冷却速率对La基非晶合金<i>β</i>弛豫行为和应力弛豫的影响

孟绍怡; 郝奇; 王兵; 段亚娟; 乔吉超

doi:10.7498/aps.73.20231417

摘要

β弛豫行为及应力弛豫是探索非晶合金微观结构非均匀性的重要切入口. β弛豫行为及应力弛豫与非晶合金扩散、玻璃转变行为以及塑性变形等密切相关, 探究它们之间关联有重要科学意义. 本文以典型的La基非晶合金作为研究载体, 系统地探究了通过不同冷却速率所得块体样品与条带样品的β弛豫特征及应力弛豫行为. 结果表明, 冷却速率是控制玻璃体系能量状态, 进而影响其物理力学性能的重要参数. 冷却速率越大, 低温内耗更大, 对应β弛豫激活能更小, β弛豫行为在温度谱中展宽更大, 表明高冷却速率导致原子移动性更大, 微观尺度结构非均匀程度更高. 基于应力弛豫测量与分析, 发现高冷却速率变形特征时间减小, 归一化应力衰减幅度更大, 在外加力场作用下更易变形, 变形单元更易激活以容纳结构形变. 本研究为进一步厘清非晶合金β弛豫、变形及微观结构非均匀性之间关联提供了思路.

关键词:

Abstract

The dynamic relaxation process and stress relaxation process are two important processes which can reflect the microstructures of materials, for they are closely related to the diffusions, the glass transition phenomena and the microstructural heterogeneities. It is of great significance to explore the relationship among them. In the current research, the β-relaxation characteristics and stress relaxation behaviors of bulk and ribbon samples obtained by different cooling rates are systematically investigated by taking the typical La-based amorphous alloys as model systems. The experimental results demonstrate that the cooling rate is an important parameter for controlling the energy state of the glass system, which further affects its physical and mechanical properties. Based on the dynamical mechanical spectra, the larger the cooling rate, the greater the low-temperature internal friction is and the smaller the beta relaxation activation energy according to Arrhenius calculations, and the greater the broadening of the beta relaxation behavior in the temperature spectra, suggesting that the higher cooling rate leads to greater atomic mobility and a high degree of heterogeneity in the microstructure. Thermodynamic analysis is conducted to study the slow process of thermal activation and the fast process driven by stress. At low temperature, the activation volume of the strip sample is larger than that of the bulk sample, and the activation volume values of the two samples are almost the same, as the cooling rate only affect the β relaxation stage, but exert little effect on the α relaxation, which is consistent with the conclusion that the stress relaxation behavior and β relaxation behavior are related to the structural non-uniformity of the amorphous alloy. The stress relaxation tests show that the characteristic time of deformation decreases at higher cooling rate, the normalized stress decay is larger, it is easier to deform under an applied force field, and the deformation unit is more likely to activate to accommodate structural deformation. The correlation between stress relaxation and β relaxation of amorphous alloy is further confirmed, and the proportion of liquid-like region is proportional to the relaxation mode spectrum, which also shows that β relaxation and stress relaxation are consistent. Finally, by calculating relaxation enthalpy $ \Delta {H}_{{\mathrm{r}}{\mathrm{e}}{\mathrm{l}}} $, the variation of microstructure heterogeneity with cooling rate is experimentally verified. The research sheds new light on further clarifying the relationship among β relaxation, deformation and microstructural heterogeneity of the amorphous alloy.

Keywords:

作者及机构信息

1.
西北工业大学力学与土木建筑学院, 西安　710072

2.
西北工业大学物理科学与技术学院, 西安　710072

3.
西北工业大学重庆科创中心, 重庆　401135

通信作者: 王兵, wangbing0614@nwpu.edu.cn ; 乔吉超, qjczy@nwpu.edu.cn

基金项目: 国家自然科学基金(批准号: 51971178, 52271153, 52101201)、陕西省杰出青年基金(批准号: 2021JC-12)、重庆市自然科学基金(批准号: cstc2021jcyj-msxmX0369)、西北工业大学硕士研究生实践创新能力培育基金(批准号: PF2023088)和陕西省科技创新团队科学基金(批准号: 2021TD-14)资助的课题.

Authors and contacts

1.
School of Mechanics, Civil Engineering and Architecture, Northwestern Polytechnical University, Xi’an 710072, China

2.
School of Physical Science and Technology, Northwestern Polytechnical University, Xi’an 710072, China

3.
Chongqing Innovation Center, Northwestern Polytechnical University, Chongqing 401135, China

Corresponding author: Wang Bing, wangbing0614@nwpu.edu.cn ; Qiao Ji-Chao, qjczy@nwpu.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 51971178, 52271153, 52101201), the Outstanding Youth Foundation of Shaanxi Province, China (Grant No. 2021JC-12), the Natural Science Foundation of Chongqing, China (Grant No. cstc2021jcyj-msxmX0369), the Practical Innovation Ability Cultivation Fund for Postgraduate Students of Northwestern Polytechnical University, China (Grant No. PF2023088), and the Science and Technology Innovation Team Science Fund of Shaanxi Province, China (Grant No. 2021TD-14).

