Evolution of defect concentration in Zr50–xCu34Ag8Al8Pdx (x = 0, 2) amorphous alloys derived using shear modulus and calorimetric data

Cheng Yi-Ting; Andrey S. Makarov; Gennadii V. Afonin; Vitaly A. Khonik; Qiao Ji-Chao

doi:10.7498/aps.70.20210256

Abstract

Amorphous alloys exhibit unique physical and mechanical properties, which are closely connected with their microstructural heterogeneity. The correlation between structural heterogeneity and mechanical properties is one of the important issues of amorphous alloys. Micro-alloying is an effective way to tune the mechanical and physical properties of amorphous alloys. In the present study, Zr_50–_xCu₃₄Ag₈Al₈Pd_x (x = 0 and 2) amorphous alloys with ability to form excellent glass are chosen as model alloys. The evolutions of heat flow and shear modulus in different states (as-cast, relaxed and crystalline) with temperature of Zr_50–_xCu₃₄Ag₈Al₈Pd_x (x = 0 and 2) glass system are studied by differential scanning calorimetry (DSC) and electromagnetic-acoustic transformation (EMAT) technique, respectively. The experiment demonstrates that a decrease of the shear modulus is accompanied by the endothermic heat flow and vice versa. The correlation between the heat flow and shear modulus is investigated according to the interstitialcy theory. The calculations of the interstitialcy defect concentration and activation energy spectra suggest that the microstructure remains stable at relatively low temperatures. When temperature increases, the interstitialcy defect structure is activated. Compared with that in the as-cast state, the interstitialcy defect concentration in the relaxed state is reduced by structural relaxation, indicating that temperature-dependent shear modulus softening is inhibited. At temperatures above glass transition temperature, a rapid growth of interstitialcy defect concentration results in the accelerated shear softening, which is accompanied by significant endothermic heat flow. It is noted that the minor addition of palladium reduces the interstitialcy defect concentration in the Zr_50–_xCu₃₄Ag₈Al₈Pd_x (x = 0 and 2) metallic glass systems. It is suggested that the introduction of Pd reduces the atomic mobility and increases the characteristic relaxation time. In parallel, the change of shear modulus as a function of the aging time (below the glass transition temperature) is studied by using EMAT equipment. The results indicate that the interstitialcy defect concentration decreases in the physical aging process, which is accompanied by an increase of shear modulus. The interstitialcy defect concentration and shear modulus change towards the quasi-equilibrium state with aging time increasing. A reduction of the interstitialcy defect concentration leads to a decrease of the shear modulus change upon microalloying by Pd into Zr_50–_x Cu₃₄Ag₈Al₈Pd_x (x = 0 and 2) metallic glass system.

Keywords:

Authors and contacts

1.
School of Mechanics, Civil Engineering and Architecture, Northwestern Polytechnical University, Xi’an 710072, China
2.
Department of General Physics, Voronezh State Pedagogical University, Voronezh 394043, Russia

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

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 51971178), the Natural Science Foundation of Shaanxi Province, China (Grant No. 2019JM-344), and the Russian Science Foundation (Grant No. 20-62-46003)

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References

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Cited By

图 1 (a) Zr₅₀Cu₃₄Ag₈Al₈和(b)Zr₄₈Cu₃₄Ag₈Al₈Pd₂非晶合金DSC曲线. Run1为由室温升温至715 K的过程, Run2为室温升温至823 K的过程, Run3为室温升温至823 K的过程. 升温速率为3 K/min; (c) Zr_50–_xCu₃₄Ag₈Al₈Pd_x(x = 0, 2)非晶合金铸态DSC曲线; (d)升温过程示意图

Figure 1. (a) DSC curves of Zr₅₀Cu₃₄Ag₈Al₈ and (b) Zr₄₈Cu₃₄Ag₈Al₈Pd₂ metallic glasses. Run1, Run2 and Run3 correspond to heating from room temperature up to 715 K, 823 K and 823 K, respectively; (c) DSC curves of Zr_50–_xCu₃₄Ag₈Al₈Pd_x (x = 0, 2) metallic glasses (as-cast state) on an enlarged scale; (d) schematic diagram of heating process.

