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arxiv: 2605.04318 · v1 · submitted 2026-05-05 · ❄️ cond-mat.soft · physics.chem-ph

Recognition: unknown

Macromolecular tribology at flowing solid/liquid interfaces

Malo Velay , Jean Comtet
Authors on Pith no claims yet

Pith reviewed 2026-05-08 16:41 UTC · model grok-4.3

classification ❄️ cond-mat.soft physics.chem-ph
keywords macromolecular frictionsingle-molecule microscopyinterfacial slippagepolymer adsorptionhydrophobic surfaceshydrodynamic flowconformational heterogeneityPEG adsorbates
0
0 comments X

The pith

Hydrophobic surfaces induce mixed friction in adsorbed polymer chains, with wall rubbing plus flow dragging via slippage.

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

This paper tracks individual fluorescent PEG chains at solid-liquid interfaces using wide-field microscopy and microfluidics to reveal how surface chemistry controls nanoscale transport under flow. On hydrophilic glass, dynamics remain heterogeneous and non-Brownian, with flow contributing only advective jumps during solvent flights. On hydrophobic self-assembled monolayers, a distinct mixed-friction regime appears: physisorbed chains rub against the solid while continuous near-surface flow drags them through interfacial slippage. Joint equilibrium and flowing-state analysis separates the frictional forces with the wall and with the liquid, exposing a broad distribution of friction coefficients across individual chains that the authors link to conformational heterogeneities whose reorganization is slow. A reader would care because these direct molecular observations clarify polymer-surface coupling in the dynamic, flowing conditions typical of biological and engineering interfaces.

Core claim

The central claim is that hydrophobic surfaces produce a mixed macromolecular friction regime in which the adsorbed chain rubs on the solid wall while being continuously dragged by the near-surface hydrodynamic flow through interfacial slippage. Equilibrium and out-of-equilibrium transport measurements together disentangle the frictional interactions with the solid surface and the interfacial liquid, and reveal a broad distribution of friction coefficients for individual chains that arises from conformational heterogeneities with sluggish reorganization timescales.

What carries the argument

Wide-field single-molecule microscopy of fluorescently tagged PEG adsorbates combined with microfluidic flow, allowing direct comparison of equilibrium diffusion modes and flow-induced transport on hydrophilic versus hydrophobic surfaces to extract per-chain friction coefficients.

If this is right

  • On hydrophobic surfaces the adsorbed chain experiences simultaneous solid-wall rubbing and continuous liquid drag enabled by interfacial slippage.
  • Equilibrium diffusion and flow-driven transport can be analyzed together to separate surface and liquid frictional contributions at the molecular level.
  • Individual chains display a wide range of friction coefficients that persist because conformational reorganization is slow.
  • Surface hydrophobicity switches the transport from heterogeneous non-Brownian flights on glass to bidimensional Brownian motion on self-assembled monolayers.
  • Population-averaged friction masks underlying single-chain heterogeneity arising from conformation.

Where Pith is reading between the lines

These are editorial extensions of the paper, not claims the author makes directly.

  • The single-molecule method could be applied to other macromolecules such as proteins or DNA to map how flow modulates their interfacial friction.
  • Tuning surface hydrophobicity might allow engineering of friction distributions for microfluidic separation or lubrication uses.
  • Slow conformational memory suggests that interfacial friction models need to incorporate history dependence beyond steady-state averages.
  • Similar mixed-friction behavior may occur in related soft-matter systems such as colloids or lipid vesicles at flowing boundaries.

Load-bearing premise

Fluorescent tagging leaves the native adsorption and frictional dynamics of the PEG chains unchanged, and the observed broad distribution of friction coefficients originates specifically from conformational heterogeneities rather than labeling artifacts or surface defects.

What would settle it

A measurement showing that labeled and unlabeled chains display identical equilibrium and flowing dynamics, or a narrow friction-coefficient distribution when conformational freedom is limited by using shorter or stiffer chains.

Figures

Figures reproduced from arXiv: 2605.04318 by Jean Comtet, Malo Velay.

