Please wait a minute...
Acta Metall Sin  2025, Vol. 61 Issue (12): 1925-1932    DOI: 10.11900/0412.1961.2024.00206
Research paper Current Issue | Archive | Adv Search |
On the Homogeneous Nucleation Characteristics of Al Droplets During Isothermal Crystallization
WANG Shucheng, PENG Ping()
School of Materials Science and Engineering, Hunan University, Changsha 410082, China
Cite this article: 

WANG Shucheng, PENG Ping. On the Homogeneous Nucleation Characteristics of Al Droplets During Isothermal Crystallization. Acta Metall Sin, 2025, 61(12): 1925-1932.

Download:  HTML  PDF(1915KB) 
Export:  BibTeX | EndNote (RIS)      
Abstract  

Owing to the important role of homogeneous nucleation in grain refinement of rapidly solidified alloys, a detailed molecular dynamics simulation is performed to investigate the incubation of embryos and their evolution into nuclei during the isothermal crystallization of liquid Al droplets. Using the cluster type index method (CTIM) based on Honeycutt-Andersen (H-A) bond-type indices, various fcc critical nuclei formed during isothermal crystallization are distinguished from numerous fcc embryos through reverse tracking of atomic trajectories, relying on the structural heredity of fcc single-crystal clusters. The results show that nuclei first appear in the shell region of Al droplets with a critical size (nc) ranging from 2 to 100 atoms at an undercooling of ΔT ≈ 0.41Tm (Tm is melting point). Both the steady-state nucleation rate (I0) and the average critical nucleus size (n¯c) in the shell are higher than those in the core region. Visual analysis of the geometry of critical nuclei reveals that most are non-spherical, and the liquid-solid interface is not a simple fcc-liquid dual-phase configuration, but rather a multi-phase structure involving fcc-liquid and hcp components. Compared with the nucleation in Al bulk, a longer average nucleation incubation time (τ¯c) of critical nuclei is observed in Al droplets, with τ¯c in the shell region being longer than that in the core. When τ¯c is divided into the average incubation time of embryos (τ¯e) and their average effective growth time (τ¯geff), it is determined that τ¯geff is considerably longer than τ¯e in both Al droplets and Al bulk. For the four modes of nucleation, i.e., (I) embryo incubation and subsequent effective growth, (II) only effective growth of embryos, (III) direct nucleation after embryo incubation, and (IV) direct transformation from liquid atoms, a tracking analysis of atomic trajectories reveals that few critical nuclei are formed directly from liquid atoms. In contrast, most critical nuclei undergo both embryo incubation and effective growth, and these exhibit the largest n¯c. Moreover, the incubation time (τe) of embryos has little effect on n¯c of critical nuclei, whereas a large n¯c typically requires a long effective growth time (τgeff) of embryos during isothermal crystallization.

Key words:  nucleation      droplet      molecular dynamics simulation     
Received:  14 June 2024     
ZTFLH:  TG111.4  
Fund: National Natural Science Foundation of China(51871096)
Corresponding Authors:  PENG Ping, professor, Tel: 13873119465, E-mail: ppeng@hnu.edu.cn

URL: 

https://www.ams.org.cn/EN/10.11900/0412.1961.2024.00206     OR     https://www.ams.org.cn/EN/Y2025/V61/I12/1925

