Ductile-to-brittle transition and yielding in soft amorphous materials: perspectives and open questions.

Soft amorphous materials are viscoelastic solids ubiquitously found around us, from clays and cementitious pastes to emulsions and physical gels encountered in food or biomedical engineering. Under an external deformation, these materials undergo a noteworthy transition from a solid to a liquid state that reshapes the material microstructure. This yielding transition was the main theme of a workshop held from January 9 to 13, 2023 at the Lorentz Center in Leiden. The manuscript presented here offers a critical perspective on the subject, synthesizing insights from the various brainstorming sessions and informal discussions that unfolded during this week of vibrant exchange of ideas. The result of these exchanges takes the form of a series of open questions that represent outstanding experimental, numerical, and theoretical challenges to be tackled in the near future.

Elasticity, Facilitation, and Dynamic Heterogeneity in Glass-Forming Liquids.

We study the role of elasticity-induced facilitation on the dynamics of glass-forming liquids by a coarse-grained two-dimensional model in which local relaxation events, taking place by thermal activation, can trigger new relaxations by long-range elastically mediated interactions. By simulations and an analytical theory, we show that the model reproduces the main salient facts associated with dynamic heterogeneity and offers a mechanism to explain the emergence of dynamical correlations at the glass transition. We also discuss how it can be generalized and combined with current theories.

Predicting Dynamic Heterogeneity in Glass-Forming Liquids by Physics-Inspired Machine Learning.

We introduce GlassMLP, a machine learning framework using physics-inspired structural input to predict the long-time dynamics in deeply supercooled liquids. We apply this deep neural network to atomistic models in 2D and 3D. Its performance is better than the state of the art while being more parsimonious in terms of training data and fitting parameters. GlassMLP quantitatively predicts four-point dynamic correlations and the geometry of dynamic heterogeneity. Transferability across system sizes allows us to efficiently probe the temperature evolution of spatial dynamic correlations, revealing a profound change with temperature in the geometry of rearranging regions.

Generalized Lotka-Volterra Equations with Random, Nonreciprocal Interactions: The Typical Number of Equilibria.

We compute the typical number of equilibria of the generalized Lotka-Volterra equations describing species-rich ecosystems with random, nonreciprocal interactions using the replicated Kac-Rice method. We characterize the multiple-equilibria phase by determining the average abundance and similarity between equilibria as a function of their diversity (i.e., of the number of coexisting species) and of the variability of the interactions. We show that linearly unstable equilibria are dominant, and that the typical number of equilibria differs with respect to the average number.

Artificial selection of communities drives the emergence of structured interactions.

Species-rich communities, such as the microbiota or microbial ecosystems, provide key functions for human health and climatic resilience. Increasing effort is being dedicated to design experimental protocols for selecting community-level functions of interest. These experiments typically involve selection acting on populations of communities, each of which is composed of multiple species. If numerical simulations started to explore the evolutionary dynamics of this complex, multi-scale system, a comprehensive theoretical understanding of the process of artificial selection of communities is still lacking. Here, we propose a general model for the evolutionary dynamics of communities composed of a large number of interacting species, described by disordered generalised Lotka-Volterra equations. Our analytical and numerical results reveal that selection for scalar community functions leads to the emergence, along an evolutionary trajectory, of a low-dimensional structure in an initially featureless interaction matrix. Such structure reflects the combination of the properties of the ancestral community and of the selective pressure. Our analysis determines how the speed of adaptation scales with the system parameters and the abundance distribution of the evolved communities. Artificial selection for larger total abundance is thus shown to drive increased levels of mutualism and interaction diversity. Inference of the interaction matrix is proposed as a method to assess the emergence of structured interactions from experimentally accessible measures.

Finite-Disorder Critical Point in the Yielding Transition of Elastoplastic Models.