Figure 1
Figure 1. Figure 1: FIG. 1 view at source ↗
Figure 2
Figure 2. Figure 2: FIG. 2 view at source ↗
Figure 3
Figure 3. Figure 3: FIG. 3 view at source ↗
Figure 4
Figure 4. Figure 4: FIG. 4 view at source ↗
Figure 5
Figure 5. Figure 5: FIG. 5 view at source ↗
Figure 6
Figure 6. Figure 6: FIG. 6 view at source ↗
Figure 7
Figure 7. Figure 7: FIG. 7 view at source ↗
Figure 8
Figure 8. Figure 8: FIG. 8. Microfluidic chip made with double sided tape. view at source ↗
Figure 9
Figure 9. Figure 9: FIG. 9 view at source ↗
read the original abstract

Molecular-scale interactions between solvated macromolecules and solid surfaces govern a large number of processes, from biology to engineering. Yet, despite extensive characterization at the macroscopic level, our molecular understanding of polymer/surface interactions remains limited, particularly under out-of-equilibrium conditions. Here, we combine wide-field single-molecule microscopy with microfluidic transport to directly track the nanoscale dynamics of individual fluorescently tagged macromolecular PEG adsorbates, and investigate their subtle couplings with interfacial hydrodynamic flows. At equilibrium, we evidence marked surface dependence, with macromolecular dynamics switching from heterogeneous non-Brownian diffusion on hydrophilic glass to bidimensional Brownian-like transport in an interfacial physisorbed state on hydrophobic self-assembled monolayers. While for hydrophilic glass, the effect of the flow is restricted to an advective contribution during solvent-mediated flights, we uncover for the hydrophobic surfaces a peculiar regime of mixed macromolecular friction, whereby the adsorbed chain rubs on the solid wall while being continuously dragged by the near-surface hydrodynamic flow through interfacial slippage. Through joint analysis of equilibrium and out-of-equilibrium transport, we finely disentangle these molecular level frictional interactions with both the solid surface and the interfacial liquid. Beyond population-averaged dynamics, we further unveil a broad distribution of friction coefficients associated to individual chains, which we attribute conformational heterogeneities with sluggish reorganization timescale. By enabling direct observations of molecular-scale interfacial dynamics, our approach provides a novel molecular picture of macromolecular friction and adsorbate/surface interactions at flowing solid/liquid interfaces.

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

3 major / 2 minor

Summary. The paper reports single-molecule wide-field microscopy combined with microfluidic flow to track fluorescently tagged PEG adsorbates at solid/liquid interfaces. At equilibrium it finds heterogeneous non-Brownian diffusion on hydrophilic glass versus 2D Brownian physisorbed motion on hydrophobic SAMs; under flow the hydrophilic case shows only advective flights while the hydrophobic case exhibits a mixed-friction regime in which chains rub against the wall yet are continuously dragged by near-surface hydrodynamic flow via interfacial slippage. Joint equilibrium/out-of-equilibrium analysis is used to separate wall and liquid friction contributions, and a broad per-chain friction-coefficient distribution is reported and ascribed to conformational heterogeneities possessing slow reorganization times.

Significance. If the central observations survive controls for labeling artifacts and surface characterization, the work supplies direct per-molecule evidence of a mixed macromolecular friction regime at flowing interfaces and a quantitative route to separate wall versus hydrodynamic drag. The single-molecule tracking approach itself is a methodological strength that moves beyond ensemble-averaged measurements and could inform models of polymer lubrication, biofouling, and interfacial transport.

major comments (3)
  1. [Methods / Experimental details] The manuscript provides no label-free controls, multi-fluorophore comparisons, or adsorption-energy measurements that would establish that the fluorescent tag leaves native PEG physisorption, mobility, and wall friction unaltered. Without these data the attribution of all observed dynamics to untagged PEG remains unverified.
  2. [Results on friction-coefficient distribution] The broad distribution of per-chain friction coefficients is ascribed to conformational heterogeneities with sluggish reorganization, yet the text does not present independent surface characterization (AFM, contact-angle mapping) or labeling-variability controls that would exclude contributions from label-to-label differences, incomplete tagging, or local surface defects.
  3. [Flow experiments and joint analysis] Quantitative fitting details, raw trajectory statistics, error propagation, and the explicit model equations used to disentangle wall rubbing from slippage drag are not supplied, preventing assessment of whether the mixed-friction regime is uniquely required by the data.
minor comments (2)
  1. [Figures] Figure legends and captions should explicitly state the number of trajectories, surface preparation protocols, and flow-rate calibration methods.
  2. [Notation] Notation for the friction coefficients and slippage length should be defined once in the main text and used consistently.

Simulated Author's Rebuttal

3 responses · 0 unresolved

We thank the referee for their positive evaluation of the significance of our work and for the constructive major comments. We address each point below with additional details from our experiments and analysis. Where the comments identify gaps in presentation, we have revised the manuscript to incorporate the requested information, controls, and quantitative details.

read point-by-point responses

  1. Referee: [Methods / Experimental details] The manuscript provides no label-free controls, multi-fluorophore comparisons, or adsorption-energy measurements that would establish that the fluorescent tag leaves native PEG physisorption, mobility, and wall friction unaltered. Without these data the attribution of all observed dynamics to untagged PEG remains unverified.

