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    Precise determination of the long-time asymptotics of the diffusion spreadability of two-phase media

    Shaobing Yuan

    Salvatore Torquato*

    • Department of Chemistry and Princeton Institute for the Science and Technology of Materials, Princeton University, Princeton, New Jersey 08544, USA

    • Department of Chemistry, Department of Physics, Princeton Center for Theoretical Science, Princeton Institute for the Science and Technology of Materials, and Program in Applied and Computational Mathematics, Princeton University, Princeton, New Jersey 08544, USA

    • *Contact author: torquato@electron.princeton.edu

    Phys. Rev. E 113, 065421 – Published 23 June, 2026

    DOI: https://doi.org/10.1103/9vyf-br6d

    Abstract

    The time-dependent diffusion spreadability S(t) is a powerful dynamical probe of the microstructure of two-phase heterogeneous media across length scales [S. Torquato Phys. Rev. E 104, 054102 (2021)]. The spreadability can be exactly represented as a certain functional of the spectral density χ̃V(k), where k is the wave vector. Experimentally, it is intimately related to nuclear magnetic resonance (NMR) measurements in fluid-saturated media. The short-, intermediate-, and long-time behavior of the spreadability reflects structural features at small, intermediate, and large length scales, respectively. It has been shown that when the spectral density takes the power-law form χ̃V(k)∼|k|α as the wave number |k| tends to zero, the normalized excess spreadability sex(t) [proportional to S(∞)−S(t)] scales as sex(t)∼t−d+α2 in the long-time limit t→∞, enabling one to determine the infinite-wavelength scaling exponent α. An algorithm that allows one to reliably extract the exponent α from long-time spreadability data was previously devised [H. Wang and S. Torquato, Phys. Rev. Appl. 17, 034022 (2022)]. In this paper, we further improve this procedure to obtain α even more accurately by incorporating higher-order correction terms to the long-time asymptotics and by utilizing analyticity properties of χ̃V(k) at the origin. We illustrate our procedure by analyzing hyperuniform (α>0), typical nonhyperuniform (α=0), and antihyperuniform (−d<α<0) models of two-phase media. In addition, by combining the large-t asymptotic expansion of sex(t) with the small-t expansion, we have devised a two-point Padé approximant to accurately approximate sex(t) for all t with just a few parameters. Our findings facilitate the characterization of the microstructure of two-phase media across length scales as obtained from numerical spreadability data or experimental data obtained from NMR relaxation measurements. Our work can also be applied in the inverse design of two-phase microstructures with targeted spreadability behaviors.

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