Metallic glasses (MGs) are one of the most attractive topics in the field of condensed physics and materials science because of their unique structure and excellent properties. As a metastable material, MGs tend to present a transition toward a more stable low-energy state under applied stress or high-temperature, known as aging or structural relaxation, accompanied by a decrease in deformability at room temperature. Rejuvenation of MGs is a converse process of aging/relaxation, which transforms the materials to their previous and higher-energy states. Rejuvenation greatly expands the energy range of MGs, which not only significantly improves the deformation capability of MGs, but also provides a new opportunity to explore the atomic structure, glass transition, and deformation mechanisms of MGs. This article reviews the recent progress in the study of rejuvenation, including the methods of rejuvenation of MGs, the effect of rejuvenation behavior on microstructures, mechanical properties, and functional characteristics. Finally, a brief outlook on the study of the rejuvenation behavior of MGs is presented.
Fig.1 Schematic of aging/relaxation and rejuvenation process in metallic glasses (MGs) drawn according to Ref.[12] (MGs with various glassy states, such as states A, B, C, …, G, could be obtained through different cooling rates. Rejuvenation is the transition process of MGs from lower to higher energy states (from II to I, as indicated by red arrow), while aging/structure relaxation is the transition process from higher to lower energy states (from I to II, as indicated by blue arrow). Tk stands for the finite temperature at which the deepest basins of the landscape are explored. Insets a and b show the typical atomic structures of MGs with high energy and low energy states, respectively)
Fig.2 Schematic of the composite structure in MGs after inhomogeneous deformation (The deformed MG can be considered as the composite of shear band and undeformed MG matrix)
Fig.3 Rejuvenation of bulk metallic glass (BMG) through triaxial compression[63]
Fig.4 Radial distribution function (RDF) analysis of as-cast and rejuvenated Zr64.13Cu15.75Ni10.12Al10 MGs[75] (r—distance from the reference atom)
Fig.5 Strain-hardening behavior in highly rejuvenated BMG[75]
Fig.6 Degradation efficiency of Fe-based MG powders with two energy states (i.e., gas-atomized (GA) and ball milled (BM) powders) in degrading organic water contaminants[102]
1
Klement W, Willens R H, Duwez P. Non-crystalline structure in solidified gold-silicon alloys [J]. Nature, 1960, 187: 869
2
Johnson W L. Bulk glass-forming metallic alloys: Science and technology [J]. MRS Bull., 1999, 24: 42
3
Inoue A. Stabilization of metallic supercooled liquid and bulk amorphous alloys [J]. Acta Mater., 2000, 48: 279
4
Wang W H, Dong C, Shek C H. Bulk metallic glasses [J]. Mater. Sci. Eng., 2004, R44: 45
5
Greer A L. Metallic glasses...on the threshold [J]. Mater. Today, 2009, 12: 14
6
Lu K, Lu L, Suresh S. Strengthening materials by engineering coherent internal boundaries at the nanoscale [J]. Science, 2009, 324: 349
7
Turnbull D, Cohen M H. Free-volume model of the amorphous phase: Glass transition [J]. J. Chem. Phys., 1961, 34: 120
8
Spaepen F. A microscopic mechanism for steady state inhomogeneous flow in metallic glasses [J]. Acta Metall., 1977, 25: 407
