Barkhausen noise in the columnar hexagonal organic ferroelectric BTA

Andrey Alekseevich Butkevich; Fabian T. Thome; Marcel Hecker; Martijn Kemerink; Toni Seiler

REVIEW 3 major objections 5 minor 43 references

Barkhausen noise in the columnar hexagonal organic ferroelectric BTA

T0 review · 3 major / 5 minor · reviewed 2026-08-11 · deepseek-v4-flash

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Pith's one-line read The paper claims that BTA polarization reversal is a critical avalanche process below about 175 K, with power-law distributed switching events too small to be seen as Barkhausen noise.

desk verdict First BTA Barkhausen kMC study with an honest experimental null result, but the claimed mean-field SOC exponents are compared against a benchmark the paper's own introduction contradicts. read the letter →

arxiv 2412.12666 v2 pith:DX5QONYJ submitted 2024-12-17 cond-mat.mtrl-sci cond-mat.other

Andrey Alekseevich Butkevich , Fabian T. Thome , Toni Seiler , Marcel Hecker , Martijn Kemerink This is my paper · ORCID

classification cond-mat.mtrl-scicond-mat.other PACS 77.80.-e77.80.Fm05.65.+b

keywords Barkhausennoisecracklingself-organizedcriticalityorganicferroelectricBTAkineticMonteCarlopower-lawexponentsswitching

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 claims that polarization reversal in the columnar organic ferroelectric BTA proceeds through dipole avalanches whose sizes and energies are power-law distributed, matching mean-field predictions of self-organized criticality below about 175 K. Above that temperature the extracted exponents grow, which the authors interpret as a thermal creep regime in which many small thermally triggered events replace field-driven cascades. The same kinetic Monte Carlo simulations produce only tiny events, several orders of magnitude below the current noise floor of a sensitive experimental setup, which the authors offer as the reason no Barkhausen noise is seen in real BTA samples. If correct, this identifies the microscopic switching unit of BTA as a subcolumn within a single supramolecular column and explains the silence of the material in Barkhausen-noise measurements.

What carries the argument

The load-bearing object is a kinetic Monte Carlo model of BTA in which each amide group is a flipable dipole on a hexagonal columnar lattice, with electrostatic dipole-dipole interactions computed inside a cutoff sphere and a reaction-field approximation for longer-range contributions. Structural disorder enters as subcolumns of randomly drawn lengths, positional shifts, rotations, and occasional chirality changes between subcolumns; a dipole flips with rate $\nu_0\exp(-\Delta U/k_BT)$ when flipping is uphill and $\nu_0$ otherwise, which lets cascades of flips become avalanches. The argument is carried by comparing the fitted exponents of the event-size and event-energy distributions against the mean-field plasticity predictions, and by the observation that increasing column height, but not lateral box width, enlarges the largest events. The machinery produces the claimed temperature threshold near 175 K, the disorder dependence analogous to a random-field Ising model, and the tiny event sizes that explain the null experimental result.

What would settle it

Run the same simulated event lists through an automated maximum-likelihood power-law fit with threshold as a free parameter: if the fitted exponents drift with threshold or depart from $\tau\approx1.5$ and $\epsilon\approx1.33$ across the 100–175 K range, the self-organized criticality claim is not supported. Experimentally, a device with a much smaller electrode area that reduces the required simultaneous-switch count to a few hundred dipoles should resolve individual BTA avalanches if they exist.

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Extended reading notes

Core claim

The authors report that field-driven polarization reversal in the supramolecular ferroelectric BTA is a critical crackling process at low temperature: dipole flips organize into avalanches whose size and energy distributions follow power laws with exponents close to the mean-field plasticity values (about 1.5 for sizes and about 1.33 for energies), and these exponents are stable against disorder strength and modest parameter changes below roughly 175 K. The avalanches propagate essentially one-dimensionally along the supramolecular columns, so lateral coupling between columns is weak. At higher temperatures the power-law exponents increase, indicating creep, and the simulated events are so small that a purpose-built high-sensitivity electrical setup should not detect them; no Barkhausen noise was observed, which the paper takes as consistency with the model rather than as evidence against switching avalanches.

Load-bearing premise

The claim of self-organized criticality rests on the assumption that the fitted power-law exponents reflect the simulated switching physics rather than the manual choices of event threshold and fit range.

