Elasticity and rheology of auxetic granular metamaterials.

The flowing, jamming, and avalanche behavior of granular materials is satisfyingly universal and vexingly hard to tune: A granular flow is typically intermittent and will irremediably jam if too confined. Here, we show that granular metamaterials made from particles with a negative Poisson's ratio yield more easily and flow more smoothly than ordinary granular materials. We first create a collection of auxetic grains based on a re-entrant mechanism and show that each grain exhibits a negative Poisson's ratio regardless of the direction of compression. Interestingly, we find that the elastic and yielding properties are governed by the high compressibility of granular metamaterials: At a given confinement, they exhibit lower shear modulus, lower yield stress, and more frequent, smaller avalanches than materials made from ordinary grains. We further demonstrate that granular metamaterials promote flow in more complex confined geometries, such as intruder and hopper geometries, even when the packing contains only a fraction of auxetic grains. Moreover, auxetic granular metamaterials exhibit enhanced impact absorption. Our findings blur the boundary between complex fluids and metamaterials and could help in scenarios that involve process, transport, and reconfiguration of granular materials.

Enumerating low-frequency nonphononic vibrations in computer glasses.

In addition to Goldstone phonons that generically emerge in the low-frequency vibrational spectrum of any solid, crystalline or glassy, structural glasses also feature other low-frequency vibrational modes. The nature and statistical properties of these modes-often termed "excess modes"-have been the subject of decades-long investigation. Studying them, even using well-controlled computer glasses, has proven challenging due to strong spatial hybridization effects between phononic and nonphononic excitations, which hinder quantitative analyses of the nonphononic contribution DG(ω) to the total spectrum D(ω), per frequency ω. Here, using recent advances indicating that DG(ω)=D(ω)-DD(ω), where DD(ω) is Debye's spectrum of phonons, we present a simple and straightforward scheme to enumerate nonphononic modes in computer glasses. Our analysis establishes that nonphononic modes in computer glasses indeed make an additive contribution to the total spectrum, including in the presence of strong hybridizations. Moreover, it cleanly reveals the universal DG(ω)∼ω4 tail of the nonphononic spectrum, and opens the way for related analyses of experimental spectra of glasses.

Scaling regimes and fluctuations of observables in computer glasses approaching the unjamming transition.

Under decompression, disordered solids undergo an unjamming transition where they become under-coordinated and lose their structural rigidity. The mechanical and vibrational properties of these materials have been an object of theoretical, numerical, and experimental research for decades. In the study of low-coordination solids, understanding the behavior and physical interpretation of observables that diverge near the transition is of particular importance. Several such quantities are length scales (ξ or l) that characterize the size of excitations, the decay of spatial correlations, the response to perturbations, or the effect of physical constraints in the boundary or bulk of the material. Additionally, the spatial and sample-to-sample fluctuations of macroscopic observables such as contact statistics or elastic moduli diverge approaching unjamming. Here, we discuss important connections between all of these quantities and present numerical results that characterize the scaling properties of sample-to-sample contact and shear modulus fluctuations in ensembles of low-coordination disordered sphere packings and spring networks. Overall, we highlight three distinct scaling regimes and two crossovers in the disorder quantifiers χz and χµ as functions of system size N and proximity to unjamming δz. As we discuss, χX relates to the standard deviation σX of the sample-to-sample distribution of the quantity X (e.g., excess coordination δz or shear modulus µ) for an ensemble of systems. Importantly, χµ has been linked to experimentally accessible quantities that pertain to sound attenuation and the density of vibrational states in glasses. We investigate similarities and differences in the behaviors of χz and χµ near the transition and discuss the implications of our findings on current literature, unifying findings in previous studies.

Self-Oscillation and Synchronization Transitions in Elastoactive Structures.

