Direct measurements of growing amorphous order and non-monotonic dynamic correlations in a colloidal glass-former

Abstract

While the transformation of flowing liquids into rigid glasses is omnipresent, a complete understanding of vitrification remains elusive. Of the numerous approaches aimed at solving the glass transition problem, the Random First-Order Theory (RFOT) is the most prominent. However, the existence of the underlying thermodynamic phase transition envisioned by RFOT remains debatable, since its key microscopic predictions concerning the growth of amorphous order and the nature of dynamic correlations lack experimental verification. Here, by using holographic optical tweezers, we freeze a wall of particles in an equilibrium configuration of a 2D colloidal glass-forming liquid and provide direct evidence for growing amorphous order in the form of a static point-to-set length. Most remarkably, we uncover the non-monotonic dependence of dynamic correlations on area fraction and show that this non-monotonicity follows directly from the change in morphology of cooperatively rearranging regions, as predicted by RFOT. Our findings suggest that the glass transition has a thermodynamic origin.

References in corpus (28)

• Theoretical perspective on the glass transition and amorphous materials
• String-like Clusters and Cooperative Motion in a Model Glass-Forming Liquid
• Direct experimental evidence of a growing length scale accompanying the glass transition
• Theory of Structural Glasses and Supercooled Liquids
• Dynamics on the Way to Forming Glass: Bubbles in Space-time
• On the Adam-Gibbs-Wolynes scenario for the viscosity increase in glasses
• The frustration-based approach of supercooled liquids and the glass transition: a review and critical assessment
• Thermodynamic signature of growing amorphous order in glass-forming liquids
• The Shapes of Cooperatively Rearranging Regions in Glass Forming Liquids
• The Relationship of Dynamical Heterogeneity to the Adam-Gibbs and Random First-Order Transition Theories of Glass Formation
• Cooperative motion and growing length scales in supercooled confined liquids
• Rigorous Inequalities between Length and Time Scales in Glassy Systems
• Non-monotonic temperature evolution of dynamic correlations in glass-forming liquids
• Static point-to-set correlations in glass-forming liquids
• Growing point-to-set length scale correlates with growing relaxation times in model supercooled liquids
• A universal origin for secondary relaxations in supercooled liquids and structural glasses
• Spatially heterogeneous dynamics and dynamic facilitation in a model of viscous silica
• Universal features of dynamic heterogeneity in supercooled liquids
• Growing Dynamical Facilitation on Approaching the Random Pinning Colloidal Glass Transition
• Order in glassy systems
• Decorrelation of the static and dynamic length scales in hard-sphere glass-formers
• Direct Estimate of the Static Length-Scale Accompanying the Glass Transition
• Caging and mosaic lengthscales in plaquette spin models of glasses
• Crossovers in the dynamics of supercooled liquids probed by an amorphous wall
• Random pinning in glassy spin models with plaquette interactions
• Manifestations of Dynamical Facilitation in Glassy Materials
• Dynamical facilitation governs glassy dynamics in suspensions of colloidal ellipsoids
• Comment: Characterizing dynamic length scales in glass forming liquids

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• A Topologically Driven Glass in Ring Polymers
• Colloidal Hard Spheres: Triumphs, Challenges and Mysteries
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• Soft Modes, Localization and Two-Level Systems in Spin Glasses
• Anatomy of cage formation in a 2D glass-forming liquid
• Locally favoured structures and dynamic length scales in a simple glass-former
• Shape of Dynamical Heterogeneities and the Stokes-Einstein and Stokes-Einstein-Debye Relations in Suspensions of Colloidal Ellipsoids
• Efficient measurement of point-to-set correlations and overlap fluctuations in glass-forming liquids
• Structures and dynamics of glass-forming colloidal liquids under spherical confinement
• Direct evidence of void induced structural relaxations in colloidal glass formers
• Cage Size and Jump Precursors in Glass-Forming Liquids: Experiment and Simulations
• Block Analysis for the Calculation of Dynamic and Static Length Scales in Glass-Forming Liquids
• Experimental Determination of Configurational Entropy in a Two-Dimensional Liquid under Random Pinning
• Differential Variance Analysis of soft glassy materials: a direct method to quantify and visualize dynamic heterogeneities
• Growing Surface Tension of Amorphous-Amorphous Interfaces on Approaching the Colloidal Glass Transition
• Coarse-grained Soft-Clusters Remain non-Diffusing in the Melt State
• Relation between heterogeneous frozen regions in supercooled liquids and non-Debye spectrum in the corresponding glasses
• The glass transition in molecules, colloids and grains: universality and specificity
• Non-monotonic dynamic correlations beneath the surface of glass-forming liquids
• On the overlap between configurations in glassy liquids
• Shear Banding, Intermittency, Jamming and Dynamic Phases for Skyrmions in Inhomogeneous Pinning Arrays
• Local Plastic Response and Slow Heterogeneous Dynamics of Supercooled Liquids
• Reduced strength and extent of dynamic heterogeneity in a strong glass former as compared to fragile glass formers
• Active Matter Shepherding and Clustering in Inhomogeneous Environments
• Fragile-to-Strong Crossover, growing length scales, and dynamic heterogeneity in Wigner Glasses
• Aging near rough and smooth boundaries in colloidal glasses
• Dynamics in two-dimensional glassy systems of crowded Penrose kites
• Continuous time random walk concepts applied to extended mode coupling theory: A study of the Stokes-Einstein breakdown
• Are strongly confined colloids good models for two dimensional liquids?
• Concentrated suspensions of Brownian beads in water: dynamic heterogeneities trough a simple experimental technique
• Influence of an amorphous wall on the distribution of localized excitations in a colloidal glass-forming liquid
• Surface melting of a colloidal glass
• Dynamics of Rod like Particles in Supercooled Liquids -- Probing Dynamic Heterogeneity and Amorphous Order
• Effective one-component model of binary mixture: molecular arrest induced by the spatially correlated stochastic dynamics
• Neglecting polydispersity degrades propensity measurements in supercooled liquids
• Breakdown of diffusivity-entropy scaling in colloidal glass forming liquids
• Particle pinning as a method to manipulate marginal stability
• Probing the Local Response of Glass-forming Liquids by Laser Excitations
• Formation of a transient amorphous solid in low density aqueous charged sphere suspensions
• Free energy cost of forming an interface between a crystal and its frozen version
• Trapping/Pinning of colloidal microspheres over glass substrate using surface features
• Inhomogeneous Diffusion in Confined Colloidal Suspensions
• The Glass Transition: From Competing Theories to Discriminating Tests
• Stirring supercooled colloidal liquids at the particle scale
• Static self-induced heterogeneity in glass-forming liquids: Overlap as a microscope