Editorial extensions

If this is right

Below about 175 K, polarization switching in BTA should be scale-invariant: the same avalanche statistics hold across decades of event size, up to the system-size cutoff.
Raising temperature or lowering sweep frequency should move the system from critical avalanches into creep, visible as larger fitted power-law exponents under the same analysis.
Barkhausen noise in BTA should be undetectable in conventional and even moderately optimized setups, because single-column avalanches involve hundreds of dipoles rather than the roughly 600,000 simultaneously switching regions needed for a measurable current.
Switching in the hexagonal columnar phase is quasi-one-dimensional: lateral column coupling is weak, so increasing the lateral box size should not change avalanche sizes, while column height sets the upper cutoff below roughly 300 molecules.

Reading between the lines

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

If the low-temperature exponents are truly disorder-independent, one testable extension is to seek the same critical exponents in other columnar supramolecular ferroelectrics with similar hydrogen-bonded stacks, since the mechanism would be morphological rather than chemical.
The null experimental result could be turned positive using nanoscale electrodes or single-column devices, where the number of switchable dipoles is small enough that individual avalanches would exceed the measurement noise; a power-law distribution of switching currents there would confirm self-organized criticality in real BTA.
The paper's logic implies that the absence of Barkhausen noise in a ferroelectric is not evidence against jerky switching; it can simply mean the switching entities are too small, so interpreting null results requires a model of event sizes such as the one provided here.
The claimed temperature crossover near 175 K and its frequency dependence could be probed by measuring coercive-field statistics across the hysteresis loop at different temperatures, since the paper argues the exponents are anti-correlated with coercivity.

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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

First thing: this is a genuine first — a kMC study of Barkhausen noise in BTA, with a new experimental null result reported honestly. The SOC claim in the abstract should not be taken at face value. The reader's stress-test note is right about the benchmark: the paper's own introduction gives tau=2 and epsilon=5/3 for whole-loop integrated mean-field events, but Figure 6 and S5.3 compare to 1.5 and 1.33. If the data are full-loop, that's the wrong reference. The only escape would be if all events used in the fits are effectively confined to a narrow field window around the coercive field, so the constant-stress limit applies. The authors mention such a filtering option in SI S2 but don't clearly say that's what the temperature sweep uses. They need to fix that.

What's good: the model is described in enough detail to reproduce; there are finite-size checks showing avalanche size saturates with column length and depends weakly on lateral width, which supports quasi-1D propagation; the disorder sweep maps out a regime where exponents are stable, with behaviour reminiscent of RFIM. The experimental null result is handled well: noise floor characterized, filament artifacts identified, and an order-of-magnitude estimate shows the expected currents sit orders below sensitivity. That part is solid and citable on its own. The circularity concern in the reader notes doesn't land: the model parameters are from earlier work, and the exponents are fitted, not imposed.

Soft spots beyond the benchmark: event threshold is set by hand just above thermal noise, fit range by eye, and the merging of runs uses a 'weight-event' correction that duplicates low-end events. There are no error bars or alternative fit tests, and no code or raw event data released. For a power-law claim, those choices are material. They might move the fitted tau by a few tenths, which is exactly the difference between the quoted values and either benchmark. I don't think it's fatal — the distributions do look power-law-like over a decade — but the central claim is more fragile than the writing suggests.

Who this is for: people working on organic ferroelectrics or crackling noise will want to read it, especially for the null result. A competent referee can fix the benchmark and ask for robustness checks; the paper deserves that step. I'd send it to review, with the request that the authors clarify the benchmark, add uncertainty estimates and alternative fits, and publish event-level data.

Referee Report

3 major / 5 minor

Summary. The paper reports kinetic Monte Carlo simulations of polarization reversal in the columnar organic ferroelectric BTA, from which avalanche size and energy distributions are extracted and fitted to power laws. The central claim is that for temperatures below 175 K and sufficiently strong structural disorder the system exhibits self-organized criticality, with exponents matching mean-field plasticity values, while at higher temperatures a creep regime is entered. The authors also report an experimental search for Barkhausen noise in BTA that found none, consistent with their simulated event sizes being well below the measurement noise floor.