The interplay between activity and elasticity often found in active and living systems triggers a plethora of autonomous behaviors ranging from self-assembly and collective motion to actuation. Among these, spontaneous self-oscillations of mechanical structures is perhaps the simplest and most widespread type of nonequilibrium phenomenon. Yet, we lack experimental model systems to investigate the various dynamical phenomena that may appear. Here, we introduce a centimeter-sized model system for one-dimensional elastoactive structures. We show that such structures exhibit flagellar motion when pinned at one end, self-snapping when pinned at two ends, and synchronization when coupled together with a sufficiently stiff link. We further demonstrate that these transitions can be described quantitatively by simple models of coupled pendula with follower forces. Beyond the canonical case considered here, we anticipate our work to open avenues for the understanding and design of the self-organization and response of active biological and synthetic solids, e.g., in higher dimensions and for more intricate geometries.

Anomalous linear elasticity of disordered networks.

Continuum elasticity is a powerful tool applicable in a broad range of physical systems and phenomena. Yet, understanding how and on what scales material disorder may lead to the breakdown of continuum elasticity is not fully understood. We show, based on recent theoretical developments and extensive numerical computations, that disordered elastic networks near a critical rigidity transition, such as strain-stiffened fibrous biopolymer networks that are abundant in living systems, reveal an anomalous long-range linear elastic response below a correlation length. This emergent anomalous elasticity, which is non-affine in nature, is shown to feature a qualitatively different multipole expansion structure compared to ordinary continuum elasticity, and a slower spatial decay of perturbations. The potential degree of universality of these results, their implications (e.g. for cell-cell communication through biological extracellular matrices) and open questions are briefly discussed.

Boson-peak vibrational modes in glasses feature hybridized phononic and quasilocalized excitations.

A hallmark of structural glasses and other disordered solids is the emergence of excess low-frequency vibrations on top of the Debye spectrum DDebye(ω) of phonons (ω denotes the vibrational frequency), which exist in any solid whose Hamiltonian is translationally invariant. These excess vibrations-a signature of which is a THz peak in the reduced density of states D(ω)/DDebye(ω), known as the boson peak-have resisted a complete theoretical understanding for decades. Here, we provide direct numerical evidence that vibrations near the boson peak consist of hybridizations of phonons with many quasilocalized excitations; the latter have recently been shown to generically populate the low-frequency tail of the vibrational spectra of structural glasses quenched from a melt and of disordered crystals. Our results suggest that quasilocalized excitations exist up to and in the vicinity of the boson-peak frequency and, hence, constitute the fundamental building blocks of the excess vibrational modes in glasses.

Pinching a glass reveals key properties of its soft spots.

It is now well established that glasses feature quasilocalized nonphononic excitations-coined "soft spots"-, which follow a universal [Formula: see text] density of states in the limit of low frequencies ω. All glass-specific properties, such as the dependence on the preparation protocol or composition, are encapsulated in the nonuniversal prefactor of the universal [Formula: see text] law. The prefactor, however, is a composite quantity that incorporates information both about the number of quasilocalized nonphononic excitations and their characteristic stiffness, in an apparently inseparable manner. We show that by pinching a glass-i.e., by probing its response to force dipoles-one can disentangle and independently extract these two fundamental pieces of physical information. This analysis reveals that the number of quasilocalized nonphononic excitations follows a Boltzmann-like law in terms of the parent temperature from which the glass is quenched. The latter, sometimes termed the fictive (or effective) temperature, plays important roles in nonequilibrium thermodynamic approaches to the relaxation, flow, and deformation of glasses. The analysis also shows that the characteristic stiffness of quasilocalized nonphononic excitations can be related to their characteristic size, a long sought-for length scale. These results show that important physical information, which is relevant for various key questions in glass physics, can be obtained through pinching a glass.

Simple and Broadly Applicable Definition of Shear Transformation Zones.