9
Wang W H. The elastic properties, elastic models and elastic perspectives of metallic glasses [J]. Prog. Mater. Sci., 2012, 57: 487
10
Debenedetti P G, Stillinger F H. Supercooled liquids and the glass transition [J]. Nature, 2001, 410: 259
11
Sun Y H, Concustell A, Greer A L. Thermomechanical processing of metallic glasses: Extending the range of the glassy state [J]. Nat. Rev. Mater., 2016, 1: 16039
12
Parisi G, Sciortino F. Structural glasses: Flying to the bottom [J]. Nat. Mater., 2013, 12: 94
13
Tong Y, Iwashita T, Dmowski W, et al. Structural rejuvenation in bulk metallic glasses [J]. Acta Mater., 2015, 86: 240
14
Ketov S V, Sun Y H, Nachum S, et al. Rejuvenation of metallic glasses by non-affine thermal strain [J]. Nature, 2015, 524: 200
15
Hufnagel T C. Cryogenic rejuvenation [J]. Nat. Mater., 2015, 14: 867
16
Guo W, Saida J, Zhao M, et al. Non-thermal crystallization process in heterogeneous metallic glass upon deep cryogenic cycling treatment [J]. J. Mater. Sci., 2019, 54: 8778
17
Kang S J, Cao Q P, Liu J, et al. Intermediate structural state for maximizing the rejuvenation effect in metallic glass via thermo-cycling treatment [J]. J. Alloys Compd., 2019, 795: 493
18
Guo W, Saida J, Zhao M, et al. Unconspicuous rejuvenation of a Pd-based metallic glass upon deep cryogenic cycling treatment [J]. Mater. Sci. Eng., 2019, A759: 59
19
Sohrabi S, Ri M C, Jiang H Y, et al. Prominent role of chemical heterogeneity on cryogenic rejuvenation and thermomechanical properties of La-Al-Ni metallic glass [J]. Intermetallics, 2019, 111: 106497
20
Guo W, Shao Y M, Saida J, et al. Rejuvenation and plasticization of Zr-based bulk metallic glass with various Ta content upon deep cryogenic cycling [J]. J. Alloys Compd., 2019, 795: 314
21
Guo W, Saida J, Zhao M, et al. Rejuvenation of Zr-based bulk metallic glass matrix composite upon deep cryogenic cycling [J]. Mater. Lett., 2019, 247: 135
22
Gu J L, Luan H W, Zhao S F, et al. Unique energy-storage behavior related to structural heterogeneity in high-entropy metallic glass [J]. Mater. Sci. Eng., 2020, A786: 139417
23
Ketov S V, Trifonov A S, Ivanov Y P, et al. On cryothermal cycling as a method for inducing structural changes in metallic glasses [J]. NPG Asia Mater., 2018, 10: 137
24
Liu W H, Sun B A, Gleiter H, et al. Nanoscale structural evolution and anomalous mechanical response of nanoglasses by cryogenic thermal cycling [J]. Nano Lett., 2018, 18: 4188
25
Li B S, Xie S H, Kruzic J J. Toughness enhancement and heterogeneous softening of a cryogenically cycled Zr-Cu-Ni-Al-Nb bulk metallic glass [J]. Acta Mater., 2019, 176: 278
26
Saida J, Yamada R, Wakeda M. Recovery of less relaxed state in Zr-Al-Ni-Cu bulk metallic glass annealed above glass transition temperature [J]. Appl. Phys. Lett., 2013, 103: 221910
27
Wakeda M, Saida J, Li J, et al. Controlled rejuvenation of amorphous metals with thermal processing [J]. Sci. Rep., 2015, 5: 10545
28
Küchemann S, Derlet P M, Liu C Y, et al. Energy storage in metallic glasses via flash annealing [J]. Adv. Funct. Mater., 2018, 28: 1805385
29
Kosiba K, Şopu D, Scudino S, et al. Modulating heterogeneity and plasticity in bulk metallic glasses: Role of interfaces on shear banding [J]. Int. J. Plast., 2019, 119: 156
30
Xiao Q R, Huang L P, Shi Y F. Suppression of shear banding in amorphous ZrCuAl nanopillars by irradiation [J]. J. Appl. Phys., 2013, 113: 083514
