arXiv subjects

Benjamin Guiselin

Publications and source records attributed to Benjamin Guiselin.

14 recordsLinked to original sources

arXiv2026

An exactly solvable macroscopic fluctuation theory of single-file diffusion

Single-file diffusion is a ubiquitous phenomenon in low-dimensional systems, arising in transport inside narrow channels. Its natural continuum model is a one-dimensional gas of extended Brownian hard rods (BHR). Perhaps owing to the perceived intractability of this problem, much of the literature has traditionally focused on lattice exclusion models, where integrability methods have yielded remarkable, albeit limited, exact results. A major recent advance comes from a formal solution of macroscopic fluctuation theory (MFT) for the exclusion process. Yet, despite the formal solution, only a handful of properties have been made explicit. We show that the corresponding MFT of the extended BHR gas is in fact exactly solvable through a canonical transformation. We demonstrate this by explicit computation of the large-deviation statistics of the tracer-position and integrated-current in both annealed and quenched ensembles. We further show that an analogous canonical transformation applies to the MFT of lattice gases with finite-volume exclusion, yielding corresponding tracer and current statistics. We validate our results using rare-event simulations for both the continuum and the lattice models.

cond-mat.stat-mech↗

arXiv2026

Universal tracer statistics in single-file transport

We uncover an emergent universality in the large-scale, long-time statistics of a one-dimensional hard-rod gas evolving under two fundamentally different classes of microscopic dynamics: stochastic (diffusive) and unitary (ballistic). Remarkably, despite the difference of the two systems, the one-time joint distribution of the positions of multiple tracers exhibits identical non-Gaussian fluctuations, up to a simple dynamical scaling. This universality holds in both annealed and quenched ensembles, demonstrating a persistent memory of the initial state. Differences between the dynamics manifest at large scales only in multi-time statistics. Our conclusions are based on explicit large-deviation results for the one-time statistics of tracer pairs and the two-time statistics of a single tracer. Similar physics extends to current fluctuations, demonstrated explicitly in the quenched ensemble. We obtain these results from exact microscopic solutions for both dynamics and, independently, from fluctuating hydrodynamics in the ballistic case in the annealed ensemble. Our rare-event simulations further corroborate these findings and provide a novel demonstration of sampling atypical fluctuations in both types of hard-rod gas.

cond-mat.stat-mech↗

arXiv2024

Dynamical phase transitions in certain non-ergodic stochastic processes

We present a class of stochastic processes in which the large deviation functions of time-integrated observables exhibit singularities that relate to dynamical phase transitions of trajectories. These illustrative examples include Brownian motion with a death rate or in the presence of an absorbing wall, for which we consider a set of empirical observables such as the net displacement, local time, residence time, and area under the trajectory. Using a backward Fokker-Planck approach, we derive the large deviation functions of these observables, and demonstrate how singularities emerge from a competition between survival and diffusion. Furthermore, we analyse this scenario using an alternative approach with tilted operators, showing that at the singular point, the effective dynamics undergoes an abrupt transition. Extending this approach, we show that similar transitions may generically arise in Markov chains with transient states. This scenario is robust and generalizable for non-Markovian dynamics and for many-body systems, potentially leading to multiple dynamical phase transitions. We have confirmed most of our findings on the singular large-deviation function using rare-event simulation techniques.

cond-mat.stat-mech↗

arXiv2023

Curvature heterogeneities act as singular perturbations to smooth Laplacian fields: a fluid mechanics demonstration

In this Letter, we use a model fluid mechanics experiment to elucidate the impact of curvature heterogeneities on two-dimensional fields deriving from harmonic potential functions. This result is directly relevant to explain the smooth stationary structures in physical systems as diverse as curved liquid crystal and magnetic films, heat and Ohmic transport in wrinkled two-dimensional materials and flows in confined channels. Combining microfluidic experiments and theory, we explain how curvature heterogeneities shape confined viscous flows. We show that isotropic bumps induce local distortions to Darcy's flows whereas anisotropic curvature heterogeneities disturb them algebraically over system-spanning scales. Thanks to an electrostatic analogy, we gain insight into this singular geometric perturbation, and quantitatively explain it using both conformal mapping and numerical simulations. Altogether our findings establish the robustness of our experimental observations and their broad relevance to all Laplacian problems beyond the specifics of our fluid mechanics experiment.

