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arxiv: 2606.24657 · v1 · pith:M5VNMRE6new · submitted 2026-06-23 · ❄️ cond-mat.soft · cond-mat.mtrl-sci

Limited surface mobility inhibits stable glass formation for 2-ethyl-1-hexanol

M. Tylinski , M. S. Beasley , Y. Z. Chua , C. Schick , M. D. Ediger This is my paper

Pith reviewed 2026-06-25 21:50 UTC · model grok-4.3

classification ❄️ cond-mat.soft cond-mat.mtrl-sci
keywords vapor depositionstable glassessurface mobilitykinetic stability2-ethyl-1-hexanolorganic glassesglass transition
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The pith

Limited surface mobility prevents 2-ethyl-1-hexanol from forming highly stable vapor-deposited glasses.

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

The paper examines why 2-ethyl-1-hexanol fails to produce highly stable glasses under standard vapor deposition conditions that work for many other organic molecules. Experiments show that lowering the deposition rate from 0.2 nm/s to 0.005 nm/s at a substrate temperature of 0.90 Tg raises the kinetic stability, measured by isothermal transformation times, by three orders of magnitude. Vapor-deposited samples also reach much higher stability than liquid-cooled glasses aged for the same total time. Comparison to ethylcyclohexane, which forms stable glasses readily, leads to the estimate that 2-ethyl-1-hexanol surface mobility is more than four orders of magnitude lower at 0.85 Tg. These findings support the claim that limited surface mobility is what blocks stable glass formation for this molecule.

Core claim

The kinetic stability of 2-ethyl-1-hexanol glasses increases by three orders of magnitude when the deposition rate is lowered at 0.90 Tg, and a vapor-deposited glass is far more stable than an aged liquid-cooled glass prepared in the same time; direct comparison shows the surface mobility of 2-ethyl-1-hexanol is more than four orders of magnitude lower than that of ethylcyclohexane at 0.85 Tg, supporting the hypothesis that limited surface mobility inhibits formation of highly stable glasses.

What carries the argument

Deposition-rate dependence of isothermal transformation times, used to quantify and compare surface mobility against ethylcyclohexane.

Load-bearing premise

That differences in stable glass formation between 2-ethyl-1-hexanol and ethylcyclohexane arise solely from their difference in surface mobility rather than from other molecular-structure or bulk-property distinctions.

What would settle it

A direct measurement of surface diffusion coefficients for both molecules at 0.85 Tg that finds the mobility ratio is not larger than four orders of magnitude.

Figures

Figures reproduced from arXiv: 2606.24657 by C. Schick, M. D. Ediger, M. S. Beasley, M. Tylinski, Y. Z. Chua.

Figure 1
Figure 1. Figure 1: Reversing heat capacity data from 20 Hz AC nanocalorimetry experiments on 2-ethyl-1-hexanol glasses, obtained during heating at 5 K/min. Panel a: Glasses deposited at Tsubstrate = 0.95 Tg. Panel b: Glasses deposited at Tsubstrate = 0.90 Tg. Panel c: Glasses deposited at Tsubstrate = 0.85 Tg. The black dashed lines in panel c demonstrate how the onset temperature (Tonset) for the transformation of the as￾de… view at source ↗
Figure 2
Figure 2. Figure 2: Characteristics of vapor-deposited glasses of 2-ethyl-1-hexanol, as a function of deposition rate, from the temperature ramping experiments shown in [PITH_FULL_IMAGE:figures/full_fig_p008_2.png] view at source ↗
Figure 5
Figure 5. Figure 5: Aging experiments on a liquid-cooled glass of 2-ethyl-1-hexanol. Panel a: Heat capacity decrease during aging at 0.95 Tg. The total aging time is equal to the time required for the longest deposition utilized to prepare the samples in [PITH_FULL_IMAGE:figures/full_fig_p013_5.png] view at source ↗
Figure 7
Figure 7. Figure 7: Relaxation times  and surface for 2-ethyl-1-hexanol and ethylcyclohexane. The surface values are obtained by fitting the data shown in [PITH_FULL_IMAGE:figures/full_fig_p020_7.png] view at source ↗
read the original abstract

Previous work has shown that vapor-deposition can prepare organic glasses with extremely high kinetic stabilities and other properties that would be expected from liquid-cooled glasses only after aging for thousands of years or more. However, recent reports have shown that some molecules form vapor-deposited glasses with only limited kinetic stability when prepared using conditions expected to yield a stable glass. In this work, we vapor deposit glasses of 2-ethyl-1-hexanol over a wide range of deposition rates and test several hypotheses for why this molecule does not form highly stable glasses under normal deposition conditions. The kinetic stability of 2-ethyl-1-hexanol glasses is found to be highly dependent on the deposition rate. For deposition at Tsubstrate = 0.90 Tg, the kinetic stability increases by 3 orders of magnitude (as measured by isothermal transformation times) when the deposition rate is decreased from 0.2 nm/s to 0.005 nm/s. We also find that, for the same preparation time, a vapor-deposited glass has much more kinetic stability than an aged liquid-cooled glass. Our results support the hypothesis that the formation of highly stable 2-ethyl-1-hexanol glasses is inhibited by limited surface mobility. We compare our deposition rate experiments to similar ones performed with ethylcyclohexane (which readily forms glasses of high kinetic stability); we estimate that the surface mobility of 2-ethyl-1-hexanol is more than 4 orders of magnitude less than that of ethylcyclohexane at 0.85 Tg.

