Static structural signatures of nearly jammed disordered and ordered hard-sphere packings: Direct correlation function

Abstract

The nonequilibrium process by which hard-particle systems may be compressed into disordered, jammed states has received much attention because of its wide utility in describing a broad class of amorphous materials. While dynamical signatures are known to precede jamming, the task of identifying static structural signatures indicating the onset of jamming have proven more elusive. The observation that compressing hard-particle packings towards jamming is accompanied by an anomalous suppression of density fluctuations (termed "hyperuniformity") has paved the way for the analysis of jamming as an "inverted critical point" in which the direct correlation function c(r), rather than the total correlation function h(r), diverges. We expand on the notion that c(r) provides both universal and protocol-specific information as packings approach jamming. By considering the degree and position of singularities (discontinuities in the nth derivative) as well as how they are changed by the convolutions found in the Ornstein-Zernike equation, we establish quantitative statements about the structure of c(r) with regards to singularities it inherits from h(r). These relations provide a concrete means of identifying features that must be expressed in c(r) if one hopes to reproduce various details in the pair correlation function accurately and provide stringent tests on the associated numerics. We also analyze the evolution of systems of three-dimensional monodisperse hard spheres of diameter D as they approach ordered and disordered jammed configurations. For the latter, we use the Lubachevsky-Stillinger (LS) molecular dynamics and Torquato-Jiao (TJ) sequential linear programming algorithms, which both generate disordered packings, but can show perceptible structural differences. We identify a short-ranged scaling c(r) -1/r as r→0 that accompanies the formation of the delta function at c(D) that indicates the formation of contacts in all cases, and show that this scaling behavior is, in this case, a consequence of the growing long rangedness in c(r), e.g., c-1/r2 as r→ for disordered packings. At densities in the vicinity of the freezing density, we find striking qualitative differences in the structure factor S(k) as well as c(r) between TJ- and LS-generated configurations, including the early formation of a delta function at c(D) in the TJ algorithm's packings, indicating the early formation of clusters of particles in near contact. Both algorithms yield structure factors that tend towards zero in the low-wave-number limit as jamming is approached. Correspondingly, we observe the expected power-law decay in c(r) for large r, in agreement with previous theoretical work. Our work advances the notion that static signatures are exhibited by hard-particle packings as they approach jamming and underscores the utility of the direct correlation function as a sensitive means of monitoring for the appearance of an incipient rigid network. © 2016 American Physical Society.