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The Zhang-Torquato conjecture [Phys. Rev. E 101, 032124 (2020)] states that any realizable pair correlation function $g_2({\bf r})$ or structure factor $S({\bf k})$ of a translationally invariant nonequilibrium system can be attained by an equilibrium ensemble involving only (up to) effective two-body interactions. To test this conjecture, we consider two singular nonequilibrium models of recent interest that also have the exotic hyperuniformity property: a 2D "perfect glass" and a 3D critical absorbing-state model. We find that each nonequilibrium target can be achieved accurately by equilibrium states with effective one- and two-body potentials, lending further support to the conjecture. To characterize the structural degeneracy of such nonequilibrium-equilibrium correspondence, we compute higher-order statistics for both models, as well as those for a hyperuniform 3D uniformly randomized lattice (URL), whose higher-order statistics can be very precisely ascertained. Interestingly, we find that the differences in the higher-order statistics between nonequilibrium and equilibrium systems with matching pair statistics, as measured by the "hole" probability distribution, provides measures of the degree to which a system is out of equilibrium. We show that all three systems studied possess the \textit{bounded-hole} property, and that holes near the maximum hole size in the URL are much rarer than those in the underlying simple cubic lattice. Remarkably, upon quenching, the effective potentials for all three systems possess local energy minima with stronger forms of hyperuniformity compared to their target counterparts. Our work is expected to facilitate the self-assembly of tunable hyperuniform soft-matter systems.

A variety of performance demands are being placed on material systems, including desirable mechanical, thermal, electrical, optical, acoustic and flow properties. The purpose of the present article is to review the emerging field of disordered hyperuniform composites and their novel multifunctional characteristics. Disordered hyperuniform media are exotic amorphous states of matter that are characterized by an anomalous suppression of large-scale volume-fraction fluctuations compared to those in "garden-variety" disordered materials. Such unusual composites can have advantages over their periodic counterparts, such as unique or nearly optimal, direction-independent physical properties and robustness against defects. It will be shown that disordered hyperuniform composites and porous media can be endowed with a broad spectrum of extraordinary physical properties, including photonic, phononic, transport, chemical and mechanical characteristics that are only beginning to be discov, 12 figures

Understanding the nature and formation of band gaps associated with the propagation of electromagnetic, electronic, or elastic waves in disordered materials as a function of system size presents fundamental and technological challenges. In particular, a basic question is whether band gaps in disordered systems exist in the thermodynamic limit. To explore this issue, we use a two-stage ensemble approach to study the formation of complete photonic band gaps (PBGs) for a sequence of increasingly large systems spanning a broad range of two-dimensional photonic network solids with varying degrees of local and global order, including hyperuniform and nonhyperuniform types. We discover that the gap in the density of states exhibits exponential tails and the apparent PBGs rapidly close as the system size increases for nearly all disordered networks considered. The only exceptions are sufficiently stealthy hyperuniform cases for which the band gaps remain open and the band tails exhibit a desirable power-law scaling reminiscent of the PBG behavior of photonic crystals in the thermodynamic limit.

An outstanding problem in statistical mechanics is the determination of whether prescribed functional forms of the pair correlation function g2( r) [or equivalently, structure factor S( k)] at some number density ρ can be achieved by many-body systems in d-dimensional Euclidean space. The Zhang–Torquato conjecture states that any realizable set of pair statistics, whether from a nonequilibrium or equilibrium system, can be achieved by equilibrium systems involving up to two-body interactions. To further test this conjecture, we study the realizability problem of the nonequilibrium iso- g2 process, i.e., the determination of density-dependent effective potentials that yield equilibrium states in which g2 remains invariant for a positive range of densities. Using a precise inverse algorithm that determines effective potentials that match hypothesized functional forms of g2( r) for all r and S( k) for all k, we show that the unit-step function g2, which is the zero-density limit of the hard-sphere potential, is remarkably realizable up to the packing fraction ϕ = 0.49 for d = 1. For d = 2 and 3, it is realizable up to the maximum “terminal” packing fraction ϕ c = 1/2 d, at which the systems are hyperuniform, implying that the explicitly known necessary conditions for realizability are sufficient up through ϕ c. For ϕ near but below ϕ c, the large- r behaviors of the effective potentials are given exactly by the functional forms exp[ − κ( ϕ) r] for d = 1, r−1/2 exp[ − κ( ϕ) r] for d = 2, and r−1 exp[ − κ( ϕ) r] (Yukawa form) for d = 3, where κ−1( ϕ) is a screening length, and for ϕ = ϕ c, the potentials at large r are given by the pure Coulomb forms in the respective dimensions as predicted by Torquato and Stillinger [Phys. Rev. E 68, 041113 (2003)]. We also find that the effective potential for the pair statistics of the 3D “ghost” random sequential addition at the maximum packing fraction ϕ c = 1/8 is much shorter ranged than that for the 3D unit-step function g2 at ϕ c; thus, it does not constrain the realizability of the unit-step function g2. Our inverse methodology yields effective potentials for realizable targets, and, as expected, it does not reach convergence for a target that is known to be non-realizable, despite the fact that it satisfies all known explicit necessary conditions. Our findings demonstrate that exploring the iso- g2 process via our inverse methodology is an effective and robust means to tackle the realizability problem and is expected to facilitate the design of novel nanoparticle systems with density-dependent effective potentials, including exotic hyperuniform states of matter.