31
Raghavan R, Boopathy K, Ghisleni R, et al. Ion irradiation enhances the mechanical performance of metallic glasses [J]. Scr. Mater., 2010, 62: 462
32
Heo J, Kim S, Ryu S, et al. Delocalized plastic flow in proton-irradiated monolithic metallic glasses [J]. Sci. Rep., 2016, 6: 23244
33
Sun K, Wang G, Wang Y W, et al. Structural rejuvenation and relaxation of a metallic glass induced by ion irradiation [J]. Scr. Mater., 2020, 180: 34
34
Magagnosc D J, Kumar G, Schroers J, et al. Effect of ion irradiation on tensile ductility, strength and fictive temperature in metallic glass nanowires [J]. Acta Mater., 2014, 74: 165
35
Bian X L, Wang G, Chen H C, et al. Manipulation of free volumes in a metallic glass through Xe-ion irradiation [J]. Acta Mater., 2016, 106: 66
36
Fu C C, Dalla Torre J, Willaime F, et al. Multiscale modelling of defect kinetics in irradiated iron [J]. Nat. Mater., 2005, 4: 68
37
Baumer R E, Demkowicz M J. Radiation response of amorphous metal alloys: Subcascades, thermal spikes and super-quenched zones [J]. Acta Mater., 2015, 83: 419
38
Zhao L, Chan K C, Chen S H, et al. Tunable tensile ductility of metallic glasses with partially rejuvenated amorphous structures [J]. Acta Mater., 2019, 169: 122
39
Wang C, Yang Z Z, Ma T, et al. High stored energy of metallic glasses induced by high pressure [J]. Appl. Phys. Lett., 2017, 110: 111901
40
Liu M, Jiang H Y, Liu X Z, et al. Energy state and properties controlling of metallic glasses by surface rejuvenation [J]. Intermetallics, 2019, 112: 106549
41
Küchemann S, Maaß R. Gamma relaxation in bulk metallic glasses [J]. Scr. Mater., 2017, 137: 5
42
Greer A L, Sun Y H. Stored energy in metallic glasses due to strains within the elastic limit [J]. Philos. Mag., 2016, 96: 1643
43
Park K W, Lee C M, Wakeda M, et al. Elastostatically induced structural disordering in amorphous alloys [J]. Acta Mater., 2008, 56: 5440
44
Lee J C. Calorimetric study of β-relaxation in an amorphous alloy: An experimental technique for measuring the activation energy for shear transformation [J]. Intermetallics, 2014, 44: 116
45
Ross P, Küchemann S, Derlet P M, et al. Linking macroscopic rejuvenation to nano-elastic fluctuations in a metallic glass [J]. Acta Mater., 2017, 138: 111
46
Wang Y M, Zhang M, Liu L. Mechanical annealing in the homogeneous deformation of bulk metallic glass under elastostatic compression [J]. Scr. Mater., 2015, 102: 67
47
Priezjev N V. Aging and rejuvenation during elastostatic loading of amorphous alloys: A molecular dynamics simulation study [J]. Comput. Mater. Sci., 2019, 168: 125
48
Lou Y, Liu X, Yang X L, et al. Fast rejuvenation in bulk metallic glass induced by ultrasonic vibration precompression [J]. Intermetallics, 2020, 118: 106687
49
Sohrabi S, Li M X, Bai H Y, et al. Energy storage oscillation of metallic glass induced by high-intensity elastic stimulation [J]. Appl. Phys. Lett., 2020, 116: 081901
50
Wang D P, Yang Y, Niu X R, et al. Resonance ultrasonic actuation and local structural rejuvenation in metallic glasses [J]. Phys. Rev., 2017, 95B: 235407
51
Meng F Q, Tsuchiya K, Ii S, et al. Reversible transition of deformation mode by structural rejuvenation and relaxation in bulk metallic glass [J]. Appl. Phys. Lett., 2012, 101: 121914
52