Plastic deformation in amorphous solids is known to be carried by stress-induced localized rearrangements of a few tens of particles, accompanied by the conversion of elastic energy to heat. Despite their central role in determining how glasses yield and break, the search for a simple and generally applicable definition of the precursors of those plastic rearrangements-the so-called shear transformation zones (STZs)-is still ongoing. Here we present a simple definition of STZs-based solely on the harmonic approximation of a glass's energy. We explain why and demonstrate directly that our proposed definition of plasticity carriers in amorphous solids is more broadly applicable compared to anharmonic definitions put forward previously. Finally, we offer an open-source library that analyzes low-lying STZs in computer glasses and in laboratory materials such as dense colloidal suspensions for which the harmonic approximation is accessible. Our results constitute a physically motivated methodological advancement towards characterizing mechanical disorder in glasses, and understanding how they yield.

Low-energy quasilocalized excitations in structural glasses.

Glassy solids exhibit a wide variety of generic thermomechanical properties, ranging from universal anomalous specific heat at cryogenic temperatures to nonlinear plastic yielding and failure under external driving forces, which qualitatively differ from their crystalline counterparts. For a long time, it has been believed that many of these properties are intimately related to nonphononic, low-energy quasilocalized excitations (QLEs) in glasses. Indeed, recent computer simulations have conclusively revealed that the self-organization of glasses during vitrification upon cooling from a melt leads to the emergence of such QLEs. In this Perspective, we review developments over the past three decades toward understanding the emergence of QLEs in structural glasses and the degree of universality in their statistical and structural properties. We discuss the challenges and difficulties that hindered progress in achieving these goals and review the frameworks put forward to overcome them. We conclude with an outlook on future research directions and open questions.

Elastic moduli fluctuations predict wave attenuation rates in glasses.

The disorder-induced attenuation of elastic waves is central to the universal low-temperature properties of glasses. Recent literature offers conflicting views on both the scaling of the wave attenuation rate Γ(ω) in the low-frequency limit (ω → 0) and its dependence on glass history and properties. A theoretical framework-termed Fluctuating Elasticity Theory (FET)-predicts low-frequency Rayleigh scattering scaling in -d spatial dimensions, Γ(ω) ∼ γ ω -d+1, where γ = γ(Vc) quantifies the coarse-grained spatial fluctuations of elastic moduli, involving a correlation volume Vc that remains debated. Here, using extensive computer simulations, we show that Γ(ω) ∼ γω3 is asymptotically satisfied in two dimensions ( -d = 2) once γ is interpreted in terms of ensemble-rather than spatial-averages, where Vc is replaced by the system size. In doing so, we also establish that the finite-size ensemble-statistics of elastic moduli is anomalous and related to the universal ω4 density of states of soft quasilocalized modes. These results not only strongly support FET but also constitute a strict benchmark for the statistics produced by coarse-graining approaches to the spatial distribution of elastic moduli.

Does mesoscopic elasticity control viscous slowing down in glassforming liquids?

The dramatic slowing down of relaxation dynamics of liquids approaching the glass transition remains a highly debated problem, where the crux of the puzzle resides in the elusive increase in the activation barrier ΔE(T) with decreasing temperature T. A class of theoretical frameworks-known as elastic models-attribute this temperature dependence to the variations of the liquid's macroscopic elasticity, quantified by the high-frequency shear modulus G∞(T). While elastic models find some support in a number of experimental studies, these models do not take into account the spatial structures, length scales, and heterogeneity associated with structural relaxation in supercooled liquids. Here, we propose and test the possibility that viscous slowing down is controlled by a mesoscopic elastic stiffness κ(T), defined as the characteristic stiffness of response fields to local dipole forces in the liquid's underlying inherent structures. First, we show that κ(T)-which is intimately related to the energy and length scales characterizing quasilocalized, nonphononic excitations in glasses-increases more strongly with decreasing T than the macroscopic inherent structure shear modulus G(T) [the glass counterpart of liquids' G∞(T)] in several computer liquids. Second, we show that the simple relation ΔE(T) ∝ κ(T) holds remarkably well for some computer liquids, suggesting a direct connection between the liquid's underlying mesoscopic elasticity and enthalpic energy barriers. On the other hand, we show that for other computer liquids, the above relation fails. Finally, we provide strong evidence that what distinguishes computer liquids in which the ΔE(T) ∝ κ(T) relation holds from those in which it does not is that the latter feature highly fragmented/granular potential energy landscapes, where many sub-basins separated by low activation barriers exist. Under such conditions, it appears that the sub-basins do not properly represent the landscape properties relevant for structural relaxation.