Significance. If the self-organized criticality claim were supportable, it would be an interesting advance for organic ferroelectrics, where crackling noise has rarely been studied, and the combination of a detailed kMC model with a null experimental result is a useful attempt at quantitative consistency. The manuscript is careful in describing the simulation protocol and the experimental setup, and it makes explicit, falsifiable statements about the temperature and disorder dependence of the exponents. However, the central claim is currently undermined by an inconsistency between the mean-field benchmark used for comparison and the field-integrated nature of the simulated events, as well as by the lack of robustness checks for the analysis choices that determine the fitted exponents.

major comments (3)

[Introduction and Figure 6 / SI S5.3] The mean-field benchmark used for the horizontal lines in Fig. 6 and for the values quoted in SI S5.3 is the constant-stress set (τ=1.5, ε=4/3), but the events are collected over a full hysteresis loop (Section 3, Fig. 2). In the Introduction the authors explicitly state that for events measured over a whole (stress-integrated) loop the mean-field values are τ=2 and ε=5/3, citing Ref. [16]. Since the simulated events come from complete field ramps, the correct benchmark under the paper's own framework is the loop-integrated set. The reported agreement with τ≈1.5 and ε≈1.33 therefore does not support the claim of self-organized criticality; it actually indicates a disagreement with the loop-integrated prediction. Please redo the comparison either against τ=2, ε=5/3, or by restricting the event analysis to the coercive-field region and stating clearly which benchmark is used.
[SI S2 and Section 3 (threshold and fitting procedure)] The extracted exponents, which form the basis of the SOC claim, depend on several manual analysis choices that are not accompanied by robustness checks. The event threshold is set 'just right of the thermal noise peak' (SI S2), the power-law fit range is determined 'by visualizing the event data' (SI S2), and data sets with different thresholds are merged by creating 'weight events' (Section 3). No error bars, bootstrap estimates, or sensitivity analyses are reported for the fitted exponents. It is therefore unclear whether the apparent low-temperature plateau in Fig. 6a is a genuine physical feature or an artifact of these choices. Please provide a systematic variation of the threshold level, the fit range, and the merging procedure, and report the resulting spread in the exponents.
[SI S5 (disorder dependence)] The claim that the exponents are invariant to disorder is not fully supported by the presented data. Table S5.1 shows that the size exponent τ varies from 1.30 to 1.71 across chirality settings, and Fig. S5.2b shows a clear increase of the exponents for small subcolumn lengths (N ≤ 5) and a breakdown of the power-law form for N = 100. These variations are acknowledged qualitatively, but they are not quantified against the proposed universal regime. If the SOC regime is defined only for an intermediate range of disorder, the boundaries of that range should be stated and the universality claim restricted accordingly.

minor comments (5)

[Section 4 and Figure 6b] The temperature unit is inconsistent: Fig. 6b and the surrounding text use '160 °C' for the sweeping-frequency study, whereas the text elsewhere uses kelvin (e.g., 'below 175 K' and 'T = 160 K' in SI S4). Please correct the unit throughout.
[SI S2] The text refers to 'Figure 1d' when describing the merging of data sets; the corresponding figure in the main text is Figure 2d. Please correct the reference.
[Section 4] There is a typo: 'the size S is defined as he highest number of flipped dipoles per time step' should read 'the highest number'. Please also clarify once whether S is the maximum instantaneous flip rate or the total number of flips, since the summed size SΣ is later defined separately.
[SI S5.3 caption] The caption says 'the extracted power-law exponents stay at the mean field predictions of τ = 1.5 and ε = 1.33'; the value 1.33 is the decimal approximation of 4/3, but the text elsewhere uses the fraction. Please use one consistent representation.
[Section 5] The estimate in SI S7 rests on the assumption that the experimental sample can be decomposed into independent ~700-molecule columns and that an event size of 200 dipoles is representative. It would be helpful to state explicitly that this is an order-of-magnitude estimate and to discuss how the conclusion would change if larger lateral avalanches (e.g., spanning several columns) were possible.

Circularity Check

0 steps flagged · score 0.0 of 10

No significant circularity: the SOC exponents are emergent outputs of the kMC model and are tested against external mean-field benchmarks, not fitted inputs.

full rationale

The central claim (self-organized criticality below ~175 K) is an emergent result of the kinetic Monte Carlo simulations. The power-law exponents are extracted from simulated avalanche-size and energy distributions and compared with externally published mean-field plasticity values (refs 12-16), not with any quantity the model was tuned to reproduce. The model parameters are inherited from prior work by the same group (refs 25-27), but those self-citations determine the Hamiltonian and switching rates, not the exponents; the simulations are not fitted to tau=1.5 or epsilon=4/3. The disorder-invariance tests in SI S5 (e.g., Fig. S5.3 and S5.4) explicitly show that the exponents remain near the mean-field values while the subcolumn-length variance is varied, which is the opposite of fitting the claim. The experimental null result is used only as a consistency check (SI S7), where simulated event sizes are compared with the setup noise floor; the absence of Barkhausen noise is not used to define or fit the exponents. The manual threshold and visually chosen fit range described in SI S2 are analysis choices that affect robustness, but they do not make the extracted exponents equal to the inputs by construction. One non-circular concern worth noting: the paper compares full-loop avalanche exponents to the constant-stress mean-field values (tau=1.5, epsilon=4/3) even though its own introduction states that the stress-integrated loop values are tau=2 and epsilon=5/3; this is a benchmark-consistency issue that should be addressed, but it is not a circular reduction of the derivation to its inputs.

