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Corentin C. L. Laudicina

Publications and source records attributed to Corentin C. L. Laudicina.

8 recordsLinked to original sources

Theory of the $β$-Relaxation Beyond Mode-Coupling Theory: A Microscopic Treatment

We develop a systematic extension of mode-coupling theory (MCT) that incorporates critical dynamical fluctuations. Starting from a microscopic diagrammatic theory, we identify dominant classes of divergent diagrams near the mode-coupling transition and show that the corresponding asymptotic series dominates the mean-field below an upper critical dimension $d_c=8$. To resum these divergences, we construct a mapping to a stochastic dynamical process in which the order parameter evolves under random spatiotemporal fields. This reformulation provides a controlled, fully dynamical derivation of an effective theory for the $β$-relaxation which remarkably coincides with stochastic beta-relaxation theory [T. Rizzo, EPL 106, 56003 (2014)]. All coupling constants of the latter theory are expressed microscopically in terms of the liquid static structure factor and are computed for the paradigmatic hard-sphere system. The analysis demonstrates that fluctuations alone restore ergodicity and replace the putative mean-field transition by a smooth crossover. Our results establish a predictive framework for structural relaxation beyond mean-field.

cond-mat.stat-mech↗

Microscopic Theory of a Fluctuation-Induced Dynamical Crossover in Supercooled Liquids

Mean-field theories of the glass transition predict a phase transition to a dynamically arrested state, yet no such transition is observed in experiments or simulations of finite-dimensional systems. We resolve this long-standing discrepancy by incorporating critical dynamical fluctuations into a microscopic mode-coupling framework. We show that these fluctuations round off the mean-field singularity and restore ergodicity at all finite densities (or temperatures) without invoking activated dynamics or facilitation. The resulting effective theory describes the order parameter as a stochastic process with self-induced, annealed disorder, determined self-consistently at the mean-field level. In the $β$-relaxation regime it reduces to stochastic beta-relaxation theory, thereby unifying mode-coupling and replica-based approaches beyond mean-field. All parameters of the stochastic $β$-relaxation theory are fixed by the static structure, enabling parameter-free predictions that extend mean-field theory into finite dimensions.

cond-mat.soft↗

Non-Monotonic Dynamical Correlations Across The Glass Crossover

The dramatic slowing down of structural relaxation in supercooled liquids is accompanied by the emergence of dynamic heterogeneity. A monotonically increasing dynamical correlation length, measured at the $α$-timescale, is one of the remarkable features of this phenomenon. Here we show that this picture is incomplete: the dynamical correlation length measured in the $β$-relaxation regime exhibits a striking non-monotonic temperature dependence, reaching a maximum near the mode-coupling crossover temperature $T_c$ and decreasing upon further cooling, even as local dynamical fluctuations continue to intensify. This behavior suggests a crossover from spatially extended, maximally cooperative motion near $T_c$ to increasingly compact and localized relaxation events below it. We demonstrate that this evolution is quantitatively captured by stochastic beta-relaxation theory, an extension of mode-coupling theory beyond mean-field that explicitly predicts an avoided dynamical transition in finite dimensions. Our results provide the first direct spatial evidence in favor of the avoided-transition picture of the mode-coupling crossover, and establish the peak of the $β$-regime correlation length as a robust indicator of the mode-coupling crossover.

cond-mat.soft↗

Simple fluctuations in simple glass formers

Critical single-particle fluctuations associated with particle displacements are inherent to simple glass-forming liquids in the limit of large dimensions and leave a pseudo-critical trace across all finite dimensions. This characteristic could serve as a crucial test for distinguishing between theories of glass formation. We here examine these critical fluctuations, as captured by the well-established non-Gaussian parameter, within both mode-coupling theory (MCT) and dynamical mean-field theory (DMFT) across dimensions for hard sphere liquids and for the minimally structured Mari--Kurchan model. We establish general scaling laws relevant to any liquid dynamics theory in large dimensions and show that the dimensional scalings predicted by MCT are inconsistent with those from DMFT. Simulation results for hard spheres in moderately high dimensions align with the DMFT scenario, reinforcing the relevance of mean-field theory for capturing glass physics in finite dimensions. We identify potential adjustments to MCT to account for certain mean-field physics. Our findings also highlight that local structure and spatial dimensionality can affect single-particle critical fluctuations in non-trivial ways.

