La基非晶合金β弛豫行为: 退火和加载应变的影响

孟绍怡; 郝奇; 吕国建; 乔吉超

doi:10.7498/aps.72.20222389

摘要

β弛豫行为是理解非晶合金扩散、塑性变形和玻璃转变行为的重要切入口. 本研究以具有显著β弛豫行为的(La_0.6Ce_0.4)₆₅Al₁₀Co₂₅非晶合金为研究载体, 利用动态力学分析仪, 研究了加载频率、退火以及加载应变等因素对非晶合金β弛豫行为的影响. 结果表明, 随着加载频率的升高, 非晶合金β弛豫峰向高温段移动. 低于玻璃转变温度退火导致非晶合金β弛豫峰内耗值降低, 非晶合金“缺陷”浓度降低, 玻璃体系向更稳定状态迁移. 随加载应变幅值增大, 非晶合金β弛豫强度增大. 本研究为进一步厘清非晶合金β弛豫起源提供新思路.

关键词:

Abstract

The dynamic relaxation process of amorphous alloys is an important issue to understand the diffusion behavior, plastic deformation as well as glass transition phenomenon. In the current research, (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅ amorphous alloy with a pronounced β relaxation process was selected as a model system to study the dynamic mechanical relaxation processes. Influence of driving frequency, physical aging and applied strain amplitude on the β relaxation of the La-based metallic glass was probed process using dynamic mechanical analysis. The experimental results demonstrated that the peak of the β relaxation process shifts to high temperature by increasing the driving frequency. Physical aging below the glass transition temperature induces a decrease of the intensity of the β relaxation process. The “defects” of amorphous alloy decreases during the physical aging process, which is ascribed to the glassy system shifts to more stable state induced by physical aging treatment. In parallel, the intensity of the β relaxation process of the amorphous alloy increases by increasing strain amplitude. The research sheds new light on further understanding the physical origin of β relaxation process of the amorphous alloy.

Keywords:

作者及机构信息

西北工业大学力学与土木建筑学院, 西安　710072

通信作者: 乔吉超, qjczy@nwpu.edu.cn

基金项目: 国家自然科学基金 (批准号: 51971178, 52271153)和陕西省杰出青年基金(批准号: 2021JC-12).

Authors and contacts

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

Corresponding author: Qiao Ji-Chao, qjczy@nwpu.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 51971178, 52271153), and the Outstanding Youth Found of Shaanxi Province, China (Grant No. 2021JC-12 ).

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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X射线衍射图谱; (b) (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅非晶合金DSC曲线

Fig. 1. (a) XRD pattern of (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅ amorphous alloy; (b) DSC curve of (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅ amorphous alloy.

下载: 全尺寸图片幻灯片

图 2 (a) (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅非晶合金归一化储能模量${E'}/{{E}}_{\text{u}}$和损耗模量${E''}/{{E}}_{\text{u}}$随温度的演化(升温速率: 3 K/min, 加载频率: 0.7 Hz); (b) (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅非晶合金归一化损耗模量${E''}/{{E}}_{\text{u}}$在不同加载频率随温度的演化 (升温速率为3 K/min). 插图是β弛豫峰温与加载频率的关系, 实线为Arrhenius方程拟合

Fig. 2. (a) Temperature dependence of the normalized storage modulus ${E'}/{{E}}_{\text{u}}$ and loss modulus ${E''}/{{E}}_{\text{u}}$ for (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅ amorphous alloy (heating rate: 3 K/min , driving frequency: 0.7 Hz); (b) temperature dependence of the normalized loss modulus ${E''}/{{E}}_{\text{u}}$ for (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅ amorphous alloy with different frequency. Inset shows the frequency versus peak temperature of the β relaxation, the solid line is the Arrhenius equation fit.

下载: 全尺寸图片幻灯片

图 3 (a) 不同温度下(La_0.6Ce_0.4)₆₅Al₁₀Co₂₅非晶合金损耗模量${E''}/{{E}}_{\text{u}}$随加载频率演化; (b) (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅非晶合金等温和连续加热条件下β弛豫峰温与频率的关系, 实线为Arrhenius方程拟合

Fig. 3. (a) Frequency dependence of the normalized loss modulus ${E''}/{{E}}_{\text{u}}$ for (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅ amorphous alloy with different temperature; (b) the frequency versus peak temperature of the β relaxation with different states (isochronal mode and frequency sweep mode), the solid line is the Arrhenius equation fit.