Fig.1  Schematics of continuous and transient heredities of fcc single crystal cluster cores, in which red and blue balls represent continuously and transiently inheritable atoms, respectively (t is the isothermal crystallization time; t0 is a designated moment for the reverse tracing of atom trajectories; Δt is the time interval; i = 1, 2, 3, … is recorded step number; tfcc and tSCC are the initial moments of transient heredity of fcc atoms and fcc single crystal cores, respectively; tinitial represents the initial moment of continuous heredity; tonset denotes the onset moment of nucleation corresponding to a critical nucleus; nc(t) and lc(t) are the quantity of continuously inheritable fcc atoms and the number of intercross-sharing (IS) linkages among continuously heritable fcc atoms in fcc single crystal clusters, respectively)
Fig.2  t dependences of average energy per atom (E(t)) in the Al droplet and Al bulk systems during the isothermal crystallization and its derivative (∂E / ∂t) with respect to t (tcs, tcm, and tce denote the beginning moment, the peak moment, and the ending moment of phase transformation, respectively)
Fig.3  Pair distribution function (g(r)) curves (a, c) and percentages of fcc, hcp, bcc, and ico atoms (b, d) during the isothermal crystallization of Al droplet (a, b) and Al bulk (c, d) (r—distance from the central atom. fcc, hcp, bcc, and ico represent faced-centered cubic, hexagonal close-packed, body-centered cubic, and icosahedral, respectively)
Fig.4  t dependences of quantity (qSCC) and average size (n¯SCC) of fcc single crystal clusters (ts—the moment corresponding to the maximum value of qSCC) (a) and snapshots of spatial distributions of atoms at several special moments (Green, red, blue, and yellow balls represent fcc, hcp, bcc, and ico atoms, respectively) (b)
Fig.5  Distribution of quantities of critical nuclei (qc) along the radius direction of Al droplet (Inset is a schematic of Al droplet partitioning. R—radius of Al droplet)
Fig.6  Total quantity of critical nuclei (qca) as a function of t (a) and qca with different critical sizes (nc) at different t (b) in the Al bulk and the core and shell of Al droplet (n¯caverage size of critical nuclei)
Fig.7  Snapshots of internal structures (a1-c1) of critical nuclei and their interfacial morphologies (a2-c2) (Green, red, and gray balls represent fcc, hcp, and other atoms, respectively. The digits on the ball are the identification codes of atoms)
(a1, a2) chainlike (b1, b2) lamellar (c1, c2) ellipsoidal/half-spherical
Regionτ¯eτ¯geffτ¯c
Droplet core1.895.197.08
Droplet shell2.315.067.37
Bulk1.834.736.20
Table 1  Average time of embryos incubation (τ¯e), effective growth (τ¯geff), and nucleation incubation (τ¯c) of core and shell of Al droplets as well as Al bulk
Fig.8  Relationships between incubation time of embryos (τe) (a) and effective growth time (τgeff)(b) of embryos with n¯c in core and shell of Al droplets as well as Al bulk
Fig.9  nc and qca of critical nuclei formed by different modes in Al droplet core (a), Al droplet shell (b), and Al bulk (c) (τc—nucleation incubation time)
[1] Wang J C, Guo C, Zhang Q, et al. Recent progresses in modeling of nucleation during solidification on the atomic scale [J]. Acta Metall. Sin., 2018, 54: 204
王锦程, 郭 灿, 张 琪 等. 原子尺度下凝固形核计算模拟研究的进展 [J]. 金属学报, 2018, 54: 204
[2] Murphy A G, Mathiesen R H, Houltz Y, et al. Direct observation of spatially isothermal equiaxed solidification of an Al-Cu alloy in microgravity on board the MASER 13 sounding rocket [J]. J. Cryst. Growth, 2016, 454: 96