Much attention has been devoted to water’s metastable phase behavior, including polyamorphism (multiple amorphous solid phases), and the hypothesized liquid-liquid transition and associated critical point. However, the possible relationship between these phenomena remains incompletely understood. Using molecular dynamics simulations of the realistic TIP4P/2005 model, we found a striking signature of the liquid-liquid critical point in the structure of water glasses, manifested as a pronounced increase in long-range density fluctuations at pressures proximate to the critical pressure. By contrast, these signatures were absent in glasses of two model systems that lack a critical point. We also characterized the departure from equilibrium upon vitrification via the non-equilibrium index; water-like systems exhibited a strong pressure dependence in this metric, whereas simple liquids did not. These results reflect a surprising relationship between the metastable equilibrium phenomenon of liquid-liquid criticality and the non-equilibrium structure of glassy water, with implications for our understanding of water phase behavior and glass physics. Our calculations suggest a possible experimental route to probing the existence of the liquid-liquid transition in water and other fluids., The subtle connections between water’s supercooled liquid and glassy states are difficult to characterize. Gartner et al. suggest with MD simulations that the long-range structure of glassy water may reflect signatures of water’s debated second critical point in the supercooled liquid.

The determination of the pair potential v(r) that accurately yields an equilibrium state at positive temperature T with a prescribed pair correlation function g_{2}(r) or corresponding structure factor S(k) in d-dimensional Euclidean space R^{d} is an outstanding inverse statistical mechanics problem with far-reaching implications. Recently, Zhang and Torquato [Phys. Rev. E 101, 032124 (2020)2470-004510.1103/PhysRevE.101.032124] conjectured that any realizable g_{2}(r) or S(k) corresponding to a translationally invariant nonequilibrium system can be attained by a classical equilibrium ensemble involving only (up to) effective pair interactions. Testing this conjecture for nonequilibrium systems as well as for nontrivial equilibrium states requires improved inverse methodologies. We have devised an optimization algorithm to precisely determine effective pair potentials that correspond to pair statistics of general translationally invariant disordered many-body equilibrium or nonequilibrium systems at positive temperatures. This methodology utilizes a parameterized family of pointwise basis functions for the potential function whose initial form is informed by small-, intermediate- and large-distance behaviors dictated by statistical-mechanical theory. Subsequently, a nonlinear optimization technique is utilized to minimize an objective function that incorporates both the target pair correlation function g_{2}(r) and structure factor S(k) so that the small intermediate- and large-distance correlations are very accurately captured. To illustrate the versatility and power of our methodology, we accurately determine the effective pair interactions of the following four diverse target systems: (1) Lennard-Jones system in the vicinity of its critical point, (2) liquid under the Dzugutov potential, (3) nonequilibrium random sequential addition packing, and (4) a nonequilibrium hyperuniform "cloaked" uniformly randomized lattice. We found that the optimized pair potentials generate corresponding pair statistics that accurately match their corresponding targets with total L_{2}-norm errors that are an order of magnitude smaller than that of previous methods. The results of our investigation lend further support to the Zhang-Torquato conjecture. Furthermore, our algorithm will enable one to probe systems with identical pair statistics but different higher-body statistics, which will shed light on the well-known degeneracy problem of statistical mechanics.

The capacity to devise order metrics to characterize and classify microstructures of multiphase heterogeneous media across length scales is an outstanding but highly challenging task, given the richness of the possible geometries and topologies of the phases that can arise. This investigation initiates a program to formulate order metrics to characterize the degree of order/disorder of the microstructures of two-phase media in d -dimensional Euclidean space R d across length scales. In particular, we propose the use of the local volume-fraction variance σ V 2 ( R ) associated with a spherical window of radius R as an order metric. We determine σ V 2 ( R ) as a function of R for 22 different models across the first three space dimensions, including both hyperuniform and nonhyperuniform systems with varying degrees of short- and long-range order. We find that the local volume-fraction variance as well as asymptotic coefficients and integral measures derived from it provide reasonably robust and sensitive order metrics to categorize disordered and ordered two-phase media across all length scales. Such order metrics could be employed to accelerate the discovery of novel heterogeneous materials by tailoring their degree of order/disorder.