DownLoad: Full-Size Img PowerPoint

图 2 (a) Zr₅₀Cu₃₄Ag₈Al₈和(b) Zr₄₈Cu₃₄Ag₈Al₈Pd₂非晶合金剪切模量在3次升温过程中随温度演化过程

Figure 2. Evolution of the shear modulus with temperature during three subsequent heating runs of (a) Zr₅₀Cu₃₄Ag₈Al₈ and (b) Zr₄₈Cu₃₄Ag₈Al₈Pd₂ metallic glasses.

DownLoad: Full-Size Img PowerPoint

图 3 Zr_50–_xCu₃₄Ag₈Al₈Pd_x(x = 0, 2)非晶合金的(a)铸态和弛豫态自间隙缺陷浓度以及(b)自间隙缺陷浓度随温度的变化率(${{{\rm{d}}c(T)} / {{\rm{d}}T}}$)随温度的演化

Figure 3. (a) Evolution of the defect concentration in the as-cast and relaxed samples and (b) the rate of defect concentration change (${{{\rm{d}}c(T)} / {{\rm{d}}T}}$) as a function of temperature for Zr_50–_xCu₃₄Ag₈Al₈Pd_x (x = 0, 2) metallic glasses.

DownLoad: Full-Size Img PowerPoint

图 4 Zr_50–_xCu₃₄Ag₈Al₈Pd_x(x = 0, 2)非晶合金的激活能谱

Figure 4. Activation energy spectra for Zr_50–_xCu₃₄Ag₈Al₈Pd_x (x = 0, 2) metallic glasses.

DownLoad: Full-Size Img PowerPoint

图 5 物理时效过程中Zr_50–_xCu₃₄Ag₈Al₈Pd_x(x = 0, 2)非晶合金剪切模量的变化$g(T)$和自间隙缺陷浓度随物理时效时间的演化过程.

Figure 5. Сhange of the shear modulus $g(T)$ and defect concentration with the aging time for Zr_50–_xCu₃₄Ag₈Al₈Pd_x (x = 0, 2) metallic glasses