cond-mat.dis-nn↗

Competing Relaxation Channels in Continuously Polydisperse Fluids: A Mode-Coupling Study

Systems with a high degree of size polydispersity are becoming standard in the computational study of deeply supercooled liquids. In this work we perform a systematic analysis of continuously polydisperse fluids as a function of the degree of polydispersity within the framework of the Mode-Coupling Theory of the glass transition (MCT). Our results show that a high degree of polydispersity tends to stabilize the liquid phase against vitrification, the magnitude of which depends on the shape of the polydispersity distribution. Further, we report on a separation between the localization lengths of the smallest and largest particles. A diameter-resolved analysis of the intermediate scattering functions reveals that this separation significantly stretches the relaxation patterns, which we quantitatively study by an analysis of the dynamical exponents predicted by the theory. Our observations have strong implications for our understanding of the nature of dynamical heterogeneities and localization lengths in continuously polydisperse systems. These results suggest that the dynamics of the smallest particles is of central importance to understand structural relaxation of continuously size polydisperse fluids, already in the mildly supercooled regime where MCT is usually applicable.

cond-mat.soft↗

Influence of polydispersity on the relaxation mechanisms of glassy liquids

State-of-the-art techniques for simulating deeply supercooled liquids require a high degree of size polydispersity to be effective. While these techniques have enabled great insight into the microscopic dynamics near the glass transition, the effect of the large polydispersity on the dynamics has remained largely unstudied. Here we show that a particle's size not only has a strong correlation with its mobility, but we also observe that, as the mode-coupling temperature is crossed and the system becomes more deeply supercooled, a dynamic separation between small mobile and larger quiescent particles emerges at timescales corresponding to cage escape. Our results suggest that the cage escape of this population of mobile particles facilitates the later structural relaxation of the quiescent particles. In the deep supercooled regime, we show that particles of different sizes display varying degrees of breakdown of the Stokes-Einstein relation and have different activation energy barriers. Overall, this indicates that it is important to account for particle-size effects when generalizing results to other glass-forming systems.

cond-mat.soft↗

Emergent structural correlations in dense liquids

The complete quantitative description of the structure of dense and supercooled liquids remains a notoriously difficult problem in statistical physics. Most studies to date focus solely on two-body structural correlations, and only a handful of papers have sought to consider additional three-body correlations. Here, we go beyond the state of the art by extracting many-body static structure factors from molecular dynamics simulations and by deriving accurate approximations up to the six-body structure factor via density functional theory. We find that supercooling manifestly increases four-body correlations, akin to the two- and three-body case. However, at small wave numbers, we observe that the four-point structure of a liquid drastically changes upon supercooling, both qualitatively and quantitatively, which is not the case in two-point structural correlations. This indicates that theories of the structure or dynamics of dense liquids should incorporate many-body correlations beyond the two-particle level to fully capture their intricate behaviour.

cond-mat.stat-mech↗

Dynamical Susceptibilities Near Ideal Glass Transitions

Building on the recently derived inhomogeneous mode-coupling theory, we extend the generalised mode-coupling theory of supercooled liquids to inhomogeneous environments. This provides a first-principles-based, systematic and rigorous way of deriving high-point dynamical susceptibilities from variations of the many-body dynamic structure factors with respect to their conjugate field. This new framework allows for a novel and fully microscopic possibility to probe for collective relaxation mechanisms in supercooled liquids near the mode-coupling glass transition.

cond-mat.stat-mech↗