[3] Abou-Khalil L, Salloum-Abou-Jaoude G, Reinhart G, et al. Influence of gravity level on columnar-to-equiaxed transition during directional solidification of Al-20 wt.% Cu alloys [J]. Acta Mater., 2016, 110: 44
[4] Ruan Y, Wang Q Q, Chang S Y, et al. Structural evolution and micromechanical properties of ternary Al-Ag-Ge alloy solidified under microgravity condition [J]. Acta Mater., 2017, 141: 456
[5] Luo S B, Wang W L, Xia Z C, et al. Theoretical prediction and experimental observation for microstructural evolution of undercooled nickel-titanium eutectic type alloys [J]. J. Alloys Compd., 2017, 692: 265
[6] Geng D L, Xie W J, Yan N, et al. Surface waves on floating liquids induced by ultrasound field [J]. Appl. Phys. Lett., 2013, 102: 041604
[7] Mahata A, Zaeem M A, Baskes M I. Understanding homogeneous nucleation in solidification of aluminum by molecular dynamics simulations [J]. Modell. Simul. Mater. Sci. Eng., 2018, 26: 025007
[8] Brandel C, ter Horst J H. Measuring induction times and crystal nucleation rates [J]. Faraday Discuss., 2015, 179: 199
[9] Yi P, Rutledge G C. Molecular origins of homogeneous crystal nucleation [J]. Annu. Rev. Chem. Biomol. Eng., 2012, 3: 157
[10] Herlach D M, Palberg T, Klassen I, et al. Overview: Experimental studies of crystal nucleation: Metals and colloids [J]. J. Chem. Phys., 2016, 145: 211703
[11] Li R, Wu Y Q, Xiao J J. The nucleation process and the roles of structure and density fluctuations in supercooled liquid Fe [J]. J. Chem. Phys., 2014, 140: 034503
[12] Li Y, Peng P. Identification and tracking of different types of crystalline nucleiduring isothermal crystallization of amorphous Ag [J]. Acta Phy. Sin., 2019, 68: 076401
李 媛, 彭 平. 非晶Ag晶化过程中不同类型晶核结构的识别与跟踪 [J]. 物理学报, 2019, 68: 076401
[13] Li Y, Peng P, Xu D S, et al. Identification of critical nuclei in the rapid solidification via configuration heredity [J]. J. Phys.: Condens. Matter, 2021, 33: 175701
[14] Liu Z B, Li Y, Peng P, et al. An exact measurement of nucleation incubation times in isothermal crystallizations of liquid metal Al via configuration heredity [J]. J. Cryst. Growth, 2023, 601: 126927
[15] Page A J, Sear R P. Heterogeneous nucleation in and out of pores [J]. Phys. Rev. Lett., 2006, 97: 065701
[16] Filipponi A, Giammatteo P. Kinetic Monte Carlo simulation of the classical nucleation process [J]. J. Chem. Phys., 2016, 145: 211913
[17] Guo Y L, Wang J C, Wang Z J, et al. Phase field crystal model for the effect of colored noise on homogenerous nucleation [J]. Acta Phys. Sin., 2012, 61: 146401
郭耀麟, 王锦程, 王志军 等. 噪声对均质形核过程影响的晶体相场法研究 [J]. 物理学报, 2012, 61: 146401
[18] Plimpton S. Fast parallel algorithms for short-range molecular dynamics [J]. J. Comput. Phys., 1995, 117: 1
[19] Mendelev M I, Kramer M J, Becker C A, et al. Analysis of semi-empirical interatomic potentials appropriate for simulation of crystalline and liquid Al and Cu [J]. Philos. Mag., 2008, 88: 1723
[20] Liu R S, Dong K J, Li J Y, et al. Formation and description of nano-clusters formed during rapid solidification processes in liquid metals [J]. J. Non-Cryst. Solids, 2005, 351: 612
[21] Wei Y D, Peng P, Yan Z Z, et al. A comparative study on local atomic configurations characterized by cluster-type-index method and Voronoi polyhedron method [J]. Comput. Mater. Sci., 2016, 123: 214
[22] Wen D D, Peng P, Jiang Y Q, et al. A track study on icosahedral clusters inherited from liquid in the process of rapid solidification of Cu64Zr36 alloy [J]. Acta Phys. Sin., 2013, 62: 196101
文大东, 彭 平, 蒋元祺 等. 快凝过程中液态Cu64Zr36合金二十面体团簇遗传与演化跟踪 [J]. 物理学报, 2013, 62: 196101