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

The central simulation uses a kMC model with parameters drawn from prior work, plus analysis choices (threshold, fit range, merging) that affect the fitted exponents. No new physical entities are introduced. The key assumptions are that the reduced electrostatic model and disorder parametrization represent real BTA films, and that mean-field universality applies.

free parameters (4)

Event threshold level = ~15 dipoles per time step
Set manually 'just right of the thermal noise peak' (SI S2) to separate thermal fluctuations from avalanches; directly determines which events are counted and hence the fitted exponents.
Power-law fit range = e.g., S = 40 to 250 (Figure S5.3)
Chosen by visualizing the event data (SI S2); the fitted exponents depend on this range.
Weight-event correction for merged thresholds = Not specified
Events below the highest threshold are duplicated to compensate for merging data sets with different thresholds (SI S2); this alters the small-event end of the distribution and can bias the power-law fit.
Subcolumn length N and variance sigma_N = N=10, sigma_N=1 (typical)
Characterize structural disorder in the kMC model; the paper shows the exponents are invariant over a range but the typical values are chosen as experimentally realistic (Table S1.1) from prior work rather than derived.

assumptions (4)

domain assumption The kMC model with fixed dipole positions and only electrostatic interactions (permanent and induced dipoles, reaction field, cutoff r_c=30) captures the essential switching dynamics of BTA.
Section 2, Model; the authors state steric interactions are accounted for by prescribed morphology and rotation rates. If this reduction misses important physics, the simulated avalanche statistics may not transfer to real BTA.
domain assumption The disorder in real BTA films is represented by subcolumns with Gaussian length distribution (mean N, variance sigma_N), positional shifts, random rotations, and helicity changes.
Section 2 and SI S1; the conclusions about SOC and 1D avalanches depend on this disorder model being representative. The paper offers no direct experimental measurement of the disorder distribution.
domain assumption The mean-field plasticity / random-field Ising universality class applies to field-driven switching in BTA, so comparison of exponents to mean-field predictions is a valid test of SOC.
Section 1 and Section 4; if BTA switching is not in this universality class, the numerical agreement of exponents is not evidence for SOC.
domain assumption The reaction-field cutoff at r_c=30 and the precomputed nearest-neighbor flipping-energy differences remain accurate throughout an avalanche.
Section 2, Equations 4 to 6; long-range interactions are approximated, and the approximation is not separately validated for avalanche statistics.

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Cite this review

Pith. "Pith review of Barkhausen noise in the columnar hexagonal organic ferroelectric BTA." pith.science (2026). https://pith.science/paper/DX5QONYJ

@misc{pith2026241212666,
  author       = {Pith},
  title        = {Pith review of: Barkhausen noise in the columnar hexagonal organic ferroelectric BTA},
  year         = {2026},
  howpublished = {\url{https://pith.science/paper/DX5QONYJ}},
  note         = {Machine review of arXiv:2412.12666}
}

read the original abstract

Upon a polarization reversal within a ferroelectric material, one stable state changes into another which is typically described by a progression of switching events of smaller fractions of the material. These events give rise to crackling or Barkhausen noise and follow a characteristic distribution in their sizes. Barkhausen noise has been studied to better understand the switching processes of ferroelectrics and has been applied for inorganic ferroelectric materials and perovskites. In this work, we present results from kinetic Monte Carlo simulations investigating the switching process of the small organic molecular ferroelectric benzene-1,3,5-tricarboxamides (BTAs). For temperatures below 175 K and sufficiently strong structural disorder, the system exhibits self-organized critical behavior; for higher temperatures, a creep regime is entered. Our extracted power-law exponents are smaller than those typically measured in inorganic crystals and ceramics which indicates that in the more disordered material BTA larger spanning avalanches are possible. The system was experimentally investigated with a high-sensitivity setup. No Barkhausen noise was observed which is consistent with the simulated event sizes, lying several orders beneath the noise threshold of the experimental setup. This finding corroborates the notion that switching in BTA progresses along the 1D columns in the hexagonal liquid crystal lattice, with little coupling between the columns that could give rise to larger lateral avalanches.

Discussion (0). Continue with ORCID to comment.

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Pith tools

Reviewed August 11, 2026 · model on record in the stance chip above.

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