Coupling mechanism between high-temperature rheological behavior and dynamic relaxation in metallic glasses

LIANG Shuyi; ZHANG Langting; ZHU Hangchen; XING Guanghui; QIAO Jichao

doi:10.7498/aps.74.20250392

Abstract
This study aims to establish the intrinsic link between the high-temperature rheological behavior and kinetic relaxation characteristics of La-based metallic glasses. By conducting dynamic mechanical analysis and high-temperature tensile strain-rate jump experiments on three La-based metallic glasses with significant β relaxation, and combining the findings within the free volume theory framework, their high-temperature rheological properties are investigated systematically. The results show that the steady-state flow stress and activation volume evolution trend are consistent within the normalized temperature range. The average activation energy for high-temperature rheology aligns with the activation energy range of α relaxation, confirming the strong association between rheological behavior and α relaxation. The activation energy for β relaxation shows an opposite trend, indicating that it may precede α relaxation. A dynamic competition between defect annihilation and generation governs the rheological behavior, and kinetic parameters reveal the temperature and strain-rate sensitivity of metallic glasses. This study lays a theoretical foundation for optimizing the high-temperature mechanical properties of La-based metallic glasses and also provides new insights into understanding the coupling relationship between multi-scale relaxation behavior and rheological mechanisms in metallic glasses.

Keywords:
metallic glass /

high-temperature rheological behavior /

relaxation /

defect evolution
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图 1 La₆₂Al₁₄Ag_2.34Ni_10.83Co_10.83, La₂₀Ce₂₀Y₂₀Ni₂₀Al₂₀和(La_0.6Ce_0.4)₆₅Al₁₀Co₂₅非晶合金归一化内耗随归一化温度的演化(驱动频率: 1 Hz; 升温速率: 3 K/min)

Figure 1. Evolution of the normalized internal friction with the normalized temperature for La₆₂Al₁₄Ag_2.34Ni_10.83Co_10.83, La₂₀Ce₂₀Y₂₀Ni₂₀Al₂₀ and (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅ metallic glasses (driving frequency: 1 Hz; heating rate: 3 K/min).

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图 2 在0.92T_α, 0.93T_α, 0.94T_α, 0.95T_α下,　(a) La₆₂Al₁₄Ag_2.34Ni_10.83Co_10.83, (b) La₂₀Ce₂₀Y₂₀Ni₂₀Al₂₀和(c) (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅非晶合金拉伸应变率跳跃实验(应变率: 2.5$ \text{×} $10^–4 —1.25$ \text{×} $10^–3 s^–1)的应力-应变曲线

Figure 2. Stress-strain curves from tensile strain-rate jump experiments (strain rate ranging from 2.5$ \text{×} $10^–4 to 1.25$ \text{×} $10^–3 s^–1) of (a) La₆₂Al₁₄Ag_2.34Ni_10.83Co_10.83, (b) La₂₀Ce₂₀Y₂₀Ni₂₀Al₂₀ and (c) (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅ metallic glasses at 0.92T_α, 0.93T_α, 0.94T_α and 0.95T_α, respectively.

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图 3 (a) La₂₀Ce₂₀Y₂₀Ni₂₀Al₂₀非晶合金(La-2)在高温拉伸应变率跳过程中峰值应力随应变率的演化及其基于(1)式的拟合曲线; (b) La基非晶合金峰值应力处激活体积随归一化温度的演化

Figure 3. (a) Evolution of the peak stress with the strain rate during the high-temperature tensile strain-rate jump process of La₂₀Ce₂₀Y₂₀Ni₂₀Al₂₀ metallic glass (La-2) and the fitting curves based on Eq. (1); (b) evolution of the activation volume at the peak stress of La-based metallic glasses with the normalized temperature.

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图 4 (a) La基非晶合金的参考应变率$ {\dot{\varepsilon }}_{0} $与归一化温度的关系; (b) La基非晶合金在0.92T_α—0.95T_α时无外力作用下扩散的平均激活能

Figure 4. (a) Relationship between the reference strain rate $ {\dot{\varepsilon }}_{0} $ and the normalized temperature of La-based metallic glasses; (b) average activation energy for diffusion without an applied force of La-based metallic glasses at 0.92T_α—0.95T_α.

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图 5 (a) 350—390 K温度下La₂₀Ce₂₀Y₂₀Ni₂₀Al₂₀非晶合金(La-2)内耗的频率谱; (b) La基非晶合金体系β弛豫过程中激励频率与峰值温度之间的关系及Arrhenius拟合; (c) 三种La基非晶合金体系的β弛豫激活能

Figure 5. (a) Frequency spectra of the internal friction of the La₂₀Ce₂₀Y₂₀Ni₂₀Al₂₀ metallic glass (La-2) at temperatures ranging from 350 to 390 K; (b) the relationship between the driving frequency and the peak temperature during β relaxation process in the La-based metallic glasses, along with the Arrhenius fitting; (c) activation energies of β relaxation for the La-based metallic glasses.

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图 6 La基非晶合金　((a) La-1, (b) La-2, (c) La-3)高温拉伸应变率跳跃实验应力随时间的演化及其基于自由体积理论的拟合结果

Figure 6. Evolution of stress with time during the high-temperature tensile strain-rate jump experiments of the La-based metallic glasses and fitting results based on the free volume theory ((a) La-1, (b) La-2, (c) La-3).

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图 7 (a) La基非晶合金流变阶段相对缺陷浓度随应变率及温度的演化; (b) La基非晶合金高温拉伸应变率跳过程中相对缺陷浓度演化

Figure 7. (a) Evolution of the relative defect concentration with strain rate and temperature during the rheological stage of La-based metallic glasses; (b) evolution of the relative defect concentration during the high-temperature tensile strain-rate jump process of La-based metallic glasses.

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图 8 (a) La基非晶合金缺陷生成速率与湮灭速率的比值随温度的演化; (b) 不同非晶合金的$ -{\mathrm{d}}({a}_{x}/{k}_{{\mathrm{r}}})/{\mathrm{d}}T $

Figure 8. (a) Evolution of the ratio between the defect generation rate and the annihilation rate with temperature for La-based metallic glasses; (b) $ -{\mathrm{d}}({a}_{x}/{k}_{{\mathrm{r}}})/{\mathrm{d}}T $ for different metallic glasses.

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