Qiang J, Tsuchiya K. Composition dependence of mechanically-induced structural rejuvenation in Zr-Cu-Al-Ni metallic glasses [J]. J. Alloys Compd., 2017, 712: 250
53
Dmowski W, Yokoyama Y, Chuang A, et al. Structural rejuvenation in a bulk metallic glass induced by severe plastic deformation [J]. Acta Mater., 2010, 58: 429
54
González S, Fornell J, Pellicer E, et al. Influence of the shot-peening intensity on the structure and near-surface mechanical properties of Ti40Zr10Cu38Pd12 bulk metallic glass [J]. Appl. Phys. Lett., 2013, 103: 211907
55
Concustell A, Méar F O, Suriñach S, et al. Structural relaxation and rejuvenation in a metallic glass induced by shot-peening [J]. Philos. Mag. Lett., 2009, 89: 831
56
Meylan C M, Orava J, Greer A L. Rejuvenation through plastic deformation of a La-based metallic glass measured by fast-scanning calorimetry [J]. J. Non-Cryst. Solids, 2020, 8X: 100051
57
Louzguine-Luzgin D V, Ketov S V, Wang Z, et al. Plastic deformation studies of Zr-based bulk metallic glassy samples with a low aspect ratio [J]. Mater. Sci. Eng., 2014, A616: 288
58
Haruyama O, Kisara K, Yamashita A, et al. Characterization of free volume in cold-rolled Zr55Cu30Ni5Al10 bulk metallic glasses [J]. Acta Mater., 2013, 61: 3224
59
Pan J, Chen Q, Liu L, et al. Softening and dilatation in a single shear band [J]. Acta Mater., 2011, 59: 5146
60
Bei H, Xie S, George E P. Softening caused by profuse shear banding in a bulk metallic glass [J]. Phys. Rev. Lett., 2006, 96: 105503
61
Liu J W, Cao Q P, Chen L Y, et al. Shear band evolution and hardness change in cold-rolled bulk metallic glasses [J]. Acta Mater., 2010, 58: 4827
62
Jiang W H, Pinkerton F E, Atzmon M. Deformation-induced nanocrystallization: A comparison of two amorphous Al-based alloys [J]. J. Mater. Res., 2005, 20: 696
63
Pan J, Wang Y X, Guo Q, et al. Extreme rejuvenation and softening in a bulk metallic glass [J]. Nat. Commun., 2018, 9: 560
64
Pan J, Wang Y X, Li Y. Ductile fracture in notched bulk metallic glasses [J]. Acta Mater., 2017, 136: 126
65
Pan J, Zhou H F, Wang Z T, et al. Origin of anomalous inverse notch effect in bulk metallic glasses [J]. J. Mech. Phys. Solids, 2015, 84: 85
66
Dong J, Feng Y H, Huan Y, et al. Rejuvenation in hot-drawn micrometer metallic glassy wires [J]. Chin. Phys. Lett., 2020, 37: 017103
67
Ma Y B, Wang B Z, Zhang Q D, et al. Change dynamic behaviors by heightening its stored energy of monolithic bulk metallic glass [J]. Mater. Des., 2019, 181: 107971
68
Tong Y, Dmowski W, Bei H, et al. Mechanical rejuvenation in bulk metallic glass induced by thermo-mechanical creep [J]. Acta Mater., 2018, 148: 384
69
Tong Y, Dmowski W, Yokoyama Y, et al. Recovering compressive plasticity of bulk metallic glasses by high-temperature creep [J]. Scr. Mater., 2013, 69: 570
70
Ding G, Li C, Zaccone A, et al. Ultrafast extreme rejuvenation of metallic glasses by shock compression [J]. Sci. Adv., 2019, 5: eaaw6249
71
Song K K, Pauly S, Zhang Y, et al. Significant tensile ductility induced by cold rolling in Cu47.5Zr47.5Al5 bulk metallic glass [J]. Intermetallics, 2011, 19: 1394
72
Yavari A R, Le Moulec A, Inoue A, et al. Excess free volume in metallic glasses measured by X-ray diffraction [J]. Acta Mater., 2005, 53: 1611
73
Zhu F, Hirata A, Liu P, et al. Correlation between local structure order and spatial heterogeneity in a metallic glass [J]. Phys. Rev. Lett., 2017, 119: 215501
