Discovery of collective nonjumping motions leading to Johari–Goldstein process of stress relaxation in model ionic glass

IF 8.3 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY
Makina Saito, Takeaki Araki, Yohei Onodera, Koji Ohara, Makoto Seto, Yoshitaka Yoda, Yusuke Wakabayashi
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Abstract

The slow β, or Johari–Goldstein (JG) relaxation process, has been widely observed in glasses and is known to induce the stress relaxation associated with mechanical properties. So far, jumping motions of only a fraction of the particles were believed to contribute to the JG process in glass. However, there is no direct experimental evidence of the atomic-scale images due to the difficulties in microscopic observation. In this study, atomic motions in the quasi-spherical model ionic-glass-former Ca0.4K0.6(NO3)1.4 were microscopically observed with one-angstrom resolution, the highest resolution to date, using X-ray time-domain interferometry. The microscopic experiment directly indicated that most particles underwent angstrom-scale motions in the time scale of the JG relaxation. This result was further supported by molecular dynamics (MD) simulations. A combined study of experiments and MD simulations revealed that most particles contributed to the JG process through unexpected collective nonjumping motions with angstrom-scale displacement, activated by jumping motions of a fraction of particles. The discovery of nonjumping motions by our atomic-scale dynamic observations has considerably advanced our understanding of the puzzling mechanism of the JG process.

Abstract Image

发现导致模型离子玻璃应力松弛的乔哈里-戈尔茨坦集体非跳跃运动过程
在玻璃中广泛观察到缓慢的 β 或乔哈里-戈尔茨坦(JG)弛豫过程,众所周知,这种过程会引起与机械特性相关的应力弛豫。迄今为止,人们认为只有一小部分颗粒的跃迁运动促成了玻璃中的 JG 过程。然而,由于显微镜观察的困难,原子尺度图像没有直接的实验证据。在这项研究中,利用 X 射线时域干涉测量法,以迄今为止最高的一埃特分辨率对准球形模型离子玻璃形成体 Ca0.4K0.6(NO3)1.4 中的原子运动进行了微观观察。显微实验直接表明,大多数粒子在 JG 松弛的时间尺度内发生了埃级运动。分子动力学(MD)模拟进一步证实了这一结果。对实验和 MD 模拟的综合研究表明,大多数粒子是通过意想不到的具有埃量级位移的集体非跳跃运动来促进 JG 过程的,而一部分粒子的跳跃运动则激活了这一过程。通过原子尺度动态观测发现的非跳跃运动大大推进了我们对令人费解的 JG 过程机制的理解。
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来源期刊
Acta Materialia
Acta Materialia 工程技术-材料科学:综合
CiteScore
16.10
自引率
8.50%
发文量
801
审稿时长
53 days
期刊介绍: Acta Materialia serves as a platform for publishing full-length, original papers and commissioned overviews that contribute to a profound understanding of the correlation between the processing, structure, and properties of inorganic materials. The journal seeks papers with high impact potential or those that significantly propel the field forward. The scope includes the atomic and molecular arrangements, chemical and electronic structures, and microstructure of materials, focusing on their mechanical or functional behavior across all length scales, including nanostructures.
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