Upon loading, amorphous solids can exhibit brittle yielding, with the abrupt formation of macroscopic shear bands leading to fracture, or ductile yielding, with a multitude of plastic events leading to homogeneous flow. It has been recently proposed, and subsequently questioned, that the two regimes are separated by a sharp critical point, as a function of some control parameter characterizing the intrinsic disorder strength and the degree of stability of the solid. In order to resolve this issue, we have performed extensive numerical simulations of athermally driven elastoplastic models with long-range and anisotropic realistic interaction kernels in two and three dimensions. Our results provide clear evidence for a finite-disorder critical point separating brittle and ductile yielding, and we provide an estimate of the critical exponents in 2D and 3D.

Local Dynamical Heterogeneity in Simple Glass Formers.

We study the local dynamical fluctuations in glass-forming models of particles embedded in d-dimensional space, in the mean-field limit of d→∞. Our analytical calculation reveals that single-particle observables, such as squared particle displacements, display divergent fluctuations around the dynamical (or mode-coupling) transition, due to the emergence of nontrivial correlations between displacements along different directions. This effect notably gives rise to a divergent non-Gaussian parameter, α_{2}. The d→∞ local dynamics therefore becomes quite rich upon approaching the glass transition. The finite-d remnant of this phenomenon further provides a long sought-after, first-principle explanation for the growth of α_{2} around the glass transition that is not based on multiparticle correlations.

Properties of Equilibria and Glassy Phases of the Random Lotka-Volterra Model with Demographic Noise.

We study a reference model in theoretical ecology, the disordered Lotka-Volterra model for ecological communities, in the presence of finite demographic noise. Our theoretical analysis, valid for symmetric interactions, shows that for sufficiently heterogeneous interactions and low demographic noise the system displays a multiple equilibria phase, which we fully characterize. In particular, we show that in this phase the number of locally stable equilibria is exponential in the number of species. Upon further decreasing the demographic noise, we unveil the presence of a second transition like the so-called "Gardner" transition to a marginally stable phase similar to that observed in the jamming of amorphous materials. We confirm and complement our analytical results by numerical simulations. Furthermore, we extend their relevance by showing that they hold for other interacting random dynamical systems such as the random replicant model. Finally, we discuss their extension to the case of asymmetric couplings.

Searching for the Gardner Transition in Glassy Glycerol.

We search for a Gardner transition in glassy glycerol, a standard molecular glass, measuring the third harmonics cubic susceptibility χ_{3}^{(3)} from slightly below the usual glass transition temperature down to 10 K. According to the mean-field picture, if local motion within the glass were becoming highly correlated due to the emergence of a Gardner phase then χ_{3}^{(3)}, which is analogous to the dynamical spin-glass susceptibility, should increase and diverge at the Gardner transition temperature T_{G}. We find instead that upon cooling |χ_{3}^{(3)}| decreases by several orders of magnitude and becomes roughly constant in the regime 100-10 K. We rationalize our findings by assuming that the low temperature physics is described by localized excitations weakly interacting via a spin-glass dipolar pairwise interaction in a random magnetic field. Our quantitative estimations show that the spin-glass interaction is twenty to fifty times smaller than the local random field contribution, thus rationalizing the absence of the spin-glass Gardner phase. This hints at the fact that a Gardner phase may be suppressed in standard molecular glasses, but it also suggests ways to favor its existence in other amorphous solids and by changing the preparation protocol.

Elastoplasticity Mediates Dynamical Heterogeneity Below the Mode Coupling Temperature.

As liquids approach the glass transition temperature, dynamical heterogeneity emerges as a crucial universal feature of their behavior. Dynamic facilitation, where local motion triggers further motion nearby, plays a major role in this phenomenon. Here we show that long-ranged, elastically mediated facilitation appears below the mode coupling temperature, adding to the short-range component present at all temperatures. Our results suggest deep connections between the supercooled liquid and glass states, and pave the way for a deeper understanding of dynamical heterogeneity in glassy systems.

Complex interactions can create persistent fluctuations in high-diversity ecosystems.

