The Cooperativity of Atomic Fluctuations in Highly Supercooled Glass-Forming Metallic Melts

IF 4.8 2区 化学 Q2 CHEMISTRY, PHYSICAL
Jürgen E. K. Schawe, Min Kyung Kwak, Mihai Stoica, Eun Soo Park, Jörg F. Löffler
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Abstract

The behavior of supercooled glass-forming metals depends on the cooperative atomic fluctuations caused by dynamic heterogeneities in the melt. These spatial and temporal heterogeneities form dynamic clusters, which are regions of cooperative rearrangement (CRR). In this study, the macroscopic kinetics and the correlation length ξ, of the CRR, are derived for Pt57.4Cu14.7Ni5.3P22.6 and Pd43Cu27Ni10P20 metallic glass-formers by fast differential scanning calorimetry near the glass transition. While the alloy composition influences the α-relaxation and vitrification kinetics, typically defined by the glass transition, as well as the limiting temperature of the Vogel–Fulcher–Tammann–Hesse equation and the fragility index, it has no significant influence on the correlation length of the cooperative atomic motions. In agreement with many other materials, ξ is about 3 nm at the glass transition for both metallic glasses. The temperature dependence of ξ correlates with the apparent activation energy of the α-relaxation and is the reason for its non-Arrhenius behavior.

Abstract Image

高度过冷玻璃成形金属熔体中原子波动的协同性
过冷玻璃成形金属的行为取决于熔体中动态非均质性引起的协同原子波动。这些时空异质性形成了动态集群,这些集群是协同重排(CRR)区域。本研究利用快速差示扫描量热法,在玻璃化转变附近得到了Pt57.4Cu14.7Ni5.3P22.6和Pd43Cu27Ni10P20金属玻璃的宏观动力学和相关长度ξ。虽然合金成分影响α-弛豫和玻璃化动力学(通常由玻璃化转变定义),以及Vogel-Fulcher-Tammann-Hesse方程的极限温度和脆性指数,但对协同原子运动的相关长度没有显著影响。与许多其他材料一致,两种金属玻璃在玻璃化转变处ξ值约为3nm。ξ的温度依赖性与α-弛豫的表观活化能有关,是其具有非arrhenius行为的原因。
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来源期刊
The Journal of Physical Chemistry Letters
The Journal of Physical Chemistry Letters CHEMISTRY, PHYSICAL-NANOSCIENCE & NANOTECHNOLOGY
CiteScore
9.60
自引率
7.00%
发文量
1519
审稿时长
1.6 months
期刊介绍: The Journal of Physical Chemistry (JPC) Letters is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An important criterion for acceptance is that the paper reports a significant scientific advance and/or physical insight such that rapid publication is essential. Two issues of JPC Letters are published each month.
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