下载: 全尺寸图片幻灯片

图 4 (a) (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅非晶合金等温原位退火过程储能模量${E'}/{{E}}_{\text{u}}$和内耗$ \tan\delta $随退火时间演化(退火温度为403 K, 加载频率为1 Hz, 实线为KWW拟合); (b) (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅非晶合金在铸态和退火态(退火样品的退火温度为403 K, 退火时间为10 h)储能模量和损耗模量随温度演化过程(升温速率: 3 K/min, 加载频率: 1 Hz)

Fig. 4. (a) Time dependence of the loss factor $ \tan\delta $ and normalized storage modulus ${E'}/{{E}}_{\text{u}}$ of (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅ amorphous alloy, annealing temperature is 403 K, driving frequency is 1 Hz, the solid line is the best fitting by the KWW equation); (b) annealing temperature is 403 K, annealing time is 10 h, temperature dependence of the normalized storage modulus ${E'}/{{E}}_{\text{u}}$ and loss modulus ${E''}/{{E}}_{\text{u}}$ of (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅ amorphous alloy with different states (as-cast and annealed state, heating rate: 3 K/min driving frequency: 1 Hz).

下载: 全尺寸图片幻灯片

图 5 退火与β弛豫在微观结构角度的关系示意图

Fig. 5. Schematic diagram of the relationship between annealing and β relaxation from the microstructural perspective.

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图 6 (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅非晶合金铸态和退火态Arrhenius方程拟合结果

Fig. 6. The frequency versus peak temperature of the β relaxation process with different states (as-cast and annealed states), the solid line is the Arrhenius equation fit.

下载: 全尺寸图片幻灯片

图 7 不同应变下(La_0.6Ce_0.4)₆₅Al₁₀Co₂₅非晶合金归一化损耗模量${E''}/{{E}}_{\text{u}}$随温度演化 (升温速率为3 K/min)

Fig. 7. Temperature dependence of the normalized loss modulus ${E''}/{{E}}_{\text{u}}$ for (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅ amorphous alloy with different strain (heating rate: 3 K/min).

下载: 全尺寸图片幻灯片

图 8 不同应变下(La_0.6Ce_0.4)₆₅Al₁₀Co₂₅非晶合金的激活能线性拟合结果

Fig. 8. Results of linear fitting of the activation energy of (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅ amorphous alloys with different strain

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图 9 (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅非晶合金激活能随应变演化示意图

Fig. 9. Strain dependence of activation energy for (La_0.6Ce_0.4)₆₅Al₁₀Co₂₅ amorphous alloy.

