高压下金属钽液体中拓扑密堆团簇对凝固路径的影响规律

莫云飞; 蒋丽贵; 稂林; 文大东; 张海涛; 李媛; 田泽安; 彭平; 刘让苏

doi:10.7498/aps.73.20241089

摘要

金属液体(或过冷液体)中的主要微观结构对最终的凝固路径(晶化或非晶化)起着决定性作用, 何种微观结构将扮演关键性角色一直处在不断的被探索和研究中. 本文采用分子动力学方法模拟研究金属钽(tantalum, Ta)液体在不同压强下的快速凝固过程, 通过原子平均能量、双体分布函数和最大标准团簇分析方法, 对凝固过程中的微观结构演变进行量化分析. 研究结果表明, 相比于低含量的二十面体, 拓扑密堆(topologically close-packed, TCP)团簇在金属Ta液体中扮演着关键角色, 它不仅含量更高, 而且更能对凝固路径起决定性作用. 当压强P∈[0, 8.75] GPa时, 金属Ta液体中的TCP团簇不仅处于能量低且稳定性好的状态, 同时TCP团簇相互连结程度高而不容易被分解, 从而促进金属Ta液体发生非晶转变; 当压强P∈[9.375, 50] GPa时, 金属Ta液体中TCP团簇处于亚稳定状态, 且很多高能量的TCP团簇在液固转变过程中容易转变成其他团簇, 此时体心立方(body-centered cubic, BCC)晶胚容易在TCP团簇堆积稀疏区域形核和长大, 最终金属Ta液体转变成比较完美的BCC晶体.

关键词:

Abstract

The main microstructures in metallic liquids (or supercooled liquids) play a decisive role in determining the final solidification pathway (crystallization or amorphization). However, what kind of microstructure plays a critical role is constantly explored and studied by scholars. Some of previous theoretical and experimental studies have suggested that icosahedron (ICO) clusters (or ICO short-range order) in metallic liquids possess lower energy than their corresponding crystals, and high abundance of ICO clusters can increase the nucleation barriers and promote amorphous transformation. Current research results indicate that the content of various clusters (especially ICO clusters) in many metallic liquids is relatively low. Therefore, it is significant to identify which microstructure plays a critical role in metallic liquids.In this work, the rapid solidification processes of tantalum (Ta) metallic liquid under various pressure conditions are investigated by using molecular dynamic (MD) simulation, and the microstructure evolutions in different solidification processes are quantitatively analyzed through the average atomic energy, pair distribution function, and largest standard cluster analysis (LaSCA). The results show that, compared with the cluster with low content of ICO, topologically close-packed (TCP) clusters are not only more abundant but also play a more decisive role in determining the solidification path of Ta metallic liquids. At a pressure P∈[0, 8.75] GPa, the TCP clusters in Ta metallic liquid not only exhibit low energy and a highly stable state, but also are highly interconnected with each other and resist decomposition, thereby promoting the amorphous transformation of the Ta metallic liquid. At pressure P∈[9.375, 50] GPa, the TCP clusters in Ta metallic liquid are in a metastable state, many TCP clusters with high energy state can easily transform into other clusters in the liquid-solid transition process. In this stage, nucleation and growth of the body-centered cubic (BCC) embryo occur mainly in areas where TCP clusters are stacked sparsely, eventually Ta metallic liquid forms a perfect BCC crystal .

Keywords:

作者及机构信息

1.
长沙学院电子信息与电气工程学院和机电工程学院, 长沙　410022

2.
湖南理工学院物理与电子科学学院, 岳阳　414000

3.
湖南工程学院计算科学与电子学院, 湘潭　411104

4.
湖南女子学院信息科学与工程学院, 长沙　410004

5.
湖南大学材料科学与工程学院, 长沙　410082

通信作者: 稂林, 12020013@hnist.edu.cn

基金项目: 国家自然科学基金(批准号: 12004053)和湖南省教育厅重点和一般研究基金(批准号: 23A0492, 22C0581)资助的课题.