The recently developed concept of spreadability, $\mathcal{S}(t)$, provides a direct link between time-dependent diffusive transport and the microstructure of two-phase media across length scales. We explicitly compute $\mathcal{S}(t)$ for well-known two-dimensional and three-dimensional model structures, including nonhyperuniform fully penetrable spheres and equilibrium hard spheres, as well as hyperuniform sphere packings derived from perfect glasses, uniformly randomized lattices (URL), disordered stealthy point processes and Bravais lattices. We further confirm that the small-, intermediate- and long-time behaviors of $\mathcal{S}(t)$ sensitively capture the small-, intermediate- and large-scale characteristics of the models. In instances in which the spectral density $\tilde{\chi}_{_V}(\mathbf{k})$ has a power-law form $B|\mathbf{k}|^\alpha$ in the limit $|\mathbf{k}|\rightarrow 0$, the long-time spreadability provides a simple means to extract the value of the coefficients $\alpha$ and $B$ that is robust against noise in $\tilde{\chi}_{_V}(\mathbf{k})$ at small wavenumbers. Interestingly, the excess spreadability $\mathcal{S}(\infty)-\mathcal{S}(t)$ for URL packings has nearly exponential decay at small to intermediate $t$, but transforms to a power-law decay at large $t$. Our study of the aforementioned models enables us to devise an algorithm that accurately extracts large-scale behaviors from diffusion data alone. Lessons learned from such analyses of our models are used to determine accurately the large-scale structural characteristics of a sample Fontainebleau sandstone, which we show is nonhyperuniform. Our study demonstrates the practical applicability of the diffusion spreadability to extract crucial microstructural information from real data across length scales and provides a basis for the inverse design of materials with desirable time-dependent diffusion properties., Comment: 21 pages, 11 figures

Dense, disordered packings of particles are useful models of low-temperature amorphous phases of matter, biological systems, granular media, and colloidal systems. The study of dense packings of nonspherical particles enables one to ascertain how rotational degrees of freedom affect packing behavior. Here, we study superballs, a large family of deformations of the sphere, defined in three dimensions by $|x_1|^{2p}+|x_2|^{2p}+|x_3|^{2p}\leq1$, where $p>0$ is a deformation parameter indicating to what extent the shape deviates from a sphere. As $p$ increases from the sphere point ($p=1$), the superball attains cubic symmetry, and attains octahedral symmetry when $p, Comment: 16 Pages, 17 Figures. SI: 4 Pages, 6 Figures

It is well known that the degeneracy of two-phase microstructures with the same volume fraction and two-point correlation function S_{2}(r) is generally infinite. To elucidate the degeneracy problem explicitly, we examine Debye random media, which are entirely defined by a purely exponentially decaying two-point correlation function S_{2}(r). In this work, we consider three different classes of Debye random media. First, we generate the "most probable" class using the Yeong-Torquato construction algorithm [Yeong and Torquato, Phys. Rev. E 57, 495 (1998)1063-651X10.1103/PhysRevE.57.495]. A second class of Debye random media is obtained by demonstrating that the corresponding two-point correlation functions are effectively realized in the first three space dimensions by certain models of overlapping, polydisperse spheres. A third class is obtained by using the Yeong-Torquato algorithm to construct Debye random media that are constrained to have an unusual prescribed pore-size probability density function. We structurally discriminate these three classes of Debye random media from one another by ascertaining their other statistical descriptors, including the pore-size, surface correlation, chord-length probability density, and lineal-path functions. We also compare and contrast the percolation thresholds as well as the diffusion and fluid transport properties of these degenerate Debye random media. We find that these three classes of Debye random media are generally distinguished by the aforementioned descriptors, and their microstructures are also visually distinct from one another. Our work further confirms the well-known fact that scattering information is insufficient to determine the effective physical properties of two-phase media. Additionally, our findings demonstrate the importance of the other two-point descriptors considered here in the design of materials with a spectrum of physical properties.

Consider the time-dependent problem of mass transfer of a solute between two phases and assume that the solute is initially distributed in one phase (phase 2) and absent from the other (phase 1). We desire the fraction of total solute present in phase 1 as a function of time, ${\cal S}(t)$, which we call the {\it spreadability}, since it is a measure of the spreadability of diffusion information as a function of time. We derive exact direct-space formulas for ${\cal S}(t)$ in any Euclidean space dimension $d$ in terms of the autocovariance function as well as corresponding Fourier representations of ${\cal S}(t)$ in terms of the spectral density. We derive closed-form general formulas for the short- and long-time behaviors of the spreadability in terms of crucial small- and large-scale microstructural information, respectively. The long-time behavior of ${\cal S}(t)$ enables one to distinguish the entire spectrum of microstructures that span from hyperuniform to nonhyperuniform media. For hyperuniform media, disordered or not, we show that the "excess" spreadability, ${\cal S}(\infty)-{\cal S}(t)$, decays to its long-time behavior exponentially faster than that of any nonhyperuniform two-phase medium, the "slowest" being antihyperuniform media. The stealthy hyperuniform class is characterized by an excess spreadability with the fastest decay rate among all translationally invariant microstructures. Moreover, we establish a remarkable connection between the spreadability and an outstanding problem in discrete geometry, namely, microstructures with "fast" spreadabilities are also those that can be derived from efficient "coverings" of space. We also identify heretofore unnoticed remarkable links between the spreadability ${\cal S}(t)$ and NMR pulsed field gradient spin-echo amplitude as well as diffusion MRI measurements., 18 pages, 10 figures

Through an extensive series of high-precision numerical computations of the optimal complete photonic band gap (PBG) as a function of dielectric contrast $\alpha$ for a variety of crystal and disordered heterostructures, we reveal striking universal behaviors of the gap sensitivity $\mathcal{S}(\alpha)\equiv d\Delta(\alpha)/d\alpha$, the first derivative of the optimal gap-to-midgap ratio $\Delta(\alpha)$. In particular, for all our crystal networks, $\mathcal{S}(\alpha)$ takes a universal form that is well approximated by the analytic formula for a one-dimensional quarter-wave stack, $\mathcal{S}_{\text{QWS}}(\alpha)$. Even more surprisingly, the values of $\mathcal{S}(\alpha)$ for our disordered networks converge to $\mathcal{S}_{\text{QWS}}(\alpha)$ for sufficiently large $\alpha$. A deeper understanding of the simplicity of this universal behavior may provide fundamental insights about PBG formation and guidance in the design of novel photonic heterostructures., Comment: Main article: 6 pages, 3 figures; supplemental material: 8 pages, 4 figures

