five on the valence side, whose pairwise energy differences line up with decades of optical absorption, Kerr rotation, reflection, and photoluminescence data. The near-Fermi pair, peak 1 at 0.25 eV and peak a at −0.31 eV, fixes the claimed small gap, while DFT+U calculations with U = 5 eV and J = 3 eV open a gap of similar size and leave CrBr3 gapless when U = J = 0.

What would settle it

Measure STS on the same material under deliberately varied junction conditions and on an insulating substrate: if the zero-bias suppression and the 0.57 eV peak separation disappear or shift when tip-sample distance, bias set point, or substrate is changed, the small gap is a tunneling artifact. Independently, infrared absorption or photoemission that finds no optical or filled-state onset near 0.3–0.6 eV would contradict the claim.

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Extended reading notes

Core claim

The central claim is that bulk CrBr3 is a small-gap semiconductor with an electronic band gap of 0.57 ± 0.04 eV, determined as the separation between the two dI/dV peaks nearest the Fermi level measured at 77 K. A more conservative reading of the same spectra puts the onset of tunneling conductance at 0.29 ± 0.05 eV. The authors argue that the two near-zero peaks are intrinsic band edges, not defect states, because the spectra are reproducible across locations and the atomic-resolution topography is defect-free. They further show that the energy differences between all other conduction-band and valence-band peaks in the dI/dV spectrum match every reported optical transition from 1.35 eV to 3.8 eV, which they take as evidence that the measured spectrum faithfully represents the density of states.

Load-bearing premise

The claim stands or falls on the assumption that the two dI/dV peaks near zero bias are the intrinsic band edges of bulk CrBr3 and that the suppressed conductance between them is the true band gap, not an artifact of tip-induced band bending, the low sample conductivity, or the HOPG substrate.

Editorial extensions

If this is right

  • The long-quoted 1.68 eV absorption feature becomes an inter-band transition between deeper peaks rather than the fundamental band gap, so optical assignments for CrBr3 need revision.
  • DFT calculations that force a gap near 1.7–2.1 eV require recalibration, and the U = 5 eV, J = 3 eV combination offers a concrete starting point for CrBr3.
  • A 0.29 eV onset gap should be observable in infrared absorption or electrical transport, giving independent experimental checks.
  • Because all reported optical transitions match the measured peak pairs, the electronic density of states appears essentially unchanged across the magnetic transition at 32 K, so spin ordering does not strongly reorganize the band structure.
  • Magnetic and optical interpretations that assume a large gap, such as exciton binding energies or d-d versus charge-transfer assignments, need re-evaluation.

Reading between the lines

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

  • If the small gap is intrinsic, CrBr3 may behave more like a narrow-gap semiconductor in transport and optical devices than previously assumed, with thermal activation across 0.3–0.6 eV accessible in ordinary experiments; the paper does not pursue this consequence.
  • A testable extension is to measure STS on CrBr3 flakes on an insulating substrate and with varied tip-sample distances to see whether the zero-bias suppression and 0.57 eV peak separation persist; the paper does not model junction effects such as tip-induced band bending.
  • The assignment of the 1.35 eV photoluminescence to a peak-pair difference rather than the band edge suggests that PL-based gap estimates for other chromium trihalides may similarly need to be re-examined.
  • If confirmed by infrared absorption or photoemission, the 0.29 eV onset would place CrBr3 alongside other narrow-gap layered magnets and could change predictions for magnetotransport and spintronic applications.
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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

5 major / 5 minor

Summary. The manuscript reports scanning tunneling microscopy and spectroscopy (STM/S) on exfoliated CrBr3 flakes on HOPG at 77 K, together with LDA+U calculations. The authors identify nine reproducible peaks in the dI/dV spectra and interpret the two closest to the Fermi level (peak 1 at +0.25 eV and peak a at -0.31 eV) as conduction and valence band edges, implying a peak-to-peak gap of 0.57 ± 0.04 eV and an onset gap of 0.29 ± 0.05 eV. This is claimed to settle a long-standing controversy about the bulk energy gap of CrBr3, which was previously believed to lie between 1.68 and 2.1 eV. The authors support their assignment by matching the remaining peak pairs to published optical transition energies and by a DFT+U calculation using U = 5 eV and J = 3 eV.

Significance. If the interpretation is correct, the result is significant because it revises the fundamental gap of CrBr3 downward by roughly 1 eV, with implications for the interpretation of optical and transport measurements and for the choice of DFT parameters for this family of 2D magnets. The strengths of the paper are that the STS data are spatially reproducible, measured on exfoliated crystals with atomic-resolution imaging, and the manuscript explicitly reports key limitations, including the absence of degassing and the poor conductivity of the flakes. The comparison with reported optical transitions is a useful consistency check. However, the central numerical claim is currently ambiguous (two different gap values are both called the energy gap), and the evidence does not yet eliminate junction/transport artifacts, so the paper overstates the certainty of an 'unambiguous determination.'