74
Zhu F, Song S X, Reddy K M, et al. Spatial heterogeneity as the structure feature for structure-property relationship of metallic glasses [J]. Nat. Commun., 2018, 9: 3965
75
Pan J, Ivanov Y P, Zhou W H, et al. Strain-hardening and suppression of shear-banding in rejuvenated bulk metallic glass [J]. Nature, 2020, 578: 559
76
Sarac B, Gammer C, Deng L, et al. Elastostatic reversibility in thermally formed bulk metallic glasses: Nanobeam diffraction fluctuation electron microscopy [J]. Nanoscale, 2018, 10: 1081
77
Hilke S, Rösner H, Geissler D, et al. The influence of deformation on the medium-range order of a Zr-based bulk metallic glass characterized by variable resolution fluctuation electron microscopy [J]. Acta Mater., 2019, 171: 275
78
Jiang S Q, Huang Y, Li M Z. Structural evolution in deformation-induced rejuvenation in metallic glasses: A cavity perspective [J]. Chin. Phys., 2019, 28B: 046103
79
Feng S D, Chan K C, Zhao L, et al. Rejuvenation by weakening the medium range order in Zr46Cu46Al8 metallic glass with pressure preloading: A molecular dynamics simulation study [J]. Mater. Des., 2018, 158: 248
80
Ge T P, Wang C, Tan J, et al. Unusual energy state evolution in Ce-based metallic glass under high pressure [J]. J. Appl. Phys., 2017, 121: 205109
81
Greer A L, Cheng Y Q, Ma E. Shear bands in metallic glasses [J]. Mater. Sci. Eng., 2013, R74: 71
82
Lewandowski J J, Wang W H, Greer A L. Intrinsic plasticity or brittleness of metallic glasses [J]. Philos. Mag. Lett., 2005, 85: 77
83
Chen L Y, Setyawan A D, Kato H, et al. Free-volume-induced enhancement of plasticity in a monolithic bulk metallic glass at room temperature [J]. Scr. Mater., 2008, 59: 75
84
Di S Y, Wang Q Q, Zhou J, et al. Enhancement of plasticity for FeCoBSiNb bulk metallic glass with superhigh strength through cryogenic thermal cycling [J]. Scr. Mater., 2020, 187: 13
85
Song W L, Meng X H, Wu Y, et al. Improving plasticity of the Zr46Cu46Al8 bulk metallic glass via thermal rejuvenation [J]. Sci. Bull., 2018, 63: 840
86
Bian X L, Zhao D, Kim J T, et al. Controlling the distribution of structural heterogeneities in severely deformed metallic glass [J]. Mater. Sci. Eng., 2019, A752: 36
87
Ebner C, Pauly S, Eckert J, et al. Effect of mechanically induced structural rejuvenation on the deformation behaviour of CuZr based bulk metallic glass [J]. Mater. Sci. Eng., 2020, A773: 138848
88
Denis P, Meylan C M, Ebner C, et al. Rejuvenation decreases shear band sliding velocity in Pt-based metallic glasses [J]. Mater. Sci. Eng., 2017, A684: 517
89
Dieter G E. Mechanical Metallurgy [M]. New York: McGraw-Hill, 1961: 1
90
Schuh C A, Hufnagel T C, Ramamurty U. Mechanical behavior of amorphous alloys [J]. Acta Mater., 2007, 55: 4067
91
Wu Y, Xiao Y H, Chen G L, et al. Bulk metallic glass composites with transformation-mediated work-hardening and ductility [J]. Adv. Mater., 2010, 22: 2770
92
Lee J C, Kim Y C, Ahn J P, et al. Deformation-induced nanocrystallization and its influence on work hardening in a bulk amorphous matrix composite [J]. Acta Mater., 2004, 52: 1525
93
Jang D C, Greer J R. Transition from a strong-yet-brittle to a stronger-and-ductile state by size reduction of metallic glasses [J]. Nat. Mater., 2010, 9: 215
94
Chen D Z, Gu X W, An Q, et al. Ductility and work hardening in nano-sized metallic glasses [J]. Appl. Phys. Lett., 2015, 106: 061903