We consider the scaling properties characterizing the hyperuniformity (or anti-hyperuniformity) of long wavelength fluctuations in a broad class of one-dimensional substitution tilings. We present a simple argument that predicts the exponent $\alpha$ governing the scaling of Fourier intensities at small wavenumbers, tilings with $\alpha>0$ being hyperuniform, and confirm with numerical computations that the predictions are accurate for quasiperiodic tilings, tilings with singular continuous spectra, and limit-periodic tilings. Tilings with quasiperiodic or singular continuous spectra can be constructed with $\alpha$ arbitrarily close to any given value between $-1$ and $3$. Limit-periodic tilings can be constructed with $\alpha$ between $-1$ and $1$ or with Fourier intensities that approach zero faster than any power law., Comment: 13 pages, 9 figures, to be submitted to Acta Crystallographica special issue: Aperiodic 2018

The study of hyperuniform states of matter is an emerging multidisciplinary field, influencing and linking developments across the physical sciences, mathematics, and biology (1, 2). A hyperuniform many-particle system in d-dimensional Euclidean space is characterized by an anomalous suppression of large-scale density fluctuations relative to those in typical disordered systems, such as liquids and amorphous solids. As such, the hyperuniformity concept generalizes the traditional notion of long-range order to include not only all perfect crystals and quasicrystals but also exotic disordered states of matter. Disordered hyperuniform states have attracted great attention across many fields over the last two decades because they can have the character of crystals on large length scales but are isotropic like liquids (2). This hybrid crystal–liquid attribute endows them with unique or nearly optimal, direction-independent physical properties and robustness against defects (3⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓–14). Adding to this flurry of research activity is the finding by Huang et al. (15) that circularly swimming marine algae can robustly self-organize into disordered hyperuniform states through long-range hydrodynamic interactions at air–liquid interfaces. How is hyperuniformity quantified? Such systems have a structure factor S ( k ) , which can be measured from scattering experiments, that tends to zero as the wavenumber | k | tends to zero (1), where k is the wavevector. Another way to ascertain hyperuniformity is to randomly place many large spherical sampling windows of radius R in the system and count the number of particles within the window. The number of particles registered within the window will fluctuate, enabling one to find the corresponding local number variance σ 2 ( R ) , as shown in Fig. 1. Garden-variety disordered systems, such as typical gases and liquids, are characterized by a variance σ 2 ( R ) … [↵][1]1Email: torquato{at}princeton.edu. [1]: #xref-corresp-1-1

We explore quantitative descriptors that herald when a many-particle system in $d$-dimensional Euclidean space $\mathbb{R}^d$ approaches a hyperuniform state as a function of the relevant control parameter. We establish quantitative criteria to ascertain the extent of hyperuniform and nonhyperuniform distance-scaling regimes n terms of the ratio $B/A$, where $A$ is "volume" coefficient and $B$ is "surface-area" coefficient associated with the local number variance $\sigma^2(R)$ for a spherical window of radius $R$. To complement the known direct-space representation of the coefficient $B$ in terms of the total correlation function $h({\bf r})$, we derive its corresponding Fourier representation in terms of the structure factor $S({\bf k})$, which is especially useful when scattering information is available experimentally or theoretically. We show that the free-volume theory of the pressure of equilibrium packings of identical hard spheres that approach a strictly jammed state either along the stable crystal or metastable disordered branch dictates that such end states be exactly hyperuniform. Using the ratio $B/A$, the hyperuniformity index $H$ and the direct-correlation function length scale $\xi_c$, we study three different exactly solvable models as a function of the relevant control parameter, either density or temperature, with end states that are perfectly hyperuniform. We analyze equilibrium hard rods and "sticky" hard-sphere systems in arbitrary space dimension $d$ as a function of density. We also examine low-temperature excited states of many-particle systems interacting with "stealthy" long-ranged pair interactions as the temperature tends to zero. The capacity to identify hyperuniform scaling regimes should be particularly useful in analyzing experimentally- or computationally-generated samples that are necessarily of finite size., Comment: 19 pages, 14 figures