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参考文献

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施引文献

图 1 (a) (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅非晶合金内耗随温度演化(升温速率为2 K/min, 加载频率为1 Hz); (b) (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅非晶合金损耗模量随温度演化, 实线为准点缺陷公式拟合β弛豫结果

Fig. 1. (a) Temperature dependence of the internal friction for (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅ amorphous alloy (heating rate: 2 K/min, driving frequency: 1 Hz); (b) temperature dependence of the loss modulus $ {E}'' $ for (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅ amorphous alloy. The solid line is the β relaxation result fitted by QPD theory.

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图 2 (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅非晶合金不同加载频率归一化损耗模量$ {E''}/{E}_{{\mathrm{u}}} $随温度演化　(a)块体样品; (b) 条带样品; 升温速率为2 K/min; 插图为β弛豫峰温与加载频率关系, 实线为Arrhenius方程拟合

Fig. 2. Temperature dependence of the normalized loss modulus ${E''}/{E}_{{\mathrm{u}}} $ for (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅ amorphous alloy with different frequency: (a) Bulk; (b) ribbon. Inset shows the frequency versus peak temperature of the β relaxation, the solid line is the Arrhenius equation fit.

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图 3 (a) 不同温度下(La_0.6Ce_0.4)₆₅Al₁₀Co₂₅非晶合金块体样品归一化损耗模量$ {E''}/{E}_{{\mathrm{u}}} $随加载频率演化^[51]; (b) 不同温度下(La_0.6Ce_0.4)₆₅Al₁₀Co₂₅非晶合金条带样品归一化损耗模量$ {E''}/{E}_{{\mathrm{u}}} $随加载频率演化; (c) (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅非晶合金块体样品和条带样品等温扫频条件β弛豫峰温和频率的关系, 实线为Arrhenius方程拟合; (d) (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅非晶合金块体样品和条带样品的损耗模量在320 K参考温度下主曲线(实线为(1)式拟合结果)

Fig. 3. (a) Frequency dependence of the normalized loss modulus ${E''}/{E}_{{\mathrm{u}}} $ for (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅ amorphous alloy with different temperature (bulk); (b) frequency dependence of the normalized loss modulus ${E''}/{E}_{{\mathrm{u}}} $ for (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅ amorphous alloy with different temperature (ribbon); (c) the frequency versus peak temperature of the β relaxation with different states (bulk and ribbon), the solid line is the Arrhenius equation fit; (d) main curve of loss modulus for amorphous alloy with different states (bulk sample and ribbon sample) at 320 K (solid line is fitting result of Eq. (1)).

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图 4 (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅非晶合金在310—425 K 的应力弛豫曲线(实线为KWW 方程拟合结果)　(a) 块体样品; (b) 条带样品; (c) 370 K下块体样品及条带样品应力弛豫曲线; (d) (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅非晶合金应力弛豫过程中特征弛豫时间$ {\tau }_{{\mathrm{c}}} $对数随温度演化

Fig. 4. Stress relaxation curve of (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅ amorphous alloy from 310 K to 425 K (solid line is the fitting results based on KWW equation): (a) Bulk; (b) ribbon; (c) stress relaxation curves of 370 K for bulk and ribbon; (d) temperature dependence of the logarithm of characteristic relaxation time $ {\tau }_{{\mathrm{c}}} $ in stress relaxation process for (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅ amorphous alloy.

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图 5 (a) (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅非晶合金块体样品$\ln(-\dot{\sigma }) $与应力关系; (b) 快过程和慢过程的激活体积随温度演化

Fig. 5. (a) Dependence of $ \ln(-\dot{\sigma }) $ on stress for (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅ amorphous alloy bulk sample; (b) temperature dependence of the derived activation volume for the fast and slow events.

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图 6 (a) (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅非晶合金不同温度下应力弛豫曲线初始应力和最终应力演化; (b) $ \theta $随温度演化; (c) $ {\mathrm{d}}\theta /{\mathrm{d}}T $随温度演化

Fig. 6. (a) Initial stress and terminal stress evolution of stress relaxation curves for (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅ amorphous alloy at different temperatures; (b) temperature dependence of the $ \theta $ for bulk and ribbon samples; (c) temperature dependence of the $ {\mathrm{d}}\theta /{\mathrm{d}}T $ for bulk and ribbon samples.

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图 7 块体样品和条带样品(La_0.6Ce_0.4)₆₅Al₁₀Co₂₅非晶合金DSC曲线

Fig. 7. DSC curves of (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅ amorphous alloy for bulk and ribbon samples.

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map

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[35]	Liang S Y, Zhang L T, Wang B, Wang Y J, Pineda E, Qiao J C 2024 Intermetallics 164 108115 Google Scholar
[36]	Luo P, Li M X, Jiang H Y, Wen P, Bai H Y, Wang W H 2017 J. Appl. Phys. 121 135104 Google Scholar
[37]	Luo P, Wen P, Bai H Y, Ruta B, Wang W H 2017 Phys. Rev. Lett. 118 225901 Google Scholar
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冷却速率对La基非晶合金β弛豫行为和应力弛豫的影响