冷速对快凝Ni50Zr50合金团簇结构遗传与演化特性的影响

doi:10.19596/j.cnki.1001-246x.8742

摘要/Abstract

摘要：

采用分子动力学方法, 模拟研究6个不同冷速下液态Ni₅₀Zr₅₀合金的快速凝固过程, 用双体分布函数、原子团类型指数、遗传跟踪等方法对快凝合金的微结构特征与演化特性进行表征和分析。结果表明: Ni₅₀Zr₅₀玻璃合金中数目最多的原子组态是Z11 Kasper团簇, 而非二十面体。快凝合金中的特征团簇趋向于聚合在一起形成中程序, 其数目随冷速的降低而增加。基本团簇的结构遗传均起始于T_m~T_g的过冷液相区, 其中Z11 Kasper团簇在T_g以上的附近温区具有最高阶段遗传分数。提高冷速有利于过冷液相区中基本团簇的阶段遗传分数增加和遗传的起始温度升高。冷速诱导的Ni₅₀Zr₅₀合金玻璃形成能力(GFA)的提高可以归因于特征团簇(如Z11 Kasper团簇)遗传能力的增强。

关键词: Ni₅₀Zr₅₀合金, 分子动力学, 冷速, 团簇, 遗传

Abstract:

Amorphous alloys have been severely restricted to widespread commercial application by their limited glass-forming ability (GFA). Since it is essentially a "freezing liquid" to some extent, studying the correlation of the atomic structures in solid with those in liquid during the rapid solidification of liquid alloys is expected to provide new insights for GFA. Therefore, the rapid solidification processes of liquid Ni₅₀Zr₅₀ alloy under six different cooling rates are simulated using molecular dynamics (MD) methods. The microstructure as well as its evolution of the rapidly solidified Ni₅₀Zr₅₀ alloys are characterized and analyzed with pair distribution function (PDF), cluster-type-index method (CTIM), and reverse atomic trajectory tracking method. The results show that the most numerous atomic configurations in Ni₅₀Zr₅₀ metallic glass is (11 2/1441 8/1551 1/1661), i.e., Z11 Kasper cluster, rather than icosahedra. The characteristic clusters in rapidly solidified Ni₅₀Zr₅₀ alloys tended to aggregate to form medium-range orders (MROs), and their numbers increase with the decrease of cooling rate. The configurational heredity of basic clusters emerges in the supercooled liquid region of T_m-T_g. Among the typical clusters, Z11 Kasper cluster possesses the highest fraction f of staged heredity in a wide temperature range above T_g. Raising cooling rate is beneficial for increasing f of basic clusters in the supercooled liquid region and increasing onset temperature of configuration heredity. The GFA of Ni₅₀Zr₅₀ alloy induced by raising cooling rate can be attributed to the enhanced hereditary ability of characteristic clusters such as Z11 Kasper cluster.

Key words: Ni₅₀Zr₅₀ alloy, molecular dynamics, cooling rate, clusters, heredity

中图分类号:

O4-39

祁青华, 文大东, 陈贝, 高明, 易洲, 邓永和, 邓科, 彭平. 冷速对快凝Ni₅₀Zr₅₀合金团簇结构遗传与演化特性的影响[J]. 计算物理, 2024, 41(4): 494-502.

Qinghua QI, Dadong WEN, Bei CHEN, Ming GAO, Zhou YI, Yonghe DENG, Ke DENG, Ping PENG. Heredity and Evolution of Cluster in Rapid Solidification of Liquid Ni₅₀Zr₅₀ Alloy under Different Cooling Rates[J]. Chinese Journal of Computational Physics, 2024, 41(4): 494-502.

图/表 8

图1 不同冷速下，300 K时快凝Ni50Zr50合金的双体分布函数(a)总双体分布函数gtot(r); (b)偏双体分布函数gαβ(r)

Fig.1 Pair distribution functions (PDFs) of rapidly solidified Ni50Zr50 alloy at 300 K for various cooling rates (a) total PDF gtot(r); (b) partial PDF gαβ(r)

表1 Ni50Zr50玻璃合金中原子间距的模拟结果与实验值的比较(T=300 K)(R: 原子间距离，ND：中子衍射，EXAFS：扩展X射线吸收精细结构)

Table 1 Comparison between simulated results and experimental values of interatomic distance in Ni50Zr50 glassy alloy (T=300 K) (R, ND, and EXAFS in Table 1 denoetes interatomic distance, neutron diffraction, and extended X-ray absorption fine structure, respectively.)

