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The substantial undercooling and rapid solidification of liquid quinary Zr57Cu20Al10Ni8Ti5 alloy are achieved by electromagnetic levitation (EML) technique. The amorphous solidification mechanism is revealed with molecular dynamics (MD) simulation. It is observed in EML experiment that the containerlessly solidified alloy is characterized by a core-shell structure, with mainly amorphous phase becoming the core and crystalline ZrCu, Zr2Cu and Zr8Cu5 phases forming the shell. The volume fraction of amorphous core structure increases with undercooling and attains a value up to 81.3% at the maximum experimental undercooling of 300 K, which indicates that the critical undercooling required for complete amorphous solidification is 334 K. TEM analyses show that the alloy microstructure is mainly composed of Zr8Cu5 phase, whereas the ZrCu phase and Zr2Cu phase are suppressed when liquid undercooling approaches this threshold. Once the critical undercooling is reached, amorphous solidification prevails over the crystallization of Zr8Cu5 phase. In addition, a small quantity of amorphous phases are found in the crystalline shell and a little trace of Zr8Cu5 nano-cluster is detected among the amorphous core. It is further verified by MD simulation that the formation of amorphous phase in the shell is caused by the microsegregation-induced solutal undercooling when liquid alloy attains the critical undercooling, while the nano-clusters within the core is mainly ascribed to the micro-thermal fluctuation effect inside highly undercooled liquid phase.
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Keywords:
- electromagnetic levitation /
- amorphous alloy /
- highly undercooling /
- rapid solidification /
- molecular dynamics
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图 1 电磁悬浮条件下液态五元Zr57Cu20Al10Ni8Ti5合金的深过冷与快速凝固 (a) ΔT = 200 K; (b) ΔT = 250 K; (c) ΔT = 300 K; (d) 核-壳界面形貌
Figure 1. High undercooling and rapid solidification of liqud quinary Zr57Cu20Al10Ni8Ti5 alloy under electromagnetic levitation condition: (a) ΔT = 200 K; (b) ΔT = 250 K; (c) ΔT = 300 K; (d) core-shell interface morphology.
图 2 合金的相组成与非晶核的形成 (a) XRD曲线; (b) 非晶核体积分数
Figure 2. Alloy phase constitution and amorphous core formation: (a) XRD curves; (b) volume fraction of amorphous core.
图 3 深过冷液态Zr57Cu20Al10Ni8Ti5合金快速凝固特征 (a) 冷却曲线; (b) 合金外壳的平均生长速率
Figure 3. Rapid solidification characteristics of highly undercooled liquid Zr57Cu20Al10Ni8Ti5 alloy: (a) Cooling curves; (b) alloy shell average growth rate.
图 4 液态Zr57Cu20Al10Ni8Ti5合金的微观结构特征 (a) 计算系统总能量; (b) 合金原子的扩散系数; (c)
$\langle0, 0, 12, 0\rangle $ 二十面体结构在多面体团簇中的比例Figure 4. Microstructure characteristics of highly undercooled liquid Zr57Cu20Al10Ni8Ti5 alloy: (a) Calculated system total energy; (b) calculated atom diffusion coefficient; (c) calculated
$\langle0, 0, 12, 0\rangle $ icosahedron ratio in Voronoi polyhedral clusters.
图 5 过冷液态Zr57Cu20Al10Ni8Ti5合金的形核能力 (a) 液态合金的黏度; (b)各相的形核率
Figure 5. Nucleation capability of the undercooled liquid Zr57Cu20Al10Ni8Ti5 alloy: (a) Calculated liquid alloy viscosity; (b) calculated nucleation rates of ZrCu, Zr2Cu and Zr8Cu5 phases.
图 7 过冷度250 K时Zr57Cu20Al10Ni8Ti5合金壳区的元素分布 (a) 壳区微观组织; (b) Ni元素含量; (c) Ti元素含量; (d) 总双体分布函数; (e) Zr-Ni偏双体分布函数; (f) Zr-Ti偏双体分布函数
Figure 7. Element distribution of Zr57Cu20Al10Ni8Ti5 alloy shell under 250 K undercooling: (a) Microstructure of alloy shell; (b) Ni content; (c) Ti content; (d) calculated total pair distribution function; (e) calculated Zr-Ni partial bipartite distribution function; (f) calculated Zr-Ti partial bipartite distribution function.
图 9 非晶凝固对合金平均显微硬度的影响 (a) Zr8Cu5结晶生长与非晶凝固的系统总体积; (b) Zr8Cu5结晶生长与非晶凝固的系统自由体积; (c) 非晶核平均显微硬度
Figure 9. Effect of amorphous solidification on alloy average microhardness: (a) System total volume of Zr8Cu5 crystal growth and amorphous solidification; (b) system free volume of Zr8Cu5 crystal growth and amorphous solidification; (c) average microhardness of alloy amorphous core.