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arXiv2022

Thirty milliseconds in the life of a supercooled liquid

We combine the swap Monte Carlo algorithm to long multi-CPU molecular dynamics simulations to analyse the equilibrium relaxation dynamics of model supercooled liquids over a time window covering ten orders of magnitude for temperatures down to the experimental glass transition temperature $T_g$. The analysis of \rev{several} time correlation functions coupled to spatio-temporal resolution of particle motion allow us to elucidate the nature of the equilibrium dynamics in deeply supercooled liquids. We find that structural relaxation starts at early times in rare localised regions characterised by a waiting time distribution that develops a power law near $T_g$. At longer times, relaxation events accumulate with increasing probability in these regions as $T_g$ is approached. This accumulation leads to a power-law growth of the linear extension of relaxed domains with time with a large, temperature-dependent dynamic exponent. Past the average relaxation time, unrelaxed domains slowly shrink with time due to relaxation events happening at their boundaries. Our results provide a complete microscopic description of the particle motion responsible for key experimental signatures of glassy dynamics, from the shape and temperature evolution of relaxation spectra to the core features of dynamic heterogeneity. They also provide a microscopic basis to understand the emergence of dynamic facilitation in deeply supercooled liquids and allow us to critically reassess theoretical descriptions of the glass transition.

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arXiv2022

Is glass a state of matter?

Glass is everywhere. We use and are surrounded by glass objects which make tangible the reality of glass as a distinct state of matter. Yet, glass as we know it is usually obtained by cooling a liquid sufficiently rapidly below its melting point to avoid crystallisation. The viscosity of this supercooled liquid increases by many orders of magnitude upon cooling, until the liquid becomes essentially arrested on experimental timescales below the ``glass transition'' temperature. From a structural viewpoint, the obtained glass still very much resembles the disordered liquid, but from a mechanical viewpoint, it is as rigid as an ordered crystal. Does glass qualify as a separate state of matter? We provide a pedagogical perspective on this question using basic statistical mechanical concepts. We recall the definitions of states of matter and of phase transitions between them. We review recent theoretical results suggesting why and how an ``ideal glass'' can indeed be defined as a separate equilibrium state of matter. We discuss recent success of computer simulations trying to analyse this glass state. We close with some experimental perspectives.

cond-mat.stat-mech↗

arXiv2022

Microscopic origin of excess wings in relaxation spectra of supercooled liquids

Glass formation is encountered in diverse materials. Experiments have revealed that dynamic relaxation spectra of supercooled liquids generically become asymmetric near the glass transition temperature, $T_g$, where an extended power law emerges at high frequencies. The microscopic origin of this "wing" remains unknown, and was so far inaccessible to simulations. Here, we develop a novel computational approach and study the equilibrium dynamics of model supercooled liquids near $T_g$. We demonstrate the emergence of a power law wing in numerical spectra, which originates from relaxation at rare, localised regions over broadly-distributed timescales. We rationalise the asymmetric shape of relaxation spectra by constructing an empirical model associating heterogeneous activated dynamics with dynamic facilitation, which are the two minimal physical ingredients revealed by our simulations. Our work offers a glimpse of the molecular motion responsible for glass formation at relevant experimental conditions.

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arXiv2022

Static self-induced heterogeneity in glass-forming liquids: Overlap as a microscope

We propose and numerically implement a local probe of the static self-induced heterogeneity characterizing glass-forming liquids. The method relies on the equilibrium statistics of the overlap between pairs of configurations measured in mesoscopic cavities with unconstrained boundaries. By systematically changing the location of the probed cavity, we directly detect spatial variations of the overlap fluctuations. We provide a detailed analysis of the statistics of a local estimate of the configurational entropy and we infer an estimate of the surface tension between amorphous states, ingredients that are both at the basis of the random first-order transition theory of glass formation. Our results represent the first direct attempt to visualize and quantify the self-induced heterogeneity underpinning the thermodynamics of glass formation. They pave the way for the development of coarse-grained effective theories and for a direct assessment of the role of thermodynamics in the activated dynamics of deeply supercooled liquids.

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arXiv2022

Statistical mechanics of coupled supercooled liquids in finite dimensions

We study the statistical mechanics of supercooled liquids when the system evolves at a temperature $T$ with a field $ε$ linearly coupled to its overlap with a reference configuration of the same liquid sampled at a temperature $T_0$. We use mean-field theory to fully characterize the influence of the reference temperature $T_0$, and we mainly study the case of a fixed, low-$T_0$ value in computer simulations. We numerically investigate the extended phase diagram in the $(ε,T)$ plane of model glass-forming liquids in spatial dimensions $d=2$ and $d=3$, relying on umbrella sampling and reweighting techniques. For both $2d$ and $3d$ cases, a similar phenomenology with nontrivial thermodynamic fluctuations of the overlap is observed at low temperatures, but a detailed finite-size analysis reveals qualitatively distinct behaviors. We establish the existence of a first-order transition line for nonzero $ε$ ending in a critical point in the universality class of the random-field Ising model (RFIM) in $d=3$. In $d=2$ instead, no phase transition is found in large enough systems at least down to temperatures below the extrapolated calorimetric glass transition temperature $T_g$. Our results confirm that glass-forming liquid samples of limited size display the thermodynamic fluctuations expected for finite systems undergoing a random first-order transition. They also support the relevance of the physics of the RFIM for supercooled liquids, which may then explain the qualitative difference between $2d$ and $3d$ glass-formers.