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[14]	Liu Y H, Wang D, Nakajima K, Zhang W, Hirata A, Nishi T, Inoue A, Chen M W 2011 Phys. Rev. Lett. 106 125504 Google Scholar
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[23]	Jiao W, Wen P, Peng H L, Bai H Y, Sun B A, Wang W H 2013 Appl. Phys. Lett. 102 101903 Google Scholar
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[26]	Liu Y H, Wang G, Wang R J, Zhao D Q, Pan M X, Wang W H 2007 Science 315 1385 Google Scholar
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[28]	Yu H B, Wang W H, Samwer K 2013 Mater. Today 16 183 Google Scholar
[29]	Wang J, Zhang X, Jiang L, Qiao J 2019 Prog. Polym. Sci. 98 101160 Google Scholar
[30]	Qiao J C, Wang Q, Crespo D, Yang Y, Pelletier J M 2017 Chin. Phys. B 26 016402 Google Scholar
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[33]	Li N, Xu X, Zheng Z, Liu L 2014 Acta Mater. 65 400 Google Scholar
[34]	Yu H B, Samwer K, Wu Y, Wang W H 2012 Phys. Rev. Lett. 109 095508 Google Scholar
[35]	Hao Q, Lyu G J, Pineda E, Pelletier J M, Wang Y J, Yang Y, Qiao J C 2022 Int. J. Plast. 154 103288 Google Scholar
[36]	Li R, Pang S, Ma C, Zhang T 2007 Acta Mater. 55 3719 Google Scholar
[37]	Menard K P 2015 Dynamic Mechanical Analysis (3rd Ed.) (Place: Published: Crc Press)
[38]	Zhao Z F, Wen P, Wang W H, Shek C H 2006 Appl. Phys. Lett. 89 071920 Google Scholar
[39]	Wang Q, Liu J J, Ye Y F, Liu T T, Wang S, Liu C T, Lu J, Yang Y 2017 Mater. Today 20 293 Google Scholar
[40]	Yu H B, Samwer K 2014 Phys. Rev. B 90 144201 Google Scholar
[41]	Goldstein M 2011 J. Non-Cryst. Solids 357 249 Google Scholar
[42]	Ke H B, Zeng J F, Liu C T, Yang Y 2014 Mater. Sci. Technol. 30 560 Google Scholar
[43]	Yang Y, Zeng J F, Volland A, Blandin J J, Gravier S, Liu C T 2012 Acta Mater. 60 5260
[44]	Perez J 1990 Solid State Ionics 39 69 Google Scholar
[45]	Cavaille J Y, Perez J, Johari G P 1989 Phys. Rev. B 39 2411
[46]	Ngai K L, Capaccioli S 2004 Phys. Rev. E 69 031501 Google Scholar
[47]	Lunkenheimer P, Wehn R, Schneider U, Loidl A 2005 Phys. Rev. Lett. 95 055702 Google Scholar
[48]	Zhao Y, Shang B, Zhang B, Tong X, Ke H, Bai H, Wang W H 2022 Sci. Adv. 8 eabn3623 Google Scholar
[49]	Qiao J, Pelletier J-M, Casalini R 2013 J. Phys. Chem. B 117 13658 Google Scholar
[50]	Wen P, Zhao Z F, Pan M X, Wang W H 2010 Phys. Status Solidi 207 2693 Google Scholar
[51]	Zhu F, Nguyen H, Song S, Aji D P, Hirata A, Wang H, Nakajima K, Chen M 2016 Nat. Commun. 7 1
[52]	Hiki Y, Tanahashi M, Takeuchi S 2008 J. Non-Cryst. Solids 354 1780 Google Scholar
[53]	Angell C A 1988 J. Non-Cryst. Solids 102 205 Google Scholar
[54]	郝奇, 乔吉超, Jean-Marc Pelletier 2020 力学学报 52 360 Google Scholar Hao Q, Qiao J C, Pelletier J M 2020 Acta Mech. Sin. 52 360 Google Scholar
[55]	Wang Z, Yu H B, Wen P, Bai H Y, Wang W H 2011 J. Phys. Condens. Mat. 23 142202 Google Scholar
[56]	Liu Y H, Fujita T, Aji D P B, Matsuura M, Chen M W 2014 Nat. Commun. 5 3238 Google Scholar
[57]	Evenson Z, Naleway S E, Wei S, Gross O, Kruzic J J, Gallino I, Possart W, Stommel M, Busch R 2014 Phys. Rev. B 89 174204 Google Scholar
[58]	Aji D P B, Johari G P 2015 J. Chem. Phys. 142 214501 Google Scholar
[59]	Johari G P 1976 Ann. Ny. Acad. Sci. 279 117 Google Scholar
[60]	Johari G P 2002 J. Non-Cryst. Solids 307-310 317
[61]	Johari G P, Goldstein M 1970 J. Chem. Phys. 53 2372 Google Scholar
[62]	Johari G P, Goldstein M 1971 J. Chem. Phys. 55 4245 Google Scholar
[63]	Perez J 1994 J. Food Eng. 22 89 Google Scholar
[64]	Wang Z, Wang W H 2019 Natl. Sci. Rev. 6 304 Google Scholar
[65]	Qiao J, Pelletier J-M, Esnouf C, Liu Y, Kato H 2014 J. Alloy. Compd. 607 139 Google Scholar
[66]	Gauthier C, David L, Ladouce L, Quinson R, Perez J 1997 J. Appl. Polym. Sci. 65 2517 Google Scholar
[67]	Sun Y, Concustell A, Greer A L 2016 Nat. Rev. Mater. 1 16039 Google Scholar

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La基非晶合金β弛豫行为: 退火和加载应变的影响