When can ecological interactions drive an entire ecosystem into a persistent non-equilibrium state, where many species populations fluctuate without going to extinction? We show that high-diversity spatially heterogeneous systems can exhibit chaotic dynamics which persist for extremely long times. We develop a theoretical framework, based on dynamical mean-field theory, to quantify the conditions under which these fluctuating states exist, and predict their properties. We uncover parallels with the persistence of externally-perturbed ecosystems, such as the role of perturbation strength, synchrony and correlation time. But uniquely to endogenous fluctuations, these properties arise from the species dynamics themselves, creating feedback loops between perturbation and response. A key result is that fluctuation amplitude and species diversity are tightly linked: in particular, fluctuations enable dramatically more species to coexist than at equilibrium in the very same system. Our findings highlight crucial differences between well-mixed and spatially-extended systems, with implications for experiments and their ability to reproduce natural dynamics. They shed light on the maintenance of biodiversity, and the strength and synchrony of fluctuations observed in natural systems.

Revisiting the concept of activation in supercooled liquids.

In this work, we revisit the description of dynamics based on the concepts of metabasins and activation in mildly supercooled liquids via the analysis of the dynamics of a paradigmatic glass former between its onset temperature [Formula: see text] and mode-coupling temperature [Formula: see text]. First, we provide measures that demonstrate that the onset of glassiness is indeed connected to the landscape, and that metabasin waiting time distributions are so broad that the system can remain stuck in a metabasin for times that exceed [Formula: see text] by orders of magnitude. We then reanalyze the transitions between metabasins, providing several indications that the standard picture of activated dynamics in terms of traps does not hold in this regime. Instead, we propose that here activation is principally driven by entropic instead of energetic barriers. In particular, we illustrate that activation is not controlled by the hopping of high energetic barriers and should more properly be interpreted as the entropic selection of nearly barrierless but rare pathways connecting metabasins on the landscape.

Random critical point separates brittle and ductile yielding transitions in amorphous materials.

We combine an analytically solvable mean-field elasto-plastic model with molecular dynamics simulations of a generic glass former to demonstrate that, depending on their preparation protocol, amorphous materials can yield in two qualitatively distinct ways. We show that well-annealed systems yield in a discontinuous brittle way, as metallic and molecular glasses do. Yielding corresponds in this case to a first-order nonequilibrium phase transition. As the degree of annealing decreases, the first-order character becomes weaker and the transition terminates in a second-order critical point in the universality class of an Ising model in a random field. For even more poorly annealed systems, yielding becomes a smooth crossover, representative of the ductile rheological behavior generically observed in foams, emulsions, and colloidal glasses. Our results show that the variety of yielding behaviors found in amorphous materials does not necessarily result from the diversity of particle interactions or microscopic dynamics but is instead unified by carefully considering the role of the initial stability of the system.

Real space renormalization group theory of disordered models of glasses.

We develop a real space renormalization group analysis of disordered models of glasses, in particular of the spin models at the origin of the random first-order transition theory. We find three fixed points, respectively, associated with the liquid state, with the critical behavior, and with the glass state. The latter two are zero-temperature ones; this provides a natural explanation of the growth of effective activation energy scale and the concomitant huge increase of relaxation time approaching the glass transition. The lower critical dimension depends on the nature of the interacting degrees of freedom and is higher than three for all models. This does not prevent 3D systems from being glassy. Indeed, we find that their renormalization group flow is affected by the fixed points existing in higher dimension and in consequence is nontrivial. Within our theoretical framework, the glass transition results in an avoided phase transition.

Can the glass transition be explained without a growing static length scale?

It was recently discovered that SWAP, a Monte Carlo algorithm that involves the exchange of pairs of particles of differing diameters, can dramatically accelerate the equilibration of simulated supercooled liquids in regimes where the normal dynamics is glassy. This spectacular effect was subsequently interpreted as direct evidence against a static, cooperative explanation of the glass transition such as the one offered by the random first-order transition (RFOT) theory. We explain the speedup induced by SWAP within the framework of the RFOT theory. We suggest that the efficiency of SWAP stems from a postponed onset of glassy dynamics. We describe this effect in terms of "crumbling metastability" and use the example of nucleation to illustrate the possibility of circumventing free-energy barriers of thermodynamic origin by a change in the local dynamical rules.