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

1 major / 2 minor

Summary. The manuscript reports vapor-deposition experiments on 2-ethyl-1-hexanol, demonstrating that the kinetic stability of the resulting glasses (quantified via isothermal transformation times) increases by three orders of magnitude when the deposition rate is lowered from 0.2 nm/s to 0.005 nm/s at T_substrate = 0.90 T_g. The authors test multiple hypotheses for the limited stability observed under standard conditions and conclude that limited surface mobility is the inhibiting factor. This conclusion rests on a direct comparison to ethylcyclohexane (which forms highly stable glasses), from which they estimate that the surface mobility of 2-ethyl-1-hexanol is more than four orders of magnitude lower at 0.85 T_g. They additionally show that, for equivalent preparation times, vapor-deposited glasses exhibit greater kinetic stability than aged liquid-cooled glasses.

Significance. If the central claim holds, the work identifies surface mobility as a key constraint on stable glass formation for hydrogen-bonding molecules and provides a concrete experimental example where rate-dependent deposition fails to produce high-stability glasses. The clear demonstration of strong rate dependence and the explicit comparison to a contrasting molecule constitute strengths; the manuscript also supplies falsifiable predictions about mobility differences that can be tested with independent diffusion measurements.

major comments (1)
  1. [abstract, final paragraph] Abstract, final paragraph: the claim that surface mobility of 2-ethyl-1-hexanol is >4 orders of magnitude lower than that of ethylcyclohexane at 0.85 T_g is load-bearing for the central hypothesis, yet the comparison does not demonstrate that bulk properties (fragility index, self-diffusion coefficients, or relaxation mechanisms) have been matched or corrected between the hydrogen-bonding alcohol and the non-polar hydrocarbon. Without such controls, differences in the mapping from deposition rate to stability cannot be attributed solely to surface mobility.
minor comments (2)
  1. The abstract states that several hypotheses were tested but does not enumerate them or report the outcome for each; a brief summary in the abstract or a dedicated section would improve clarity.
  2. Error analysis, uncertainties on transformation times, and full data tables for the rate series are not referenced; inclusion of these would strengthen the reported three-order-of-magnitude effect.

Simulated Author's Rebuttal

1 responses · 0 unresolved

We thank the referee for their careful review and for raising this important point about our comparison between 2-ethyl-1-hexanol and ethylcyclohexane. We address the comment below and have revised the manuscript to qualify the surface-mobility estimate and to discuss potential confounding bulk-property differences.

read point-by-point responses

  1. Referee: [abstract, final paragraph] Abstract, final paragraph: the claim that surface mobility of 2-ethyl-1-hexanol is >4 orders of magnitude lower than that of ethylcyclohexane at 0.85 T_g is load-bearing for the central hypothesis, yet the comparison does not demonstrate that bulk properties (fragility index, self-diffusion coefficients, or relaxation mechanisms) have been matched or corrected between the hydrogen-bonding alcohol and the non-polar hydrocarbon. Without such controls, differences in the mapping from deposition rate to stability cannot be attributed solely to surface mobility.

    Authors: We agree that the original manuscript does not demonstrate explicit matching or correction for bulk properties such as fragility index, self-diffusion coefficients, or relaxation mechanisms between the two molecules. The >4-order-of-magnitude estimate is an inference based on the deposition rates needed to reach comparable kinetic stabilities at the same reduced temperature (0.85 Tg). We have revised the abstract and added a dedicated paragraph in the discussion to state this limitation explicitly, to note the known differences in bulk dynamics between hydrogen-bonding and non-polar glass-formers, and to emphasize that independent surface-diffusion measurements would be required for a definitive separation of surface versus bulk contributions. The strong rate dependence observed for 2-ethyl-1-hexanol nevertheless remains the primary experimental evidence supporting limited surface mobility as the inhibiting factor. revision: yes

Circularity Check

0 steps flagged

No circularity; experimental comparison stands on independent measurements

full rationale

The paper reports direct measurements of isothermal transformation times versus deposition rate for 2-ethyl-1-hexanol, then compares those rates to published ethylcyclohexane data to infer a surface-mobility difference. No equation defines surface mobility from the stability result and then re-uses that definition as a prediction; the central claim is an inference from two independent data sets rather than a self-referential fit or self-citation chain. The derivation chain therefore remains self-contained against external benchmarks.

Axiom & Free-Parameter Ledger

0 free parameters · 0 axioms · 0 invented entities

Experimental study with no mathematical derivations; no free parameters, axioms, or invented entities are introduced.

pith-pipeline@v0.9.1-grok · 5831 in / 1144 out tokens · 30957 ms · 2026-06-25T21:50:32.381990+00:00 · methodology

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    The third hypothesis, that stable glass formation in 2-ethyl-1-hexanol is inhibited by limited surface mobility, is consistent with our experimental results as we discuss below

    These observations in combination with the reasonably high kinetic stability achieved at the lowest deposition rates allow us to reject the second hypothesis. The third hypothesis, that stable glass formation in 2-ethyl-1-hexanol is inhibited by limited surface mobility, is consistent with our experimental results as we discuss below. For the rest of the ...

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