Authors and contacts

1.
School of Electronic Information and Electrical Engineering, School of Mechanical and Electrical Engineering, Changsha University, Changsha 410022, China

2.
School of Physics and Electrical Science, Hunan Institute of Science and Technology, Yueyang 414000, China

3.
School of Computational Science & Electronics, Hunan Institute of Engineering, Xiangtan 411104, China

4.
College of Information Science and Engineering, Hunan Woman's University, Changsha 410004, China

5.
School of Materials Science and Engineering, Hunan University, Changsha 410082, China

Corresponding author: Lang Lin, 12020013@hnist.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 12004053) and the Scientific Research Fund of Education Department of Hunan Province, China (Grant Nos. 23A0492, 22C0581).

文章全文

参考文献

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施引文献

图 1 BCC和某一类TCP团簇的拓扑结构　(a) 中心原子标号为9655的BCC最大标准团簇; (b) 由根对原子(标号: 9655与5676)与4个共有近邻原子构成的共有近邻子团簇444; (c)图(b)中4个共有近邻原子的拓扑结构; (d), (e)分别表示图(a)中的另一类共有近邻子团簇666和6个共有近邻原子的拓扑结构; (f) 中心原子标号为9875的TCP最大标准团簇; (g), (i)分别表示图(f)中两类共有近邻子团簇555和666; (h), (j) 分别表示图(g)和(i)中共有近邻原子的拓扑结构

Fig. 1. Topology of BCC and one kind of TCP clusters: (a) A BCC LaSC with a central atom (9655); (b) a CNS of 444 composed of an interconnected root pair (9655 and 5676) and 4 CNNs; (c) the topology of 4 CNNs in panel (b); (d), (e) another CNS of 666 and the topology of 6 CNNs respectively; (f) a TCP LaSC with a central atom (9875); (g), (i) another two CNS of 555 and 666 respectively; (h), (j) the topology of CNNs in panel (g) and (i) respectively.

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图 2 不同压强下系统的原子平均势能量随温度的关系

Fig. 2. Average atomic potential energy of system dependence of the temperature under different pressure.

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图 3 S(q)和g(r)曲线随温度的演变关系　(a) 0 GPa下的S(q)曲线; (b), (c) 5 GPa和30 GPa下的g(r)曲线; (d) 100 K时g(r)曲线随压强的演变关系

Fig. 3. S(q) and g(r) curves as a function of temperature: (a) S(q) curves under 0 GPa; (b), (c) the g(r) curves under 5 GPa and 30 GPa respectively; (d) g(r) curves dependence of pressure at 100 K.

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图 4 共有近邻子团簇CNS的百分比与温度的关系　(a) 5 GPa; (b) 30 GPa

Fig. 4. Percentage of CNS dependence of temperature: (a) 5 GPa; (b) 30 GPa.

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图 5 不同压强下且100 K时CNS的百分含量分布图　(a), (c) 555, 544和433; (b), (d) 444和666

Fig. 5. At 100 K, the distribution figure for the percentage of the CNS under different pressure: (a), (c) 555, 544 and 433; (b), (d) 444 and 666.

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图 6 主要LaSC百分比在凝固过程中的演变　(a) 5 GPa; (b) 30 GPa; (c) 9.375—50 GPa 下BCC 晶体团簇百分比在凝固过程的演变及对比

Fig. 6. Percentage of several main LaSCs as a function temperature: (a) 5 GPa; (b) 30 GPa; (c) evolution and comparison of the percentage of BCC crystal clusters during the solidification process under pressure P∈[9.375, 50] GPa.

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图 7 压强为5 GPa和30 GPa时, (a) TCP团簇和BCC团簇百分比与温度的关系, 以及(b) TCP原子和BCC原子的平均势能与温度的关系

Fig. 7. (a) Percentage of TCP and BCC LaSC dependence of temperature; (b) the average atomic potential energy of TCP and BCC atoms dependence of temperature. The pressure is 5 GPa and 30 GPa

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图 8 选定温度下TCP原子和BCC原子的三维空间分布图　(a)—(d) 5 GPa; (e)—(h) 30 GPa; 白色原子代表TCP原子, 蓝色原子代表BCC原子

Fig. 8. Snapshots of the samples at selected temperatures for TCP and BCC atoms: (a)–(d) 5 GPa; (e)–(h) 30 GPa. Colour configuration: white and blue balls represent TCP and BCC atoms, respectively.