cond-mat.stat-mech↗

arXiv2021

Excess wings and asymmetric relaxation spectra in a facilitated trap model

In a recent computer study, we have shown that the combination of spatially heterogeneous dynamics and kinetic facilitation provides a microscopic explanation for the emergence of excess wings in deeply supercooled liquids. Motivated by these findings, we construct a minimal empirical model to describe this physics and introduce dynamic facilitation in the trap model, which was initially developed to capture the thermally-activated dynamics of glassy systems. We fully characterise the relaxation dynamics of this facilitated trap model varying the functional form of energy distributions and the strength of dynamic facilitation, combining numerical results and analytic arguments. Dynamic facilitation generically accelerates the relaxation of the deepest traps, thus making relaxation spectra strongly asymmetric, with an apparent "excess" signal at high frequencies. For well-chosen values of the parameters, the obtained spectra mimic experimental results for organic liquids displaying an excess wing. Overall, our results identify the minimal physical ingredients needed to describe excess processes in relaxation spectra of supercooled liquids.

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arXiv2020

On the overlap between configurations in glassy liquids

The overlap, or similarity, between liquid configurations is at the core of the mean-field description of the glass transition, and remains a useful concept when studying three-dimensional glass-forming liquids. In liquids, however, the overlap involves a tolerance, typically of a fraction $a/σ$ of the inter-particle distance, associated with how precisely similar two configurations must be for belonging to the same physically relevant "state". Here, we systematically investigate the dependence of the overlap fluctuations and of the resulting phase diagram when the tolerance is varied over a large range. We show that while the location of the dynamical and thermodynamic glass transitions (if present) is independent of $a/σ$, that of the critical point associated with a transition between a low- and a high-overlap phases in the presence of an applied source nontrivially depends on the value of $a/σ$. We rationalize our findings by using liquid-state theory and the hypernetted chain (HNC) approximation for correlation functions. In addition, we confirm the theoretical trends by studying a three-dimensional glass-former by computer simulations. We show in particular that \rev{a range of $a/σ$ below what is commonly considered maximizes the temperature of the critical point, pushing it up in a liquid region where viscosity is low and computer investigations are easier due to a significantly faster equilibration.

cond-mat.stat-mech↗

arXiv2020

Random-field Ising model criticality in a glass-forming liquid

We use computer simulations to investigate the extended phase diagram of a supercooled liquid linearly coupled to a quenched reference configuration. An extensive finite-size scaling analysis demonstrates the existence of a random-field Ising model (RFIM) critical point and of a first-order transition line, in agreement with recent field-theoretical approaches. The dynamics in the vicinity of this critical point resembles the peculiar activated scaling of RFIM-like systems, and the overlap autocorrelation displays a logarithmic stretching. Our study demonstrates RFIM criticality in the thermodynamic limit for a three-dimensional supercooled liquids at equilibrium.

cond-mat.stat-mech↗

arXiv2020

Stable glassy configurations of the Kob-Andersen model using swap Monte Carlo

The swap Monte Carlo algorithm allows the preparation of highly stable glassy configurations for a number of glass-formers, but is inefficient for some models, such as the much studied binary Kob-Andersen (KA) mixture. We have recently developed generalisations to the KA model where swap can be very effective. Here, we show that these models can in turn be used to considerably enhance the stability of glassy configurations in the original KA model at no computational cost. We successfully develop several numerical strategies both in and out of equilibrium to achieve this goal and show how to optimise them. We provide several physical measurements indicating that the proposed algorithms considerably enhance mechanical and thermodynamic stability in the KA model, including a transition towards brittle yielding behaviour. Our results thus pave the way for future studies of stable glasses using the KA model.

cond-mat.stat-mech↗

arXiv2018

Dynamic Morphologies and Stability of Droplet Interface Bilayers

We develop a theoretical framework for understanding dynamic morphologies and stability of droplet interface bilayers (DIBs), accounting for lipid kinetics in the monolayers and bilayer, and droplet evaporation due to imbalance between osmotic and Laplace pressures. Our theory quantitatively describes distinct pathways observed in experiments when DIBs become unstable. We find that when the timescale for lipid desorption is slow compared to droplet evaporation, the lipid bilayer will grow and the droplets approach a hemispherical shape. In contrast, when lipid desorption is fast, the bilayer area will shrink and the droplets eventually detach. Our model also suggests there is a critical size below which DIBs cannot be stable, which may explain experimental difficulties in miniaturising the DIB platform.

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