major comments (5)
  1. [Results and Discussions, Fig. 2(c) and Conclusions] The manuscript reports two different quantities as 'the energy gap' of CrBr3: the peak-to-peak separation of peaks 1 and a (0.57 ± 0.04 eV) and the onset of the dI/dV signal near zero bias (0.29 ± 0.05 eV). These two numbers are not interchangeable: the peak-to-peak separation in STS is a measure of the energetic distance between two maxima in the LDOS and is generally not equal to the band gap, whereas the onset is the physically relevant gap. The abstract and conclusion emphasize the 0.57 eV value, but the body text gives no rigorous extraction criterion for the onset gap, and the Feenstra normalization with ΔV values of 0.15–0.9 V can shift the apparent onset. This ambiguity is load-bearing because the paper's central claim is the unambiguous determination of a small gap.
  2. [Results and Discussions, Fig. 2(c)] The inference that the suppression of dI/dV between peaks 1 and a is the intrinsic band gap is not controlled against junction/transport artifacts. The manuscript itself notes the measurements are noisy because of the poor conductivity of CrBr3 and the absence of degassing (p. 6-7), and the monolayer spectrum is explicitly unusable for gap extraction because of the HOPG contribution (Fig. 4(c)). On such a sample, tip-induced band bending, a bias-dependent series resistance of the flake, or the underlying HOPG layer can suppress dI/dV near zero bias even if the true DOS gap is different. No measurement at constant height with varied tip-sample separation, no flake-thickness series, and no temperature dependence across TC = 32 K are provided to rule out these effects. The paper's claim of an 'unambiguous' small gap therefore goes beyond the current evidence.
  3. [Results and Discussions, Fig. 3(a)] The LDA+U calculation is presented as confirming the small gap, but the parameters U = 5 eV and J = 3 eV are selected specifically because they reproduce the measured spectrum ('A combination of U = 5 and J = 3 was chosen as it fits the best to the experimental results'). This is circular and cannot serve as independent support for the measured gap. At most, it demonstrates that a plausible parameter set yields a similar gap magnitude; the DFT results should be presented as a model whose parameters are set by the STS data, not as a confirmation.
  4. [Results and Discussions, Table 2] The optical-transition matching is post-hoc and combinatorially permissive. With nine measured peaks, there are numerous possible conduction-valence band pairs, and the table selects one pair for each reported transition without a statistical assessment of how likely a match is by chance. For example, the 1.35 eV PL feature is assigned to pair 2-a with a separation of 1.27 ± 0.05 eV, which deviates by 80 meV from the reported PL energy; this discrepancy is not discussed. The matching therefore does not provide strong independent evidence that peaks 1 and a are the band edges.
  5. [Experiments and Methods; Fig. S2, Fig. S3, Table S1] The manuscript repeatedly relies on the supplementary figures and table (Fig. S2(d), Fig. S3(b), Fig. S3(c), Table S1) for the raw dI/dV spectra, the Gaussian peak fitting, and the complete peak-pair list. None of these were included with the submitted manuscript, so the quantitative peak positions and uncertainties, and hence the central gap determination, cannot be independently verified. The authors should submit the supplementary material for review or present the essential data in the main text.
minor comments (5)
  1. [Abstract and Methods] Abstract: 'pyropytic graphite' should be 'pyrolytic graphite'; in the Methods section, 'PMDS' should be 'PDMS'.
  2. [Table 1] The header 'Valance band' should be 'Valence band'.
  3. [References] Reference [48] is incomplete: 'Phys. Rev. B 50, (1994)' lacks the article/page information.
  4. [Fig. 2(c) and Results] The onset gap of 0.29 ± 0.05 eV is reported without a description of the onset criterion (e.g., threshold crossing, linear extrapolation); this should be specified in the figure caption or Methods.
  5. [Conclusions] The statement that 'the DOS is not sensitive to the magnetic phase transition' is not directly tested because all dI/dV spectra were taken at 77 K, well above TC = 32 K; this should be worded as an inference from the optical comparison.

Circularity Check

1 steps flagged · score 3.0 of 10

STS gap determination is self-contained; DFT+U agreement is circular because U and J were fitted to the measured gap.

  1. fitted input called prediction [Experiments and Methods; Results and Discussions, DFT+U paragraph and Conclusions]
    "A combination of U = 5 and J = 3 was chosen as it fits the best to the experimental results. ... By varying a wide range of J and U values (J varied from 0 to 3 eV while U varied from 0 to 11 eV), it is found that the energy gap in the DOS calculated with J = 3 and U = 5 agrees reasonably well with the measured dI/dV spectrum. ... The DFT calculation along with the observed dI/dV spectra confirms that CrBr3 has a smaller energy gap than ever reported."