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下载: 全尺寸图片幻灯片

map

[1]	Wang H P, Liao H, Hu L, Zheng C H, Chang J, Liu D N, Li M X, Zhao J F, Xie W J, Wei B B 2024 Adv. Mater. 36 2313162 Google Scholar
[2]	Wang Q, Zhai B, Wang H P, Wei B 2021 J. Appl. Phys. 130 185103 Google Scholar
[3]	Wang H P, Li M X, Zou P F, Cai X, Hu L, Wei B B 2018 Phys. Rev. B. 98 063106 Google Scholar
[4]	Zou P F, Wang H P, Yang S J, Hu L, Wei B B 2018 Metall. Mater. Trans. A 49 5488 Google Scholar
[5]	陈长军, 张超, 王晓南, 张敏, 敬和民 2014 热加工工艺 43 5 Google Scholar Chen C J, Zhang C, Wang X N, Zhang M, Jing H M 2014 Hot Working Technology 43 5 Google Scholar
[6]	何季麟, 张学清, 杨国启, 郑爱国 2014 中国材料进展 33 545 Google Scholar He J L, Zhang X Q, Yang Q G, Zheng A G 2014 Mater. China 33 545 Google Scholar
[7]	张嘉祺, 巩琛, 冯典英, 黄辉, 李颖, 李本涛 2024 山东化工 53 94 Google Scholar Zhang J Y, Gong C, Feng D Y, Huang H, Li Y, Li B T 2024 Shandong Chem. Industry 53 94 Google Scholar
[8]	Gladczuk L, Patel A, Demaree J D, Sosnowski M 2005 Thin Solid Films 476 295 Google Scholar
[9]	Marcus R B, Quigley S 1968 Thin Solid Films 2 467 Google Scholar
[10]	Read M H, Altman C 1965 Appl. Phys. Lett. 7 51 Google Scholar
[11]	Janish M T, Kotula P G, Boyce B L, Carter C B 2015 J. Mater. Sci. 50 3706 Google Scholar
[12]	Moriarty J A, Belak J F, Rudd R E, Soderlind P, Streitz F H, Yang L H 2002 J. Phys. Condens. Mater. 14 2825 Google Scholar
[13]	Moriarty J A 1990 Phys. Rev. B 42 1609 Google Scholar
[14]	Moriarty J A 1994 Phys. Rev. B 49 12431 Google Scholar
[15]	Moriarty J A, Benedict L X, Glosli J N, Hood R Q, Orlikowski D A, Patel M V, Soderlind P, Streitz F H, Tang M J, Yang L H 2006 J. Mater. Res. 21 563 Google Scholar
[16]	Zhong L, Wang J W, Sheng H W, Zhang Z, Mao S X 2014 Nature 512 177 Google Scholar
[17]	Frank F C 1952 Proc. R. Soc. Lond. A 215 43 Google Scholar
[18]	Kelton K, Gangopadhyay A K, Kim T H, Lee G W 2006 J. Non. Cryst. Solid 352 5318 Google Scholar
[19]	Schenk T, Holland-Moritz D, Simonet V, Bellissent R, Herlach D 2002 Phys. Rev. Lett. 89 075507 Google Scholar
[20]	Zhang J C, Chen C, Pei Q X, Zhang W X, Sha Z D 2015 Mater. Des. 77 1 Google Scholar
[21]	Chen L Y, Mohr M, Wunderlich R K, Fecht H J, Wang X D, Cao Q P, Zhang D X, Jiang J Z 2019 J. Mol. Liq. 293 111544 Google Scholar
[22]	Sheng H W, Ma E, Kramer M J 2012 JOM 64 856 Google Scholar
[23]	Sheng H W, Luo W K, Alamgir F M, Bai J M, Ma E 2006 Nature 439 419 Google Scholar