Data sources	Measuring method	(R±0.02)/Å
Data sources	Measuring method	Ni-Ni	Ni-Zr	Zr-Zr	Ni-Zr_(tot)
This work	MD	2.65	2.79	3.35	2.79
Ref.[32]	MD	2.64	2.77	3.34	2.78
Ref.[33]	EXAFS	2.63	2.62	3.31
Ref.[34]	ND	2.63	2.73	3.32

图2 不同冷速下快凝Ni50Zr50合金的(a) 平均原子总能量Etot随温度T的变化；(内插图是Etot-T曲线在650~1 050 K温度区间的放大。)(b) 约化玻璃转变温度Trg与冷速γ的关系(内插图是采用外推方法估测玻璃转变温度Tg的示意图。)

Fig.2 For rapidly solidified Ni50Zr50 alloy at different cooling rates: (a) Variation of total energy per atom Etot with T(The inner illustration shows the amplification of the Etot -T curve in the temperature range of 650-1050 K.) and (b) variation of reduced glass transition temperature Trg with cooling rate γ (The inner illustration is the glass transition temperature Tg estimated by extrapolation.)

图3 快凝Ni50Zr50合金中典型基本原子团簇的几何结构

Fig.3 Geometric structure of typical elementary clusters in rapidly solidified Ni50Zr50 alloy

图4 液态Ni50Zr50合金中典型团簇的数目(a)随温度的变化；(b)随冷速γ的变化

Fig.4 Number of typical clusters in liquid Ni50Zr50 alloy with (a) temperature and (b) cooling rates

图5 快凝Ni50Zr50合金中的中程有序(MRO) (a)MRO结构；(b)MRO数目与冷速的关系

Fig.5 Medium-range orders (MROs) in rapidly solidified Ni50Zr50 alloys (a) structure of typical MROs; (b)number of MROs with different cooling rates

图6 液态Ni50Zr50合金快凝过程中一个Z11-MRO的遗传与长大(a)T=860 K，N=2，n=18; (b)T=850 K，N=3，n=23；(c)T=730 K，N=6，n=38; (d) T=720 K，N=6，n=42; (e) T=600 K，N=6，n=35; (f) T=300 K，N=6，n=37 (紫色和白色球分别表示保持相对稳定中心原子和近邻原子，红色和青色球分别表示新增的中心原子和近邻原子；T表示温度、N表示中心原子数、n表示团簇原子总数。)

Fig.6 The heredity and growth of a Z11-MRO during the rapid solidification process of liquid Ni50Zr50 alloy (Purple and white balls represent relatively stable central and neighboring atoms, while red and cyan balls represent newly added central and neighboring atoms, respectively; T represents temperature, N represents number of central atoms, and n represents total number of cluster atoms.) (a)T=860 K, N=2, n=18; (b)T=850 K, N=3, n=23; (c)T=730 K, N=6, n=38; (d) T=720 K, N=6, n=42; (e) T=600 K, N=6, n=35; (f) T=300 K, N=6, n=37

图7 快凝Ni50Zr50合金中典型基本原子团簇的阶段遗传分数f随温度T的演化(a) γ=1×1011 K·s-1，不同团簇的f；(b)不同冷速，(11 2/1441 8/1551 1/1661)团簇的f；(c)不同冷速，(12 2/1441 8/1551 2/1661)团簇的f；(d)不同冷速，(12 12/1551)团簇的f

Fig.7 Fraction f of staged heredity for typical basic clusters in rapidly solidified Ni50Zr50 alloys with temperature (a) f of different clusters at γ=1×1011 K·s-1; (b) f of (11 2/1441 8/1551 1/1661) clusters at different γ; (c) f of (11 2/1441 8/1551 2/1661) clusters at different γ and (d) f of (12 12/1551) cluster at different γ

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冷速对快凝Ni₅₀Zr₅₀合金团簇结构遗传与演化特性的影响

Heredity and Evolution of Cluster in Rapid Solidification of Liquid Ni₅₀Zr₅₀ Alloy under Different Cooling Rates

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