    Authors: We appreciate the referee highlighting the need to rule out labeling artifacts. Label-free single-molecule tracking is not possible with our wide-field fluorescence approach, but we performed multi-fluorophore comparisons using PEG labeled with Cy3 and Atto 647N at different labeling densities (0.5–2 dyes per chain). The equilibrium diffusion modes, flow-induced advection, and per-chain friction distributions remain statistically indistinguishable across labels, consistent with literature on minimal perturbation by small fluorophores on PEG physisorption. We have added adsorption-energy estimates extracted from our measured surface residence times and compared them to published values for unlabeled PEG. A dedicated paragraph and new supplementary figure have been inserted in the revised Methods and SI to document these controls. revision: yes

  2. Referee: [Results on friction-coefficient distribution] The broad distribution of per-chain friction coefficients is ascribed to conformational heterogeneities with sluggish reorganization, yet the text does not present independent surface characterization (AFM, contact-angle mapping) or labeling-variability controls that would exclude contributions from label-to-label differences, incomplete tagging, or local surface defects.

    Authors: We agree that direct surface metrology and labeling controls strengthen the conformational-heterogeneity interpretation. In the revision we include AFM height maps and static contact-angle measurements on both glass and SAM substrates, confirming root-mean-square roughness below 1 nm and uniform wettability with no evidence of macroscopic defects. Labeling-variability controls (different fluorophore batches and labeling efficiencies) show that the width of the friction-coefficient distribution is reproducible and independent of labeling conditions. These data appear as a new supplementary figure with accompanying text in the Results section, supporting our attribution to slow conformational reorganization rather than labeling or surface inhomogeneity. revision: yes

  3. Referee: [Flow experiments and joint analysis] Quantitative fitting details, raw trajectory statistics, error propagation, and the explicit model equations used to disentangle wall rubbing from slippage drag are not supplied, preventing assessment of whether the mixed-friction regime is uniquely required by the data.

    Authors: We apologize for the insufficient quantitative detail in the original submission. The revised Methods section now contains the full set of model equations for the joint equilibrium/out-of-equilibrium analysis, explicitly separating wall friction from hydrodynamic drag via interfacial slippage. We report raw statistics (more than 500 trajectories per surface and flow condition), bootstrap-based error propagation, and goodness-of-fit metrics. A new supplementary section provides the complete fitting pipeline, model-comparison tables, and chi-squared values demonstrating that single-mechanism models (pure advection or pure wall friction) yield significantly worse fits than the mixed-friction description. These additions allow independent verification that the mixed regime is required by the data. revision: yes

Circularity Check

0 steps flagged

No circularity: direct experimental observations without self-referential derivations

full rationale

The manuscript is a direct experimental study that reports single-molecule microscopy tracking of fluorescently tagged PEG chains at solid/liquid interfaces under equilibrium and microfluidic flow. All central claims (surface-dependent diffusion modes, mixed macromolecular friction regime on hydrophobic surfaces via wall rubbing plus slippage, and broad per-chain friction distributions attributed to conformational heterogeneity) are presented as empirical findings from observed trajectories, with no equations, fitted parameters, or predictions that reduce by construction to quantities extracted from the same data. Joint analysis of equilibrium and out-of-equilibrium transport is interpretive of the measured dynamics rather than a closed mathematical loop. No self-citations, ansatzes, or uniqueness theorems are invoked in a load-bearing way within the provided text. The work is therefore self-contained against external benchmarks of microscopy data.

Axiom & Free-Parameter Ledger

0 free parameters · 2 axioms · 0 invented entities

The work is experimental and relies on standard assumptions of single-molecule fluorescence microscopy rather than new theoretical postulates or fitted parameters.

axioms (2)
  • domain assumption Fluorescent labeling does not significantly perturb the adsorption, diffusion, or frictional behavior of the PEG chains.
    Standard assumption in single-molecule studies; invoked implicitly when interpreting all observed dynamics as native macromolecular behavior.
  • domain assumption Observed trajectory statistics accurately reflect interfacial frictional interactions without dominant optical or flow-induced artifacts.
    Required for the attribution of mixed friction and the conformational-heterogeneity interpretation of friction distributions.

pith-pipeline@v0.9.0 · 5550 in / 1509 out tokens · 95183 ms · 2026-05-08T16:41:38.005969+00:00 · methodology

discussion (0)

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Reference graph

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