Transport properties of porous media are intimately linked to their pore-space microstructures. We quantify geometrical and topological descriptors of the pore space of certain disordered and ordered distributions of spheres, including pore-size functions and the critical pore radius ${\ensuremath{\delta}}_{c}$. We focus on models of porous media derived from maximally random jammed sphere packings, overlapping spheres, equilibrium hard spheres, quantizer sphere packings, and crystalline sphere packings. For precise estimates of the percolation thresholds, we use a strict relation of the void percolation around sphere configurations to weighted bond percolation on the corresponding Voronoi networks. We use the Newman-Ziff algorithm to determine the percolation threshold using universal properties of the cluster size distribution. The critical pore radius ${\ensuremath{\delta}}_{c}$ is often used as the key characteristic length scale that determines the fluid permeability $k$. A recent study [Torquato, Adv. Wat. Resour. 140, 103565 (2020)] suggested for porous media with a well-connected pore space an alternative estimate of $k$ based on the second moment of the pore size $\ensuremath{\langle}{\ensuremath{\delta}}^{2}\ensuremath{\rangle}$, which is easier to determine than ${\ensuremath{\delta}}_{c}$. Here, we compare ${\ensuremath{\delta}}_{c}$ to the second moment of the pore size $\ensuremath{\langle}{\ensuremath{\delta}}^{2}\ensuremath{\rangle}$, and indeed confirm that, for all porosities and all models considered, ${\ensuremath{\delta}}_{c}^{2}$ is to a good approximation proportional to $\ensuremath{\langle}{\ensuremath{\delta}}^{2}\ensuremath{\rangle}$. However, unlike $\ensuremath{\langle}{\ensuremath{\delta}}^{2}\ensuremath{\rangle}$, the permeability estimate based on ${\ensuremath{\delta}}_{c}^{2}$ does not predict the correct ranking of $k$ for our models. Thus, we confirm $\ensuremath{\langle}{\ensuremath{\delta}}^{2}\ensuremath{\rangle}$ to be a promising candidate for convenient and reliable estimates of the fluid permeability for porous media with a well-connected pore space. Moreover, we compare the fluid permeability of our models with varying degrees of order, as measured by the $\ensuremath{\tau}$ order metric. We find that (effectively) hyperuniform models tend to have lower values of $k$ than their nonhyperuniform counterparts. Our findings could facilitate the design of porous media with desirable transport properties via targeted pore statistics.

The study of hard-particle packings is of fundamental importance in physics, chemistry, cell biology, and discrete geometry. Much of the previous work on hard-particle packings concerns their densest possible arrangements. By contrast, we examine kinetic effects inevitably present in both numerical and experimental packing protocols. Specifically, we determine how changing the compression/shear rate of a two-dimensional packing of noncircular particles causes it to deviate from its densest possible configuration, which is always periodic. The adaptive shrinking cell (ASC) optimization scheme maximizes the packing fraction of a hard-particle packing by first applying random translations and rotations to the particles and then isotropically compressing and shearing the simulation box repeatedly until a possibly jammed state is reached. We use a stochastic implementation of the ASC optimization scheme to mimic different effective time scales by varying the number of particle moves between compressions/shears. We generate dense, effectively jammed, monodisperse, two-dimensional packings of obtuse scalene triangle, rhombus, curved triangle, lens, and "ice cream cone" (a semicircle grafted onto an isosceles triangle) shaped particles, with a wide range of packing fractions and degrees of order. To quantify these kinetic effects, we introduce the kinetic frustration index $K$, which measures the deviation of a packing from its maximum possible packing fraction. To investigate how kinetics affect short- and long-range ordering in these packings, we compute their spectral densities and characterize their contact networks. We find that kinetic effects are most significant when the particles have greater asphericity, less curvature, and less rotational symmetry. This work may be relevant to the design of laboratory packing protocols., 25 pages, 18 figures

We derive exact expressions for effective elastodynamic properties of two-phase composites in the long-wavelength (quasistatic) regime via homogenized constitutive relations that are local in space. This is accomplished by extending the "strong-contrast" expansion formalism that was previously applied to the static problem. These strong-contrast expansions explicitly incorporate complete microstructural information of the composite via an infinite set of $n$-point correlation functions. Utilizing the rapid-convergence properties of these series expansions (even for extreme contrast ratios), we extract accurate approximations that depend on the microstructure via the spectral density, which is easy to compute or measure for any composite. We also investigate the predictive power of modifications of such approximation formulas postulated elsewhere [J. Kim and S. Torquato, Proc. Nat. Acad. Sci. ${\bf 117}$, 8764 (2020)] to extend their applicability ${\it beyond ~the ~quasistatic ~regime.}$ The accuracy of these nonlocal microstructure-dependent approximations is validated by comparison to full-waveform simulation results for certain models of dispersions. We apply our formulas to a variety of models of nonhyperuniform and hyperuniform disordered composites. We demonstrate that hyperuniform systems are less lossy than their nonhyperuniform counterparts in the quasistatic regime, and stealthy hyperuniform media can be perfectly transparent for a wide range of wavenumber. Finally, we discuss how to utilize our approximations for engineering composites with prescribed elastic wave characteristics., 30 pages, 7 figures, 1 Supplementary Material. arXiv admin note: text overlap with arXiv:2007.00701