    The DFT+U parameters (U = 5 eV, J = 3 eV) were selected to reproduce the STS-measured energy gap, so the subsequent statement that 'the DFT calculation along with the observed dI/dV spectra confirms' the small gap is not an independent confirmation. The calculated gap agrees with the measured dI/dV gap because the calculation was tuned to that gap. This circularity affects only the supporting DFT comparison; the primary STS gap value itself is obtained directly from dI/dV spectra and does not depend on the DFT fit.

full rationale

The paper's central claim, that the peak-to-peak energy gap of CrBr3 is 0.57 ± 0.04 eV (onset 0.29 ± 0.05 eV), is derived directly from measured dI/dV spectra. No fitted parameter is used to produce this value; the Gaussian peak fitting only extracts peak positions from the data, and the reported uncertainty reflects the scatter across eight spectra. The defect-intrinsic argument is based on spatial reproducibility and atomic-resolution imaging, which are experimental controls rather than fitted inputs. The matching of dI/dV peak-pair energies to previously reported optical transitions is a post-hoc consistency check against external literature values, not a derivation of the gap from those values. The one clearly circular step is the DFT+U section: the authors sweep U and J and choose U = 5, J = 3 'as it fits the best to the experimental results,' then present the resulting agreement as confirmation of the small gap. This is a fitted input called a prediction, and it weakens the DFT corroboration, but it is not load-bearing for the central STS measurement. The paper's experimental gap conclusion would stand even if the DFT comparison were removed entirely. Hence a modest circularity score of 3 is appropriate: the main result is self-contained, while the DFT confirmation reduces to a fit.

Assumptions & free parameters 3 free parameters · 4 assumptions · 0 invented entities

The central claim does not rely on invented entities. Two on-site correlation parameters (U, J) are fitted to the experimental gap, and the resulting DOS is used as confirmation, which limits the independent value of the DFT part. The normalization broadening parameters are chosen by hand. The interpretation relies on several domain assumptions, one of which (negligible tip effects) is not explicitly justified.

free parameters (3)
  • U (on-site Coulomb repulsion) = 5 eV
    Chosen to match the measured dI/dV gap; varying U changes the calculated gap.
  • J (on-site exchange interaction) = 3 eV
    Chosen together with U to reproduce the measured gap.
  • Delta V normalization broadening = 0.15, 0.25, 0.35, 0.9 V
    Chosen by hand for each bias range to reduce noise; authors claim no effect on peak positions.
assumptions (4)
  • domain assumption dI/dV signal is proportional to the local density of states of the sample
    Standard STS assumption, referenced to Feenstra (ref 47).
  • domain assumption The peaks near the Fermi level are intrinsic electronic states of CrBr3 and not defect states
    Authors argue reproducibility and defect-free atomic resolution, but this is an assumption entering the interpretation of Fig. 2(c).
  • domain assumption The measured small gap is not significantly distorted by tip-induced band bending or sample series resistance
    No analysis of junction effects is provided for the poorly conductive CrBr3 flakes; this is an unflagged critical assumption.
  • domain assumption DFT+U with LDA pseudopotentials and U/J applied to Cr d orbitals is an adequate model for the CrBr3 electronic structure
    Standard but approximate; U and J are material-specific fitted parameters.

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Pith. "Pith review of Small Energy Gap Revealed in CrBr3 by Scanning Tunneling Spectroscopy." pith.science (2026). https://pith.science/paper/4KDLA3XH

@misc{pith2026190900074,
  author       = {Pith},
  title        = {Pith review of: Small Energy Gap Revealed in CrBr3 by Scanning Tunneling Spectroscopy},
  year         = {2026},
  howpublished = {\url{https://pith.science/paper/4KDLA3XH}},
  note         = {Machine review of arXiv:1909.00074}
}
abstract

CrBr$_{3}$ is a layered van der Waals material with magnetic ordering down to the 2D limit. For decades, based on optical measurements, it is believed that the energy gap of CrBr$_{3}$ is in the range of 1.68-2.1 eV. However, controversial results have indicated that the band gap of CrBr$_{3}$ is possibly smaller than that. An unambiguous determination of the energy gap is critical to the correct interpretations of the experimental results of CrBr$_{3}$. Here, we present the scanning tunneling microscopy and spectroscopy (STM/S) results of CrBr$_{3}$ thin and thick flakes exfoliated onto pyropytic graphite (HOPG) surfaces and density functional theory (DFT) calculations to reveal the small energy gap (peak-to-peak energy gap to be 0.57 eV $\pm$ 0.04 eV; or the onset signal energy gap to be 0.29 $\pm$ 0.05 eV from dI/dV spectra). Atomic resolution topography images show the defect-free crystal structure and the dI/dV spectra exhibit multiple peak features measured at 77 K. The conduction band - valence band peak pairs in the multi-peak dI/dV spectrum agree very well with all reported optical transitions. STM topography images of mono- and bi-layer CrBr$_{3}$ flakes exhibit edge degradation due to short air exposure (~15 min) during sample transfer. The unambiguously determined small energy gap settles the controversy and is the key in better understanding CrBr$_{3}$ and similar materials.

Figures

Figures reproduced from arXiv: 1909.00074 by the authors.

Figure 2
Figure 2. a, The top view of the crystal structure of CrBr3 (ML: monolayer, BL: bilayer). In the ML structure, the unit cell is indicated with the thick bonds. In the BL structure, the green circles represent Cr atom at the top layer, the blue circles represent Cr at the bottom layer and the sky-blue circles represent Cr atoms appeared at both layers. The thick blue hexagon shows the overlaid structure used in b (the magnifie… view at source ↗

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