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Acta Metall Sin  2024, Vol. 60 Issue (10): 1439-1450    DOI: 10.11900/0412.1961.2024.00143
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Neural Network Molecular Dynamics Study of Ultrafast Laser-Induced Melting of Copper Nanofilms
GAO Tianyu1,2, ZENG Qiyu1,2(), CHEN Bo1,2, KANG Dongdong1,2, DAI Jiayu1,2()
1 College of Science, National University of Defense Technology, Changsha 410072, China
2 Hunan Key Laboratory of Extreme Matter and Applications, National University of Defense Technology, Changsha 410072, China
Cite this article: 

GAO Tianyu, ZENG Qiyu, CHEN Bo, KANG Dongdong, DAI Jiayu. Neural Network Molecular Dynamics Study of Ultrafast Laser-Induced Melting of Copper Nanofilms. Acta Metall Sin, 2024, 60(10): 1439-1450.

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Abstract  

Exploring ultrafast structural transitions in materials triggered by femtosecond laser pulses—from their condensed states to high-temperature, high-pressure conditions, and potentially to ideal plasmas—is a crucial scientific endeavor with profound implications for fields such as inertial confinement fusion, metal additive manufacturing, and laser processing. These extreme conditions, which are challenging to replicate and directly observe in experiments due to temporal and spatial resolution limitations, require theoretical models and simulations to decode the underlying microscopic mechanisms. Molecular dynamics (MD) simulations, especially when paired with advanced potential energy surfaces, are effective tools for addressing these challenges. However, maintaining a balance between computational efficiency and physical accuracy, particularly when simulating excited states induced by laser interactions, remains a formidable task. In this context, neural network potential energy surfaces (NNPES) have demonstrated exceptional capability for capturing the complex interactions and properties of materials under extreme conditions, providing vital links between quantum mechanics and macroscale phenomena. Using Cu as a prototypical example, the ability of NNPES to accurately depict lattice vibrations, thermophysical properties, and complex dynamics during laser-matter interactions has been demonstrated. By seamlessly integrating NNPES with a two-temperature MD model, this study directly simulates the atomic-scale dynamics of Cu thin films subjected to intense pulsed laser irradiation. This innovative approach, which combines quantum-level accuracy with large-scale thermodynamics and detailed microstructural evolution, provides unprecedented insights into the fundamental mechanisms of laser-induced melting. Our findings reveal two distinct melting behaviors in Cu, dependent on laser fluence. At fluences near the melting threshold, a heterogeneous melting process initiated at the film surface because of the lower free energy barrier was observed. The solid-liquid interface then moves inward at velocities of tens of meters per second, requiring hundreds of picoseconds for melting to complete. Conversely, at fluences well above the threshold, Cu films experience rapid and homogeneous melting, markedly different from conventional heating-induced melting. Here, the lattice temperature almost instantaneously exceeds the thermal stability limit, leading to uniform liquid nucleation and rapid growth throughout the film, culminating in complete melting within just tens of picoseconds. This study not only illuminates the atomic-scale dynamics of laser-induced melting but also underscores the transition from heterogeneous to homogeneous melting mechanisms as a function of laser fluence. This study serves as an invaluable research tool for enhancing our understanding of laser-matter interactions and their potential applications in optimizing laser-based manufacturing processes and predicting material behavior under extreme conditions. Moreover, the reliability and versatility of NNPES set the stage for extending the research to more complex systems, including alloys and amorphous materials. This expansion fosters robust connections between microscopic theories and macroscale applications, deepening our understanding of material responses to intense laser irradiation. Future studies employing this framework could explore complex physical phenomena such as explosive boiling and material disintegration during laser ablation, offering unique atomic-scale insights that could pave the way for groundbreaking discoveries and technological advancements.

Key words:  neural network      laser-matter interaction      melting dynamics      two-temperature model     
Received:  07 May 2024     
ZTFLH:  O469  
Fund: National Natural Science Foundation of China(12104507);Science and Technology Innovation Program of Hunan Province(2021RC4026);Postgraduate Technology Innovation Program of Hunan Province(CX20220070)
Corresponding Authors:  DAI Jiayu, professor, Tel: (0731)87001006, E-mail: jydai@nudt.edu.cn;
ZENG Qiyu, Tel: 18374847919, E-mail: zengqiyu@nudt.edu.cn

URL: 

https://www.ams.org.cn/EN/10.11900/0412.1961.2024.00143     OR     https://www.ams.org.cn/EN/Y2024/V60/I10/1439