Hyperuniform states of matter are characterized by anomalous suppression of long-wavelength density fluctuations. While most of interesting cases of disordered hyperuniformity are provided by complex many-body systems like liquids or amorphous solids, classical spin chains with certain long-range interactions have been shown to demonstrate the same phenomenon. It is well-known that the transverse field Ising model shows a quantum phase transition (QPT) at zero temperature. Under the quantum effects of a transverse magnetic field, classical hyperuniform spin chains are expected to lose their hyperuniformity. High-precision simulations of these cases are complicated because of the presence of highly nontrivial long-range interactions. We perform extensive analysis of these systems using density matrix renormalization group to study the possibilities of phase transitions and the mechanism by which they lose hyperuniformity. We discover first-order QPTs in the hyperuniform spin chains. An interesting feature of the phase transitions in these disordered hyperuniform spin chains is that, depending on the parameter values, the presence of transverse magnetic field may remarkably lead to increase in the order of the ground state as measured by the "$\tau$ order metric," even if hyperuniformity is lost. Therefore, it would be possible to design materials to target specific novel quantum behaviors in the presence of a transverse magnetic field. Our numerical investigations suggest that these spin chains can show no more than two QPTs. We further analyze the long-range interacting spin chains via the Jordan-Wigner mapping, showing that under the pairwise interacting approximation and a mean-field treatment, there can be at most two QPTs. Based on these numerical and theoretical explorations, we conjecture that these spin chains can show a maximum of two QPTs at zero temperature., Comment: SM was missing in the previous version. Added here

The local number variance associated with a spherical sampling window of radius $R$ enables a classification of many-particle systems in $d$-dimensional Euclidean space according to the degree to which large-scale density fluctuations are suppressed, resulting in a demarcation between hyperuniform and nonhyperuniform phyla. To better characterize density fluctuations, we carry out an extensive study of higher-order moments, including the skewness $\gamma_1(R)$, excess kurtosis $\gamma_2(R)$ and the corresponding probability distribution function $P[N(R)]$ of a large family of models across the first three space dimensions, including both hyperuniform and nonhyperuniform models. Specifically, we derive explicit integral expressions for $\gamma_1(R)$ and $\gamma_2(R)$ involving up to three- and four-body correlation functions, respectively. We also derive rigorous bounds on $\gamma_1(R)$, $\gamma_2(R)$ and $P[N(R)]$. High-quality simulation data for these quantities are generated for each model. We also ascertain the proximity of $P[N(R)]$ to the normal distribution via a novel Gaussian distance metric $l_2(R)$. Among all models, the convergence to a central limit theorem (CLT) is generally fastest for the disordered hyperuniform processes. The convergence to a CLT is slower for standard nonhyperuniform models, and slowest for the antihyperuniform model studied here. We prove that one-dimensional hyperuniform systems of class I or any $d$-dimensional lattice cannot obey a CLT. Remarkably, we discovered that the gamma distribution provides a good approximation to $P[N(R)]$ for all models that obey a CLT, enabling us to estimate the large-$R$ scalings of $\gamma_1(R)$, $\gamma_2(R)$ and $l_2(R)$. For any $d$-dimensional model that "decorrelates" or "correlates" with $d$, we elucidate why $P[N(R)]$ increasingly moves toward or away from Gaussian-like behavior, respectively., Comment: 23 pages, 8 figures

In their seminal paper on scattering by an inhomogeneous solid, Debye and coworkers proposed a simple exponentially decaying function for the two-point correlation function of an idealized class of two-phase random media. Such {\it Debye random media}, which have been shown to be realizable, are singularly distinct from all other models of two-phase media in that they are entirely defined by their one- and two-point correlation functions. To our knowledge, there has been no determination of other microstructural descriptors of Debye random media. In this paper, we generate Debye random media in two dimensions using an accelerated Yeong-Torquato construction algorithm. We then ascertain microstructural descriptors of the constructed media, including their surface correlation functions, pore-size distributions, lineal-path function, and chord-length probability density function. Accurate semi-analytic and empirical formulas for these descriptors are devised. We compare our results for Debye random media to those of other popular models (overlapping disks and equilibrium hard disks), and find that the former model possesses a wider spectrum of hole sizes, including a substantial fraction of large holes. Our algorithm can be applied to generate other models defined by their two-point correlation functions, and their other microstructural descriptors can be determined and analyzed by the procedures laid out here.

Quantitative structure–property relationships are crucial for the understanding and prediction of the physical properties of complex materials. For fluid flow in porous materials, characterizing the geometry of the pore microstructure facilitates prediction of permeability, a key property that has been extensively studied in material science, geophysics and chemical engineering. In this work, we study the predictability of different structural descriptors via both linear regressions and neural networks. A large data set of 30,000 virtual, porous microstructures of different types, including both granular and continuous solid phases, is created for this end. We compute permeabilities of these structures using the lattice Boltzmann method, and characterize the pore space geometry using one-point correlation functions (porosity, specific surface), two-point surface-surface, surface-void, and void-void correlation functions, as well as the geodesic tortuosity as an implicit descriptor. Then, we study the prediction of the permeability using different combinations of these descriptors. We obtain significant improvements of performance when compared to a Kozeny-Carman regression with only lowest-order descriptors (porosity and specific surface). We find that combining all three two-point correlation functions and tortuosity provides the best prediction of permeability, with the void-void correlation function being the most informative individual descriptor. Moreover, the combination of porosity, specific surface, and geodesic tortuosity provides very good predictive performance. This shows that higher-order correlation functions are extremely useful for forming a general model for predicting physical properties of complex materials. Additionally, our results suggest that artificial neural networks are superior to the more conventional regression methods for establishing quantitative structure–property relationships. We make the data and code used publicly available to facilitate further development of permeability prediction methods.