95
Wang Z T, Pan J, Li Y, et al. Densification and strain hardening of a metallic glass under tension at room temperature [J]. Phys. Rev. Lett., 2013, 111: 135504
96
Taylor G I. The mechanism of plastic deformation of crystals. Part I. -Theoretical [J]. Proc. Roy. Soc., 1934, 145A: 362
97
Demetriou M D, Launey M E, Garrett G, et al. A damage-tolerant glass [J]. Nat. Mater., 2011, 10: 123
98
Grell D, Dabrock F, Kerscher E. Cyclic cryogenic pretreatments influencing the mechanical properties of a bulk glassy Zr-based alloy [J]. Fatigue Fract. Eng. Mater. Struct., 2018, 41: 1330
99
Ketkaew J, Yamada R, Wang H, et al. The effect of thermal cycling on the fracture toughness of metallic glasses [J]. Acta Mater., 2020, 184: 100
100
Zhang L C, Jia Z, Lyu F, et al. A review of catalytic performance of metallic glasses in wastewater treatment: Recent progress and prospects [J]. Prog. Mater. Sci., 2019, 105: 100576
101
Wang Z J, Li M X, Yu J H, et al. Low-iridium-content IrNiTa metallic glass films as intrinsically active catalysts for hydrogen evolution reaction [J]. Adv. Mater., 2020, 32: 1906384
102
Wang J Q, Liu Y H, Chen M W, et al. Rapid degradation of azo dye by Fe-based metallic glass powder [J]. Adv. Funct. Mater., 2012, 22: 2567
103
Wang J Q, Liu Y H, Chen M W, et al. Excellent capability in degrading azo dyes by MgZn-based metallic glass powders [J]. Sci. Rep., 2012, 2: 418
104
Lv Z W, Yan Y Q, Yuan C C, et al. Making Fe-Si-B amorphous powders as an effective catalyst for dye degradation by high-energy ultrasonic vibration [J]. Mater. Des., 2020, 194: 108876
105
Miao F, Wang Q Q, Di S Y, et al. Enhanced dye degradation capability and reusability of Fe-based amorphous ribbons by surface activation [J]. J. Mater. Sci. Technol., 2020, 53: 163
106
Zhang C Q, Sun Q L. Annealing-induced different decolorization performances of Fe-Mo-Si-B amorphous alloys [J]. J. Non-Cryst. Solids, 2017, 470: 93
107
Zheng H, Zhu L, Jiang S S, et al. Recovering the bending ductility of the stress-relieved Fe-based amorphous alloy ribbons by cryogenic thermal cycling [J]. J. Alloys Compd., 2019, 790: 529
108
Ri M C, Sohrabi S, Ding D W, et al. Serrated magnetic properties in metallic glass by thermal cycle [J]. Chin. Phys., 2017, 26B: 066101
109
Gu J, Shao Y, Shi L, et al. Novel corrosion behaviours of the annealing and cryogenic thermal cycling treated Ti-based metallic glasses [J]. Intermetallics, 2019, 110: 106467
110
Li S B, Lan F J, Chen S Y, et al. Bulk intrinsic heterogeneity of metallic glasses probed by Meissner effect [J]. Intermetallics, 2020, 119: 106721
111
Zhong L, Wang J W, Sheng H W, et al. Formation of monatomic metallic glasses through ultrafast liquid quenching [J]. Nature, 2014, 512: 177
112
Yu H B, Luo Y S, Samwer K. Ultrastable metallic glass [J]. Adv. Mater., 2013, 25: 5904
113
Lüttich M, Giordano V M, Le Floch S, et al. Anti-aging in ultrastable metallic glasses [J]. Phys. Rev. Lett., 2018, 120: 135504
114
Yamada R, Tanaka N, Guo W, et al. Crystallization behavior of thermally rejuvenated Zr50Cu40Al10 metallic glass [J]. Mater. Trans., 2017, 58: 1463
115
Zhou H B, Hilke S, Pineda E, et al. X-ray photon correlation spectroscopy revealing the change of relaxation dynamics of a severely deformed Pd-based bulk metallic glass [J]. Acta Mater., 2020, 195: 446