Iter.Lattice structureTime / psEnsemble typeTemperature / KPressure / GPaSampled configuration
0fcc0.5NPT30000
1fcc1NPT30000
2fcc2NPT30000
3fcc4NPT30000
4fcc8NPT30000
5fcc16NPT30005
6fcc4NVT200, 4007
7fcc16NVT200, 4001
8fcc2NVT50060
9fcc4NVT5005
10fcc16NVT50010
11fcc2NVT80013
12fcc4NVT8009
13fcc16NVT80060
14fcc2NVT1000, 1200, 150060
15fcc4NVT1000, 1200, 150060
16fcc16NVT1000, 1200, 150060
17fcc0.5NPT300021
18fcc1NPT300046
19fcc2NPT300060
20fcc4NPT300060
21fcc8NPT300060
22fcc16NVT30060
23fcc4NVT200, 40060
24fcc16NVT200, 40060
25fcc2NVT50060
26fcc4NVT50060
27fcc16NVT50060
28fcc2NVT80060
29fcc4NVT80060
30fcc16NVT80060
31fcc2NVT1000, 120060
32fcc4NVT1000, 120060
33fcc8NVT1000, 120060
34fcc, liquid2NVT1500, 2000, 250060, 60
35fcc, liquid4NVT1500, 2000, 250060, 60
36fcc, liquid8NVT1500, 2000, 250060, 60
37Liquid2NVT300060
Table 1  Details of the exploration strategy for the deep potential (DP) model of Cu system under different thermodynamics conditions
Fig.1  Comparisions of DP model predicted energy from DP model (EDP),force (fDP), and virial tensor (VDP) of Cu with the energy (EDFT), force (fDFT), and virial tensor (VDFT) on the training set calculated by density functional theory (DFT)
(a) EDP-EDFT (b) fDP-fDFT (c) VDP-VDFT
Itema0 / nmTm / KΔHm / (kJ·kg-1)εm / (kJ·kg-1)
Relative error / %1.120.390.520.40
DP result0.36551275 ± 25232.3 ± 11.2658.7 ± 49.1
Experiment result0.3615[48]1280[51]231.1[53]661.3[51,53-56]
Table 2  Lattice constant (a0), melting point (Tm), latent heat of phase transition (ΔHm), and melting threshold (εm) of Cu obtained by using deep potential, and experimental results [48,51,53-56] for comparison
Fig.2  Phonon spectrum of solid copper obtained using DP model, and the experimental result[50] for comparison (The horizontal axis shows the value of the in-plane wave vector, along the Γ-X-W-X-U-Γ-L paths in the frst Brillouin zone)
Fig.3  DP model results and experimental results of Cu melting point under different pressure conditions (The red dots are the melting points under different pressure conditions calculated using DP, the red curve is the melting curve fitted using Simon-Glatzel equation[52], and the silver squares are the experimental result[51])
Fig.4  Lattice heat capacity (cp ) and electron heat capacity (ce) of Cu
(a) cp of Cu varied with ionic temperature (T) (The red dots are the result obtained using the DP potential, and the silver squares are the experimental result[54])
(b) ce of Cu varied with electron temperature (Te) (The red dots are the result of this work, the dashed blue lines are Smirnov's KS-DFT result[55] and the silver squares are the experimental result[56])
Fig.5  Evolutionary dynamics of Cu thin films at the laser flux of 18 mJ/cm2
(a) evolution of ion temperature (Ti) and (Te) over time
(b1-b4) evolutions of Te (b1), Ti (b2), density (ρ) (b3), and pressure (P) (b4) in different regions in the z direction of the Cu film with time
(c1-c6) atomic scale structural evolutions at time t = 0 ps (c1), 50 ps (c2), 100 ps (c3, c6), 150 ps (c4), and 200 ps (c5) (Fig.5c6 is the locally enlarged view of Fig.5c3, and polyhedral surface meshes (white interface) around fcc-type (brass) and liquid-type (gray) particles are constructed to highlight the heterogeneous phase transition)
Fig.6  Evolutionary dynamics of Cu thin films at the laser flux of 30 mJ/cm2
(a) evolutions of Ti and Te over time
(b1-b4) evolutions of Te (b1), Ti (b2), ρ (b3), and P (b4) in different regions in the z direction of the Cu film with time
(c1-c6) atomic scale structural evolutions at t = 0 ps (c1), 4 ps (c2), 8 ps (c3, c6), 12 ps (c4), and 16 ps (c5) (Fig.6c6 is the locally enlarged view of Fig.6c3, and polyhedral surface meshes (white interface) around fcc-type (brass) and liquid-type (gray) particles are constructed to highlight the homogeneous phase transition)
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