Universality of the Nonphononic Vibrational Spectrum across Different Classes of Computer Glasses.

It has been recently established that the low-frequency spectrum of simple computer glass models is populated by soft, quasilocalized nonphononic vibrational modes whose frequencies ω follow a gapless, universal distribution D(ω)∼ω^{4}. While this universal nonphononic spectrum has been shown to be robust to varying the glass history and spatial dimension, it has so far only been observed in simple computer glasses featuring radially symmetric, pairwise interaction potentials. Consequently, the relevance of the universality of nonphononic spectra seen in simple computer glasses to realistic laboratory glasses remains unclear. Here, we demonstrate the emergence of the universal ω^{4} nonphononic spectrum in a broad variety of realistic computer glass models, ranging from tetrahedral network glasses with three-body interactions, through molecular glasses and glassy polymers, to bulk metallic glasses. Taken together with previous observations, our results indicate that the low-frequency nonphononic vibrational spectrum of any glassy solid quenched from a melt features the universal ω^{4} law, independently of the nature of its microscopic interactions.

An energy-landscape-based crossover temperature in glass-forming liquids.

The systematic identification of temperature scales in supercooled liquids that are key to understanding those liquids' underlying glass properties, and their formation-history dependence, is a challenging task. Here, we study the statistics of particles' squared displacements δr2 between equilibrium liquid configurations at temperature T and their underlying inherent states, using computer simulations of 11 different computer glass formers. We show that the relative fluctuations of δr2 are nonmonotonic in T, exhibiting a maximum whose location defines the crossover temperature TX. Therefore, TX marks the point of maximal heterogeneity during the process of tumbling down the energy landscape, starting from an equilibrium liquid state at temperature T down to its underlying inherent state. We extract TX for the 11 employed computer glasses, ranging from tetrahedral glasses to packs of soft elastic spheres, and demonstrate its usefulness in putting the elastic properties of different glasses on the same footing. Interestingly, we further show that TX marks the crossover between two distinct regimes of the mean ⟨δr2⟩: a high temperature regime in which ⟨δr2⟩ scales approximately as T0.5 and a deeply supercooled regime in which ⟨δr2⟩ scales approximately as T1.3. Further research directions are discussed.

Statistical mechanics of local force dipole responses in computer glasses.

Soft quasilocalized modes (QLMs) are universally featured by structural glasses quenched from a melt, and are involved in several glassy anomalies such as the low-temperature scaling of their thermal conductivity and specific heat, and sound attenuation at intermediate frequencies. In computer glasses, QLMs may assume the form of harmonic vibrational modes under a narrow set of circumstances; however, direct access to their full distribution over frequency is hindered by hybridizations of QLMs with other low-frequency modes (e.g., phonons). Previous studies to overcome this issue have demonstrated that the response of a glass to local force dipoles serves as a good proxy for its QLMs; we, therefore, study here the statistical-mechanical properties of these responses in computer glasses, over a large range of glass stabilities and in various spatial dimensions, with the goal of revealing properties of the yet-inaccessible full distribution of QLMs' frequencies. We find that as opposed to the spatial-dimension-independent universal distribution of QLMs' frequencies ω (and, consequently, also of their stiffness κ = ω2), the distribution of stiffnesses associated with responses to local force dipoles features a (weak) dependence on spatial dimension. We rationalize this dependence by introducing a lattice model that incorporates both the real-space profiles of QLMs-associated with dimension-dependent long-range elastic fields-and the universal statistical properties of their frequencies. Based on our findings, we propose a conjecture about the form of the full distribution of QLMs' frequencies and its protocol-dependence. Finally, we discuss possible connections of our findings to basic aspects of glass formation and deformation.