[24]	彭超, 李媛, 邓永和, 彭平 2017 金属学报 53 1659 Google Scholar Peng C, Li Y, Deng Y H, Peng P 2017 Acta Metall. Sin. 53 1659 Google Scholar
[25]	Angell C A 1995 Science 267 1924 Google Scholar
[26]	Berthier L, Biroli G 2011 Rev. Mod. Phys. 83 587 Google Scholar
[27]	Liu Z L, Cai L C, Chen X R, Jing F Q 2008 Phys. Rev. B. 77 024103 Google Scholar
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[29]	Katagiri K, Ozaki N, Ohmura S, Albertazzi B, Hironaka Y, Inubushi Y, Ishida K, Koenig M, Miyanishi K, Nakamura H, Nishikino M, Okuchi T, Sato T 2021 Phys. Rev. Lett. 126 175503 Google Scholar
[30]	Wu Z Z, Mo Y F, Lang L, Yu A B, Xie Q, Liu R S, Tian Z A 2018 Phys. Chem. Chem. Phys 20 28088 Google Scholar
[31]	Tian Z A, Zhang Z Y, Jiang X, Wei F, Ping S, Wu F 2023 Metals 13 415 Google Scholar
[32]	Mo Y F, Tian Z A, Zhou L L, Liang Y C, Dong K J, Zhang X F, Zhang H T, Peng P, Liu R S 2024 Chem. Phys. 581 112238 Google Scholar
[33]	Mōller J, Schottelius A, Caresana M, Boesenberg U, Kim C, Dallari F, Ezquerra T A, Fernández J M, Gelisio L, Glaesener A, Goy C, Hallmann J, Kalinin A, Kurta R P 2024 Phys. Rev. Lett. 132 206102 Google Scholar
[34]	Plimpton S 1995 J. Comput. Phys. 117 1 Google Scholar
[35]	Martyna G J, Tobias D J, Klein M L 1994 J. Chem. Phys. 101 4177 Google Scholar
[36]	https://sites.google. com/site/eampotentials/ta [2024-8-3]
[37]	Mo Y F, Tian Z A, Lang L, Zhou L L, Liang Y C, Zhang H T, Liu R S, Peng P, Wen D D 2020 Phy. Chem. Chem. Phys. 22 18078 Google Scholar
[38]	文大冬, 祁青华, 黄欣欣, 易洲, 邓永和, 田泽安, 彭平 2020 69 196101 Google Scholar We D D, Deng Y H, Dai X Y, Wu A R, Tian Z A, Peng P 2020 Acta Phys. Sin. 69 196101 Google Scholar
[39]	Kbirou M, Atila A, Hasnaoui A 2024 Phys. Scr. 99 085946 Google Scholar
[40]	Khmich A, Sbiaai K, Hasnaoui A 2019 J. Non-Cryst. Solids 510 81 Google Scholar
[41]	Fan X, Pan D, Li M 2019 J. Phys. Condens. Matte 31 095402 Google Scholar
[42]	Guder V, Celtek M, Celik F A, Sengul S 2023 J. Non-Cryst. Solid 602 122067 Google Scholar
[43]	Chen Y X, Feng S D, Lu X Q, Kang H, Ngai K L, Wang L M 2022 J. Mol. Liq. 368 120706 Google Scholar
[44]	Nosé S 1984 J. Chem. Phys. 81 511 Google Scholar
[45]	Parrinello M, Rahman A 1981 J. Appl. Phys. 52 7182 Google Scholar
[46]	Wang B, Shang B S, Gao X Q, Sun Y T, Qiao J C, Wang W H, Pan M X, Guan P F 2022 J. Non-Cryst. Solid 576 121247 Google Scholar
[47]	Jafary-Zadeh M, Aitken Z H, Tavakoli R, Zhang Y W 2018 J. Alloys Compd. 748 679 Google Scholar

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高压下金属钽液体中拓扑密堆团簇对凝固路径的影响规律