DownLoad: Full-Size Img PowerPoint

[1]	Qiao J C, Wang Q, Crespo D, Yang Y, Pelletier J M 2017 Chin. Phys. B 26 016402 Google Scholar
[2]	Debenedetti P G, Stillinger F H 2001 Nature 410 259 Google Scholar
[3]	Torquato S 2000 Nature 405 521 Google Scholar
[4]	王军强, 欧阳酥 2017 物理学报 66 176102 Google Scholar Wang J Q, Ouyang S 2017 Acta Phys. Sin. 66 176102 Google Scholar
[5]	Qiao J C, Wang Q, Pelletier J M, Kato H, Casalini R, Crespo D, Pineda E, Yao Y, Yang Y 2019 Prog. Mater Sci. 104 250 Google Scholar
[6]	Wang W H 2012 Prog. Mater Sci. 57 487 Google Scholar
[7]	王峥, 汪卫华 2017 物理学报 66 176103 Google Scholar Wang Z, Wang W H 2017 Acta Phys. Sin. 66 176103 Google Scholar
[8]	Perez J 1988 Polymer 29 483 Google Scholar
[9]	Perez J 1990 Solid State Ion. 39 69 Google Scholar
[10]	Spaepen F 1977 Acta Metall. 25 407
[11]	Dyre, J C 2008 Rev. Mod. Phys. 78 953
[12]	Makarov A S, Khonik V A, Mitrofanov Y P, Granato A V, Joncich D M, Khonik S V 2013 Appl. Phys. Lett. 102 091908 Google Scholar
[13]	Chen H S 1980 Rep. Prog. Phys. 43 353 Google Scholar
[14]	Kobelev N P, Khonik V A 2015 J. Non-Cryst. Solids 427 184 Google Scholar
[15]	Khonik V A 2015 Metals 5 504 Google Scholar
[16]	Demetriou M D, Harmon J S, Tao M, Duan G, Samwer K, Johnson W L 2006 Phys. Rev. Lett. 97 065502 Google Scholar
[17]	Granato A V 1992 Phys. Rev. Lett. 68 974 Google Scholar
[18]	Granato A V 2014 Eur. Phys. J. B 87 18 Google Scholar
[19]	Khonik V A 2017 Chin. Phys. B 26 016401 Google Scholar
[20]	Makarov A S, Mitrofanov Y P, Afonin G V, Kobelev N P, Khonik V A 2019 Scripta Mater. 168 10 Google Scholar
[21]	Hao Q, Qiao J C, Goncharova E V, Afonin G V, Liu M N, Cheng Y T, Khonik V A 2020 Chin. Phys. B 29 86402 Google Scholar
[22]	Duan Y J, Qiao J C, Crespo D, Goncharova E V, Makarov A S, Afonin G V, Khonik V A 2020 J. Alloys Compd. 830 154564 Google Scholar
[23]	Jiang Q K, Wang X D, Nie X P, Zhang G Q, Ma H, Fecht H J, Bednarcik J, Franz H, Liu Y G, Cao Q P, Jiang J Z 2008 Acta Mater. 56 1785 Google Scholar
[24]	Afonin G V, Mitrofanov Y P, Makarov A S, Kobelev N P, Wang W H, Khonik V A 2016 Acta Mater. 115 204 Google Scholar
[25]	张浪渟, Khonik V A, 乔吉超 2020 力学学报 52 1709 Google Scholar Zhang L T, Khonik V A, Qiao J C 2020 Chin. J Theor. Appl. Mech. 52 1709 Google Scholar
[26]	Cheng Y T, Hao Q, Qiao J C, Crespo D, Pineda E, Pelletier J M 2021 J. Non-Cryst. Solids 553 120496 Google Scholar
[27]	Vasilev A N, Gaidukov Y P 1983 Uspekhi Fizicheskikh Nauk 141 431 Google Scholar
[28]	Zhang W, Zhang Q, Inoue A 2008 Adv. Eng. Mater. 10 1034 Google Scholar
[29]	Makarov S, Mitrofanov Y P, Afonin G V, Kobelev N P, Khonik V A 2017 Intermetallics 87 1 Google Scholar
[30]	Tao K, Qiao J C, He Q F, Song K K, Yang Y 2021 Int. J. Mech. Sci. 201 106469 Google Scholar
[31]	Khonik S V, Granato A V, Joncich D M, Pompe A, Khonik V A 2008 Phys. Rev. Lett. 100 065501 Google Scholar
[32]	Ma E 2015 Nat. Mater. 14 547 Google Scholar
[33]	Yu H B, Shen X, Wang Z, Gu L, Wang W H, Bai H Y 2012 Phys. Rev. Lett. 108 015504 Google Scholar
[34]	Shen J, Huang Y J, Sun J F 2007 J. Mater. Res. 22 3067 Google Scholar
[35]	Ketov S V, Sun Y H, Nachum S, Lu Z, Checchi A, Beraldin A R, Bai H Y, Wang W H, Louzguine-Luzgin D V, Carpenter M A, Greer A L 2015 Nature 524 200 Google Scholar
[36]	Park K W, Lee C M, Wakeda M, Shibutani Y, Falk M L, Lee J C 2008 Acta Mater. 56 5440 Google Scholar
[37]	Tong Y, Iwashita T, Dmowski W, Bei H, Yokoyama Y, Egami T 2015 Acta Mater. 86 240 Google Scholar
[38]	Lu Z, Jiao W, Wang W H, Bai H Y 2014 Phys. Rev. Lett. 113 045501 Google Scholar
[39]	Qiao J C, Yao Y, Pelletier J M, Keer L M 2016 Int. J. Plast. 82 62 Google Scholar

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Evolution of defect concentration in Zr_50–_xCu₃₄Ag₈Al₈Pd_x (x = 0, 2) amorphous alloys derived using shear modulus and calorimetric data