Disordered stealthy many-particle systems in $\mathbb{R}^d$ are exotic states of matter that suppress single scattering events for a finite range of wavenumbers around the origin in reciprocal space. We derive analytical formulas for the nearest-neighbor functions of disordered stealthy systems. First, we analyze asymptotic small-$r$ approximations and bounding expressions of the nearest-neighbor functions based on the pseudo-hard-sphere ansatz. We then determine how many of the standard $n$-point correlation functions are needed to determine the nearest neighbor functions, and find that a finite number suffice. Via theoretical and computational methods, we compare the large-$r$ behavior of these functions for disordered stealthy systems to those belonging to crystalline lattices. Such ordered and disordered stealthy systems have bounded hole sizes. However, we find that the approach to the critical-hole size can be quantitatively different. We argue that the probability of finding a hole close to the critical-hole size should decrease as a power law with an exponent only dependent on the space dimension $d$ for ordered systems, but that this probability decays asymptotically faster for disordered systems. This implies that holes close to the critical-hole size are rarer in disordered systems. The rarity of observing large holes in disordered systems creates substantial numerical difficulties in sampling the nearest neighbor distributions near the critical-hole size. This motivates both the need for new computational methods for efficient sampling and the development of novel theoretical methods. We also devise a simple analytical formula that accurately describes these systems in the underconstrained regime for all $r$. These results provide a foundation for the analytical description of the nearest-neighbor functions of stealthy systems in the disordered, underconstrained regime., 41 pages, 17 figures

4 pags., 4 figs., The creation of disordered hyperuniform materials with extraordinary optical properties (e.g., large complete photonic band gaps) requires a capacity to synthesize large samples that are effectively hyperuniform down to the nanoscale. Motivated by this challenge, we propose a feasible equilibrium fabrication protocol using binary paramagnetic colloidal particles confined in a 2D plane. The strong and long-ranged dipolar interaction induced by a tunable magnetic field is free from screening effects that attenuate long-ranged electrostatic interactions in charged colloidal systems. Specifically, we numerically find a family of optimal size ratios that makes the two-phase system effectively hyperuniform. We show that hyperuniformity is a general consequence of low isothermal compressibilities, which makes our protocol suitable to treat more general systems with other long-ranged interactions, dimensionalities, and/or polydispersity. Our methodology paves the way to synthesize large photonic hyperuniform materials that function in the visible to infrared range and hence may accelerate the discovery of novel photonic materials., Z. M. and S. T. acknowledge the support of the National Science Foundation under Grant No. DMR-1714722. E. L. acknowledges the support from the Agencia Estatal de Investigacin and Fondo Europeo de Desarrollo Regional (FEDER) under Grant No. FIS2017-89361-C3-2-P and from European Unions Horizon 2020 Research and Innovation Staff Exchange programme under the Marie Skodowska-Curie Grant Agreement No. 734276.

Random, uncorrelated displacements of particles on a lattice preserve the hyperuniformity of the original lattice, that is, normalized density fluctuations vanish in the limit of infinite wavelengths. In addition to a diffuse contribution, the scattering intensity from the the resulting point pattern typically inherits the Bragg peaks (long-range order) of the original lattice. Here we demonstrate how these Bragg peaks can be hidden in the effective diffraction pattern of independent and identically distributed perturbations. All Bragg peaks vanish if and only if the sum of all probability densities of the positions of the shifted lattice points is a constant at all positions. The underlying long-range order is then 'cloaked' in the sense that it cannot be reconstructed from the pair correlation function alone. On the one hand, density fluctuations increase monotonically with the strength of perturbations $a$, as measured by the hyperuniformity order metric $\overline{\Lambda}$. On the other hand, the disappearance and reemergence of long-range order, depending on whether the system is cloaked or not as the perturbation strength increases, is manifestly captured by the $\tau$ order metric. Therefore, while the perturbation strength $a$ may seem to be a natural choice for an order metric of perturbed lattices, the $\tau$ order metric is a superior choice. It is noteworthy that cloaked perturbed lattices allow one to easily simulate very large samples (with at least $10^6$ particles) of disordered hyperuniform point patterns without Bragg peaks., Comment: 10 pages, 9 figures