Local thermal energy as a structural indicator in glasses.

Identifying heterogeneous structures in glasses-such as localized soft spots-and understanding structure-dynamics relations in these systems remain major scientific challenges. Here, we derive an exact expression for the local thermal energy of interacting particles (the mean local potential energy change caused by thermal fluctuations) in glassy systems by a systematic low-temperature expansion. We show that the local thermal energy can attain anomalously large values, inversely related to the degree of softness of localized structures in a glass, determined by a coupling between internal stresses-an intrinsic signature of glassy frustration-anharmonicity and low-frequency vibrational modes. These anomalously large values follow a fat-tailed distribution, with a universal exponent related to the recently observed universal [Formula: see text] density of states of quasilocalized low-frequency vibrational modes. When the spatial thermal energy field-a "softness field"-is considered, this power law tail manifests itself by highly localized spots, which are significantly softer than their surroundings. These soft spots are shown to be susceptible to plastic rearrangements under external driving forces, having predictive powers that surpass those of the normal modes-based approach. These results offer a general, system/model-independent, physical/observable-based approach to identify structural properties of quiescent glasses and relate them to glassy dynamics.

Rigidity and auxeticity transitions in networks with strong bond-bending interactions.

A widely studied model for gels or biopolymeric fibrous materials are networks with central force interactions, such as Hookean springs. Less commonly studied are materials whose mechanics are dominated by non-central force interactions such as bond-bending potentials. Inspired by recent experimental advancements in designing colloidal gels with tunable interactions, we study the micro- and macroscopic elasticity of two-dimensional planar graphs with strong bond-bending potentials, in addition to weak central forces. We introduce a theoretical framework that allows us to directly investigate the limit in which the ratio of characteristic central-force to bending stiffnesses vanishes. In this limit we show that a generic isostatic point exists at [Formula: see text], coinciding with the isostatic point of frames with central-force interactions in two dimensions. We further demonstrate the emergence of a stiffening transition when the coordination is increased towards the isostatic point, which shares similarities with the strain-induced stiffening transition observed in biopolymeric fibrous materials, and coincides with an auxeticity transition above which the material's Poisson's ratio approaches -1 when bond-bending interactions dominate.

Wave attenuation in glasses: Rayleigh and generalized-Rayleigh scattering scaling.

The attenuation of long-wavelength phonons (waves) by glassy disorder plays a central role in various glass anomalies, yet it is neither fully characterized nor fully understood. Of particular importance is the scaling of the attenuation rate Γ(k) with small wavenumbers k → 0 in the thermodynamic limit of macroscopic glasses. Here, we use a combination of theory and extensive computer simulations to show that the macroscopic low-frequency behavior emerges at intermediate frequencies in finite-size glasses, above a recently identified crossover wavenumber k†, where phonons are no longer quantized into bands. For k < k†, finite-size effects dominate Γ(k), which is quantitatively described by a theory of disordered phonon bands. For k > k†, we find that Γ(k) is affected by the number of quasilocalized nonphononic excitations, a generic signature of glasses that feature a universal density of states. In particular, we show that in a frequency range in which this number is small, Γ(k) follows a Rayleigh scattering scaling ∼k¯d+1 (¯d is the spatial dimension) and that in a frequency range in which this number is sufficiently large, the recently observed generalized-Rayleigh scaling of the form ∼k¯d+1 log(k0/k) emerges (k0 > k† is a characteristic wavenumber). Our results suggest that macroscopic glasses-and, in particular, glasses generated by conventional laboratory quenches that are known to strongly suppress quasilocalized nonphononic excitations-exhibit Rayleigh scaling at the lowest wavenumbers k and a crossover to generalized-Rayleigh scaling at higher k. Some supporting experimental evidence from recent literature is presented.