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[1] Liu X F, Wang R J, Zhao D Q, Pan M X, Wang W H 2007 Appl. Phys. Lett. 91 041901
Google Scholar
[2] Sniadecki Z, Mielniczuk B, Idzikowski B, Greneche J M, Robler U K 2010 J. Appl. Phys. 108 073516
Google Scholar
[3] Zhao R, Jiang H Y, Luo P, Sun Y T, Li Z A, Wu W W, Shen L Q, Liu M, Zhao S F, Wen P, Zhang Q H, Gu L, Bai H Y, Wang W H 2020 Appl. Phys. Lett. 117 131903
Google Scholar
[4] Shao L L, Xue L, Wang Q Q, Ma K L, Huang J D, Shen B L 2021 J. Alloy. Compd. 874 159964
Google Scholar
[5] Wei B C, Zhang Y, Zhuang Y X, Zhao D Q, Pan M X, Wang W H 2001 J. Appl. Phys. 89 3529
Google Scholar
[6] Nishiyama N, Takenaka K, Miura H, Saidoh N, Zeng Y Q, Inoue A 2012 Intermetallics 30 19
Google Scholar
[7] Tang M Q, Zhang H F, Zhu Z W, Fu H M, Wang A M, Li H, Hu Z Q 2010 J. Mater. Sci. Technol. 26 481
Google Scholar
[8] Haruyama O, Watanabe T, Yuki K, Horiuchi M, Kato H, Nishiyama N 2011 Phys. Rev. B 83 064201
Google Scholar
[9] Liu C Y, Wang F, Rao F F, Hou Y 2013 J. Appl. Phys. 113 869
Google Scholar
[10] Turci F, Tarjus G, Royall C P 2017 Phys. Rev. Lett 118 215501
Google Scholar
[11] 陈季香, 周朔瑶 2014 物理学报 63 066101
Google Scholar
Chen J X, Zhou S Y 2014 Acta Phys. Sin. 63 066101
Google Scholar
[12] Guerdane M, Teichler H 2001 Phys. Rev. B 65 014203
Google Scholar
[13] Qi L, Zhang H F, Hu Z Q, Liaw P K 2004 Phys. Lett. A 327 506
Google Scholar
[14] Brillo J, Pommrich A I, Meyer A 2011 Phys. Rev. Lett. 107 165902
Google Scholar
[15] Wall J J, Weber R, Kim J, Liaw P K, Choo H 2007 Mat. Sci. Eng. A 445 219
Google Scholar
[16] Lü P, Wang H P 2017 Scripta Mater. 137 31
Google Scholar
[17] Hong S J, Chun H, Lee J, Kim B H, Seo M H, Kang J, Han B 2021 J. Phys. Chem. Lett. 12 6000
Google Scholar
[18] Yao N, Chen X, Fu Z H, Zhang Q 2022 Chem. Rev. 122 10970
Google Scholar
[19] Wang H, Zhang L F, Han J Q, E W N Deep 2018 Comput. Phys. Commun. 228 178
Google Scholar
[20] Ketkaew R, Creazzo F, Luber S 2022 J. Phys. Chem. Lett. 13 1797
Google Scholar
[21] 徐山森, 常健, 吴宇昊, 沙莎, 魏炳波 2019 物理学报 68 196401
Google Scholar
Xu S S, Chang J, Wu Y H, Sha S, Wei B B 2019 Acta Phys. Sin. 68 196401
Google Scholar
[22] Xu S S, Chang J, Sha S, Wei B 2022 Metall. Mater. Trans. A 53 762
Google Scholar
[23] Xing L Q, Ochina P 1997 Mater. Lett. 30 283
Google Scholar
[24] Baskes M I 1992 Phys. Rev. B 46 2727
Google Scholar
[25] Sun Q Q, Qin J Y, Li X X, Wang J, Pan S P 2021 J. Phase Equilib. Diff. 42 166
Google Scholar
[26] Dai Y, Li J H, Liu B X 2011 J. Appl. Phys. 109 053505
Google Scholar
[27] Garzon I L, Pasada-Amarillas A 1996 Phys. Rev. B 54 796
Google Scholar
[28] Turnbull D, Fisher J C 1949 J. Chem. Phys. 1771
Google Scholar
[29] Tsoutsouva M G, Duffar T, Chaussende D, Kamguem M 2016 J. Cryst. Growth 451 103
Google Scholar
[30] Kim T H, Gangopadhyay A K, Xing L Q, Lee G W, Shen Y T, Kelton K F, Goldman A I, Hyers R W, Rogers J R 2005 Appl. Phys. Lett. 87 251924
Google Scholar
[31] Kim S J, Kim Y H, Yang Y S 2001 Mat. Sci. Eng. A 304-306 767
Google Scholar
[32] Bondi A 1964 J. Phys. Chem. Lett. 68 441
[33] Bondi A 1966 J. Phys. Chem. C 70 3006
Google Scholar
[34] Launey M E, Kruzic J J, Li C, Busch R 2007 Appl. Phys. Lett. 91 51913
Google Scholar
[35] 周边, 杨亮 2020 物理学报 69 116101
Google Scholar
Zhou B, Yang L 2020 Acta Phys. Sin. 69 116101
Google Scholar
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