The capacity to identify realizable many-body configurations associated with targeted functional forms for the pair correlation function ${g}_{2}(r)$ or its corresponding structure factor $S(k)$ is of great fundamental and practical importance. While there are obvious necessary conditions that a prescribed structure factor at number density $\ensuremath{\rho}$ must satisfy to be configurationally realizable, sufficient conditions are generally not known due to the infinite degeneracy of configurations with different higher-order correlation functions. A major aim of this paper is to expand our theoretical knowledge of the class of pair correlation functions or structure factors that are realizable by classical disordered ensembles of particle configurations, including exotic ``hyperuniform'' varieties. We first introduce a theoretical formalism that provides a means to draw classical particle configurations from canonical ensembles with certain pairwise-additive potentials that could correspond to targeted analytical functional forms for the structure factor. This formulation enables us to devise an improved algorithm to construct systematically canonical-ensemble particle configurations with such targeted pair statistics, whenever realizable. As a proof of concept, we test the algorithm by targeting several different structure factors across dimensions that are known to be realizable and one hyperuniform target that is known to be nontrivially unrealizable. Our algorithm succeeds for all realizable targets and appropriately fails for the unrealizable target, demonstrating the accuracy and power of the method to numerically investigate the realizability problem. Subsequently, we also target several families of structure-factor functions that meet the known necessary realizability conditions but are not known to be realizable by disordered hyperuniform point configurations, including $d$-dimensional Gaussian structure factors, $d$-dimensional generalizations of the two-dimensional one-component plasma (OCP), and the $d$-dimensional Fourier duals of the previous OCP cases. Moreover, we also explore unusual nonhyperuniform targets, including ``hyposurficial'' and ``antihyperuniform'' examples. In all of these instances, the targeted structure factors are achieved with high accuracy, suggesting that they are indeed realizable by equilibrium configurations with pairwise interactions at positive temperatures. Remarkably, we also show that the structure factor of nonequilibrium perfect glass, specified by two-, three-, and four-body interactions, can also be realized by equilibrium pair interactions at positive temperatures. Our findings lead us to the conjecture that any realizable structure factor corresponding to either a translationally invariant equilibrium or nonequilibrium system can be attained by an equilibrium ensemble involving only effective pair interactions. Our investigation not only broadens our knowledge of analytical functional forms for ${g}_{2}(\mathbf{r})$ and $S(\mathbf{k})$ associated with disordered point configurations across dimensions but also deepens our understanding of many-body physics. Moreover, our work can be applied to the design of materials with desirable physical properties that can be tuned by their pair statistics.

We derive exact nonlocal expressions for the effective dielectric constant tensor ${\boldsymbol \varepsilon}_e({\bf k}_I, \omega)$ of disordered two-phase composites and metamaterials from first principles. This formalism extends the long-wavelength limitations of conventional homogenization estimates of ${\boldsymbol \varepsilon}_e({\bf k}_I, \omega)$ for arbitrary microstructures so that it can capture spatial dispersion well beyond the quasistatic regime (where $\omega$ and ${\bf k}_I$ are frequency and wavevector of the incident radiation). This is done by deriving nonlocal strong-contrast expansions that exactly account for multiple scattering for the range of wavenumbers for which our extended homogenization theory applies, i.e., $0 \le |{\bf k}_I| \ell \lesssim 1$ (where $\ell$ is a characteristic heterogeneity length scale). Due to the fast-convergence properties of such expansions, their lower-order truncations yield accurate closed-form approximate formulas for ${\varepsilon}_e({\bf k}_I,\omega)$ that incorporate microstructural information via the spectral density, which is easy to compute for any composite. The accuracy of these microstructure-dependent approximations is validated by comparison to full-waveform simulation methods for both 2D and 3D ordered and disordered models of composite media. Thus, our closed-form formulas enable one to predict accurately and efficiently the effective wave characteristics well beyond the quasistatic regime without having to perform full-blown simulations. Among other results, we show that certain disordered hyperuniform particulate composites exhibit novel wave characteristics. Our results demonstrate that one can design the effective wave characteristics of a disordered composite by engineering the microstructure to possess tailored spatial correlations at prescribed length scales., Comment: 26 pages, 13 figures (revised after the review process)

11 pags., 9 figs., 2 apps., Birds are known for their extremely acute sense of vision. The very peculiar structural distribution of five different types of cones in the retina underlies this exquisite ability to sample light. It was recently found that each cone population as well as their total population display a disordered pattern in which long-wavelength density fluctuations vanish [Jiao et al., Phys. Rev. E 89, 022721 (2014)PLEEE81539-375510.1103/PhysRevE.89.022721]. This property, known as hyperuniformity, is also present in perfect crystals. In situations like the avian retina in which both the global structure and that of each component display hyperuniformity, the system is said to be multihyperuniform. In this work, we aim at devising a minimal statistical-mechanical model that can reproduce the main features of the spatial distribution of photoreceptors in avian retina, namely the presence of disorder, multihyperuniformity, and local heterocoordination. This last feature is key to avoiding local clustering of the same type of photoreceptors, an undesirable feature for the efficient sampling of light. For this purpose, we formulate a minimal statistical-mechanical model that definitively exhibits the required structural properties: an equimolar three-component mixture (one component to sample each primary color: red, green, and blue) of nonadditive hard disks to which a long-range logarithmic repulsion is added between like particles. Interestingly, a Voronoi analysis of our idealized system of photoreceptors shows that the space-filling Voronoi polygons display a rather uniform area distribution, symmetrically centered around that of a regular lattice, a structural property also found in human retina. Disordered multihyperuniformity offers an alternative to generate photoreceptor patterns with minimal long-range concentration and density fluctuations. This is the key to overcoming the difficulties in devising an efficient visual system in which crystal-like order is absent., E.L. acknowledges the support from the Agencia Estatal de Investigación and Fondo Europeo de Desarrollo Regional (FEDER) under Grant No. FIS2017-89361-C3-2-P. E.L. and L.G. were also supported by the European Union’s Horizon 2020 Research and Innovation Staff Exchange programme under the Marie Skłodowska-Curie grant agreement No. 734276. S.T. was supported by the National Science Foundation under Award No. DMR-1714722.