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金属玻璃中笼状动力学、α弛豫和乔哈里-戈尔茨坦β弛豫的等时叠加

Isochronal superpositioning of the caged dynamics, the α, and the Johari-Goldstein β relaxations in metallic glasses.

作者信息

Ren N N, Guan P F, Ngai K L

机构信息

Beijing Computational Science Research Center, Beijing 100193, China.

CNR-IPCF, Largo B. Pontecorvo 3, I-56127 Pisa, Italy.

出版信息

J Chem Phys. 2021 Dec 28;155(24):244502. doi: 10.1063/5.0072527.

Abstract

The superposition of the frequency dispersions of the structural α relaxation determined at different combinations of temperature T and pressure P while maintaining its relaxation time τ(T, P) constant (i.e., isochronal superpositioning) has been well established in molecular and polymeric glass-formers. Not known is whether the frequency dispersion or time dependence of the faster processes including the caged molecule dynamics and the Johari-Goldstein (JG) β relaxation possesses the same property. Experimental investigation of this issue is hindered by the lack of an instrument that can cover all three processes. Herein, we report the results from the study of the problem utilizing molecular dynamics simulations of two different glass-forming metallic alloys. The mean square displacement 〈Δrt〉, the non-Gaussian parameter αt, and the self-intermediate scattering function Fq,t at various combinations of T and P were obtained over broad time range covering the three processes. Isochronal superpositioning of 〈Δrt〉, αt, and Fq,t was observed over the entire time range, verifying that the property holds not only for the α relaxation but also for the caged dynamics and the JG β relaxation. Moreover, we successfully performed density ρ scaling of the time τT,P at the peak of αt and the diffusion coefficient D(T, P) to show both are functions of ρ/T with the same γ. It follows that the JG β relaxation time τ(T, P) is also a function of ρ/T since τT,P corresponds to τ(T, P).

摘要

在分子和聚合物玻璃形成体中,在保持结构α弛豫的弛豫时间τ(T, P)恒定的情况下(即等时叠加),确定在不同温度T和压力P组合下的结构α弛豫的频率色散叠加已经得到了很好的确立。尚不清楚的是,包括笼中分子动力学和乔哈里-戈尔茨坦(JG)β弛豫在内的较快过程的频率色散或时间依赖性是否具有相同的性质。由于缺乏能够涵盖所有这三个过程的仪器,对这个问题的实验研究受到了阻碍。在此,我们报告利用两种不同的玻璃形成金属合金的分子动力学模拟对该问题的研究结果。在涵盖这三个过程的宽广时间范围内,获得了在各种T和P组合下的均方位移〈Δrt〉、非高斯参数αt和自中间散射函数Fq,t。在整个时间范围内观察到〈Δrt〉、αt和Fq,t的等时叠加,证实该性质不仅适用于α弛豫,也适用于笼中动力学和JGβ弛豫。此外,我们成功地对αt峰值处的时间τT,P和扩散系数D(T, P)进行了密度ρ标度,以表明两者都是ρ/T的函数,且具有相同的γ。由此可知,JGβ弛豫时间τ(T, P)也是ρ/T的函数,因为τT,P对应于τ(T, P)。

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