[23] Hou Z Y, Liu R S, Liu H R, et al. Formation mechanism of critical nucleus during nucleation process of liquid metal sodium [J]. J. Chem. Phys., 2007, 127: 174503
[24] E J C, Wang L, Cai Y, et al. Crystallization in supercooled liquid Cu: Homogeneous nucleation and growth [J]. J. Chem. Phys., 2015, 142: 6
[25] Song H, Sun Y, Zhang F, et al. Nucleation of stoichiometric compounds from liquid: Role of the kinetic factor [J]. Phys. Rev. Mater., 2018, 2: 023401
[26] Wedekind J, Reguera D. Kinetic reconstruction of the free-energy landscape [J]. J. Phys. Chem., 2008, 112B: 11060
[27] Kalikmanov V I. Nucleation Theory [M]. Dordrecht: Springer, 2013: 17
[1] ZHANG Wenbin, LI Xiaolong, HAO Shuo, LIU Shengjie, CAI Xingzhou, CHEN Lei, JIN Miao. Microcrack Nucleation and Propagation of TRIP-Assisted Duplex Stainless Steel Fe-19.6Cr-2Ni-2.9Mn-1.6Si[J]. 金属学报, 2025, 61(4): 608-618.
[2] LIU Yong, ZENG Gang, LIU Hong, WANG Yu, LI Jianlong. Grain Refinement Mechanism and Research Progress of Magnesium Alloy Incorporating Zr[J]. 金属学报, 2024, 60(2): 129-142.
[3] LI Yanqiang, ZHAO Jiuzhou, JIANG Hongxiang, ZHANG Lili, HE Jie. Liquid-Solid Phase Separation Process of Pb-Al Alloy Under the Effect of Electric Current Pulses[J]. 金属学报, 2024, 60(12): 1710-1720.
[4] GENG Ruwei, WANG Lin, WEI Zhengying, MA Ninshu. Microstructure Evolution and Epitaxial Growth Characteristics of Droplet and Arc Deposition Additive Manufacturing for Aluminum Alloy[J]. 金属学报, 2024, 60(11): 1584-1594.
[5] CHEN Mingyi, HU Junwei, YU Yaochen, NIU Haiyang. Advances in Machine Learning Molecular Dynamics to Assist Materials Nucleation and Solidification Research[J]. 金属学报, 2024, 60(10): 1329-1344.
[6] LI Zhishang, ZHAO Long, ZONG Hongxiang, DING Xiangdong. Machine-Learning Force Fields for Metallic Materials: Phase Transformations and Deformations[J]. 金属学报, 2024, 60(10): 1388-1404.
[7] ZHAO Yafeng, LIU Sujie, CHEN Yun, MA Hui, MA Guangcai, GUO Yi. Critical Inclusion Size and Void Growth in Dual-Phase Ferrite-Bainite Steel During Ductile Fracture[J]. 金属学报, 2023, 59(5): 611-622.
[8] WU Caihong, FENG Di, ZANG Qianhao, FAN Shichun, ZHANG Hao, LEE Yunsoo. Microstructure Evolution and Recrystallization Behavior During Hot Deformation of Spray Formed AlSiCuMg Alloy[J]. 金属学报, 2022, 58(7): 932-942.
[9] LI Xifeng, LI Tianle, AN Dayong, WU Huiping, CHEN Jieshi, CHEN Jun. Research Progress of Titanium Alloys and Their Diffusion Bonding Fatigue Characteristics[J]. 金属学报, 2022, 58(4): 473-485.
[10] HOU Yubai, YU Yueguang, GUO Zhimeng. Simulation Study of Smoothed Particle Hydrodynamics (SPH) Method in Plasma Spheroidization of W-Ni-Fe Ternary Alloys[J]. 金属学报, 2021, 57(2): 247-256.
[11] LIANG Jinjie, GAO Ning, LI Yuhong. Interaction Between Interstitial Dislocation Loop and Micro-Crack in bcc Iron Investigated by Molecular Dynamics Method[J]. 金属学报, 2020, 56(9): 1286-1294.
[12] ZHOU Xia,LIU Xiaoxia. Mechanical Properties and Strengthening Mechanism of Graphene Nanoplatelets Reinforced Magnesium Matrix Composites[J]. 金属学报, 2020, 56(2): 240-248.
[13] Juan DU, Xiaoxing CHENG, Tiannan YANG, Longqing CHEN, Frédéric Mompiou, Wenzheng ZHANG. In Situ TEM Study on the Sympathetic Nucleation of Austenite Precipitates[J]. 金属学报, 2019, 55(4): 511-520.
[14] Haifeng ZHANG, Haile YAN, Nan JIA, Jianfeng JIN, Xiang ZHAO. Exploring Plastic Deformation Mechanism of MultilayeredCu/Ti Composites by Using Molecular Dynamics Modeling[J]. 金属学报, 2018, 54(9): 1333-1342.
[15] Dandan FAN, Junfeng XU, Yanan ZHONG, Zengyun JIAN. Effect of Superheated Temperature and Cooling Rate on the Solidification of Undercooled Ti Melt[J]. 金属学报, 2018, 54(6): 844-850.
No Suggested Reading articles found!