Gardner physics in amorphous solids and beyond.

One of the most remarkable predictions to emerge out of the exact infinite-dimensional solution of the glass problem is the Gardner transition. Although this transition was first theoretically proposed a generation ago for certain mean-field spin glass models, its materials relevance was only realized when a systematic effort to relate glass formation and jamming was undertaken. A number of nontrivial physical signatures associated with the Gardner transition have since been considered in various areas, from models of structural glasses to constraint satisfaction problems. This perspective surveys these recent advances and discusses the novel research opportunities that arise from them.

Spinodals with Disorder: From Avalanches in Random Magnets to Glassy Dynamics.

We revisit the phenomenon of spinodals in the presence of quenched disorder and develop a complete theory for it. We focus on the spinodal of an Ising model in a quenched random field (RFIM), which has applications in many areas from materials to social science. By working at zero temperature in the quasistatically driven RFIM, thermal fluctuations are eliminated and one can give a rigorous content to the notion of spinodal. We show that the latter is due to the depinning and the subsequent expansion of rare droplets. We work out the associated critical behavior, which, in any finite dimension, is very different from the mean-field one: the characteristic length diverges exponentially and the thermodynamic quantities display very mild nonanalyticities much like in a Griffith phenomenon. From the recently established connection between the spinodal of the RFIM and glassy dynamics, our results also allow us to conclusively assess the physical content and the status of the dynamical transition predicted by the mean-field theory of glass-forming liquids.

Spin glass in a field: a new zero-temperature fixed point in finite dimensions.

By using real-space renormalization group (RG) methods, we show that spin glasses in a field display a new kind of transition in high dimensions. The corresponding critical properties and the spin-glass phase are governed by two nonperturbative zero-temperature fixed points of the RG flow. We compute the critical exponents and discuss the RG flow and its relevance for three-dimensional systems. The new spin-glass phase we discovered has unusual properties, which are intermediate between the ones conjectured by droplet and full replica symmetry-breaking theories. These results provide a new perspective on the long-standing debate about the behavior of spin glasses in a field.

Ideal glass transitions by random pinning.

We study the effect of freezing the positions of a fraction c of particles from an equilibrium configuration of a supercooled liquid at a temperature T. We show that within the random first-order transition theory pinning particles leads to an ideal glass transition for a critical fraction c = c(K)(T) even for moderate supercooling; e.g., close to the Mode-Coupling transition temperature. First we derive the phase diagram in the T - c plane by mean field approximations. Then, by applying a real-space renormalization group method, we obtain the critical properties for |c - c(K)(T)| â†’ 0, in particular the divergence of length and time scales, which are dominated by two zero-temperature fixed points. We also show that for c = c(K)(T) the typical distance between frozen particles is related to the static point-to-set length scale of the unconstrained liquid. We discuss what are the main differences when particles are frozen in other geometries and not from an equilibrium configuration. Finally, we explain why the glass transition induced by freezing particles provides a new and very promising avenue of research to probe the glassy state and ascertain, or disprove, the validity of the theories of the glass transition.

Random-field-like criticality in glass-forming liquids.

We introduce an approach to derive an effective scalar field theory for the glass transition; the fluctuating field is the overlap between equilibrium configurations. We apply it to the case of constrained liquids for which the introduction of a conjugate source to the overlap field was predicted to lead to an equilibrium critical point. We show that the long-distance physics in the vicinity of this critical point is in the same universality class as that of a paradigmatic disordered model: the random-field Ising model. The quenched disorder is provided here by a reference equilibrium liquid configuration. We discuss to what extent this field-theoretical description and the mapping to the random field Ising model hold in the whole supercooled liquid regime, in particular, near the glass transition.