Hidden Hyperuniformity in Soft Polymeric Materials

Chremos, Alexandros; Douglas, Jack F.

doi:10.1103/physrevlett.121.258002

Cited by 50 publications

(48 citation statements)

References 53 publications

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“…118003 The behavior of long-wavelength density fluctuations and their anomalous suppression-hyperuniformity [1,2]have been the subject of recent interest in the study of disordered systems for they provide an avenue to probe long-range order in problems that do not possess translational or bond-orientational symmetry [3][4][5][6][7][8][9]. At the same time, hyperuniformity is also emergent in a diverse variety of naturally occurring or model systems that range from granular or colloidal materials [4,5,[10][11][12][13] to soft biological tissues [14][15][16]. This has led to speculations on its universality [3,6] and the need for greater understanding of its causal role in the organization and structure of complex systems.…”

Section: Hidden Order Beyond Hyperuniformity In Critical Absorbing Statesmentioning

confidence: 99%

Hidden Order Beyond Hyperuniformity in Critical Absorbing States

Zheng

Parmar²,

Ciamarra³

2021

Phys. Rev. Lett.

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Section: Hidden Order Beyond Hyperuniformity In Critical Absorbing Statesmentioning

confidence: 99%

Hidden Order Beyond Hyperuniformity in Critical Absorbing States

Zheng

Parmar²,

Ciamarra³

2021

Phys. Rev. Lett.

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“…The segmental packing for polymer melts result in values of S(0) that are small in comparison to hard particles, but the core particles and, by extension of the above discussion, the polymer center of mass, exhibit anomalous small density fluctuations, a feature known as “hyperuniformity” [71,72]. This large suppression of density fluctuations in these floppy molecules is associated with the localization of the core particle within the polymeric structure and renders branched polymers as candidates for hyperuniform materials [70,73]. These results illustrate the importance of understanding molecular packing in material properties.…”

Section: Resultsmentioning

confidence: 99%

“…Total static structure factor S(q) (continuous line) and partial structure factor of star polymer melts. The relation between the S(0)=ρ0.166667emkBT0.166667emκT for S(q) and a schematic of the packing for star polymers are also shown, Reproduced with permission from [73]. Copyright American Physical Society, 2018.…”

Section: Figurementioning

confidence: 99%

Influence of Branching on the Configurational and Dynamical Properties of Entangled Polymer Melts

Chremos

Douglas

2019

Polymers

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We probe the influence of branching on the configurational, packing, and density correlation function properties of polymer melts of linear and star polymers, with emphasis on molecular masses larger than the entanglement molecular mass of linear chains. In particular, we calculate the conformational properties of these polymers, such as the hydrodynamic radius R h , packing length p, pair correlation function g ( r ) , and polymer center of mass self-diffusion coefficient, D, with the use of coarse-grained molecular dynamics simulations. Our simulation results reproduce the phenomenology of simulated linear and branched polymers, and we attempt to understand our observations based on a combination of hydrodynamic and thermodynamic modeling. We introduce a model of “entanglement” phenomenon in high molecular mass polymers that assumes polymers can viewed in a coarse-grained sense as “soft” particles and, correspondingly, we model the emergence of heterogeneous dynamics in polymeric glass-forming liquids to occur in a fashion similar to glass-forming liquids in which the molecules have soft repulsive interactions. Based on this novel perspective of polymer melt dynamics, we propose a functional form for D that can describe our simulation results for both star and linear polymers, covering both the unentangled to entangled polymer melt regimes.

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“…Such hyperuniform states encompass all perfect crystals, many quasicrystals, as well as some exotic disordered systems. Disordered hyperuniform states of matter have been the subject of intense interest across a variety of fields, including physics [4][5][6][7][8][9][10][11][12][13], materials science [14][15][16][17][18][19][20], chemistry [21][22][23], biology [24][25][26][27], and mathematics [28][29][30]. The notion of hyperuniformity was first defined in the context of point-particle systems [2] and then extended to two-phase heterogeneous systems [1] and random scalar/vector fields [31].…”

Section: Introductionmentioning

confidence: 99%

Methodology to construct large realizations of perfectly hyperuniform disordered packings

Kim

Torquato

2019

Phys. Rev. E

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Disordered hyperuniform packings (or dispersions) are unusual amorphous two-phase materials that are endowed with exotic physical properties. Such hyperuniform systems are characterized by an anomalous suppression of volume-fraction fluctuations at infinitely long-wavelengths, compared to ordinary disordered materials. While there has been growing interest in such singular states of amorphous matter, a major obstacle has been an inability to produce large samples that are perfectly hyperuniform due to practical limitations of conventional numerical and experimental methods. To overcome these limitations, we introduce a general theoretical methodology to construct perfectly hyperuniform packings in d-dimensional Euclidean space R d . Specifically, beginning with an initial general tessellation of space by disjoint cells that meets a "bounded-cell" condition, hard particles are placed inside each cell such that the local-cell particle packing fractions are identical to the global packing fraction. We prove that the constructed packings with a polydispersity in size in R d are perfectly hyperuniform in the infinite-sample-size limit and the hyperuniformity of such packings is independent of particle shapes, positions, and numbers per cell. We use this theoretical formulation to devise an efficient and tunable algorithm to generate extremely large realizations of such packings. We employ two distinct initial tessellations: Voronoi as well as sphere tessellations. Beginning with Voronoi tessellations, we show that our algorithm can remarkably convert extremely large nonhyperuniform packings into hyperuniform ones in R 2 and R 3 . Implementing our theoretical methodology on sphere tessellations, we establish the hyperuniformity of the classical Hashin-Shtrikman multiscale coated-spheres structures, which are known to be two-phase media microstructures that possess optimal effective transport and elastic properties. A consequence of our work is a rigorous demonstration that packings that have identical tessellations can either be nonhyperuniform or hyperuniform by simply tuning local characteristics. It is noteworthy that our computationally designed hyperuniform two-phase systems can easily be fabricated via state-of-theart methods, such as 2D photolithographic and 3D printing technologies. In addition, the tunability of our methodology offers a route for the discovery of novel disordered hyperuniform two-phase materials.

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Hidden Hyperuniformity in Soft Polymeric Materials

Cited by 50 publications

References 53 publications

Hidden Order Beyond Hyperuniformity in Critical Absorbing States

Hidden Order Beyond Hyperuniformity in Critical Absorbing States

Influence of Branching on the Configurational and Dynamical Properties of Entangled Polymer Melts

Methodology to construct large realizations of perfectly hyperuniform disordered packings

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