Universal Nonphononic Density of States in 2D, 3D, and 4D Glasses.

It is now well established that structural glasses possess disorder- and frustration-induced soft quasilocalized excitations, which play key roles in various glassy phenomena. Recent work has established that in model glass formers in three dimensions, these nonphononic soft excitations may assume the form of quasilocalized, harmonic vibrational modes whose frequency follows a universal density of states D(ω)∼ω^{4}, independently of microscopic details, and for a broad range of glass preparation protocols. Here, we further establish the universality of the nonphononic density of vibrational modes by direct measurements in model structural glasses in two dimensions and four dimensions. We also investigate their degree of localization, which is generally weaker in lower spatial dimensions, giving rise to a pronounced system-size dependence of the nonphononic density of states in two dimensions, but not in higher dimensions. Finally, we identify a fundamental glassy frequency scale ω_{c} above which the universal ω^{4} law breaks down.

Quasilocalized states of self stress in packing-derived networks.

States of self stress (SSS) are assignments of forces on the edges of a network that satisfy mechanical equilibrium in the absence of external forces. In this work we show that a particular class of quasilocalized SSS in packing-derived networks, first introduced by D.M. Sussman, C.P. Goodrich, A.J. Liu (Soft Matter 12, 3982 (2016)), are characterized by a decay length that diverges as [Formula: see text] , where [Formula: see text] is the mean connectivity of the network, and [Formula: see text] is the Maxwell threshold in two dimensions, at odds with previous claims. Our results verify the previously proposed analogy between quasilocalized SSS and the mechanical response to a local dipolar force in random networks of relaxed Hookean springs. We show that the normalization factor that distinguishes between quasilocalized SSS and the response to a local dipole constitutes a measure of the mechanical coupling of the forced spring to the elastic network in which it is embedded. We further demonstrate that the lengthscale that characterizes quasilocalized SSS does not depend on its associated degree of mechanical coupling, but instead only on the network connectivity.

A characteristic energy scale in glasses.

Intrinsically generated structural disorder endows glassy materials with a broad distribution of various microscopic quantities-such as relaxation times and activation energies-without an obvious characteristic scale. At the same time, macroscopic glassy responses-such as Newtonian (linear) viscosity and nonlinear plastic deformation-are widely interpreted in terms of a characteristic energy scale, e.g., an effective temperature-dependent activation energy in Arrhenius relations. Nevertheless, despite its fundamental importance, such a characteristic energy scale has not been robustly identified. Inspired by the accumulated evidence regarding the crucial role played by disorder- and frustration-induced soft quasilocalized excitations in determining the properties and dynamics of glasses, we propose that the bulk average of the glass response to a localized force dipole defines such a characteristic energy scale. We show that this characteristic glassy energy scale features remarkable properties: (i) It increases dramatically in underlying inherent structures of equilibrium supercooled states approaching the glass transition temperature Tg, significantly surpassing the corresponding increase in the macroscopic shear modulus, dismissing the common view that structural variations in supercooled liquids upon vitrification are minute. (ii) Its variation with annealing and system size is very similar in magnitude and form to that of the energy of the softest non-phononic vibrational mode, thus establishing a nontrivial relation between a rare glassy fluctuation and a bulk average response. (iii) It exhibits striking dependence on spatial dimensionality and system size due to the long-ranged fields associated with quasilocalization, which are speculated to be related to peculiarities of the glass transition in two dimensions. In addition, we identify a truly static growing lengthscale associated with the characteristic glassy energy scale and discuss possible connections between the increase of this energy scale and the slowing down of dynamics near the glass transition temperature. Open questions and future directions are discussed.