摘要
本文采用分子动力学模拟方法,结合双体分布函数、键型指数法和团簇类型指数法(CTIM)等微观结构表征方法,以及基于CTIM的团簇跟踪技术,从微观结构的不同方面,系统研究了液态金属Na在不同条件下凝固过程中微观结构的形成和演变机理。并根据模拟研究的结果,对一些重要实验现象和凝固理论进行了微观解释。
对液态金属Na在不同冷速和熔体初始温度条件下的凝固过程进行了模拟,考察了不同热历史条件对凝固过程微观结构的影响。结果表明,冷速对凝固过程中微观结构的转变起关键性作用,当液态金属Na以1×10~(14) K/s和1×10~(13) K/s的冷速凝固时,形成以二十面体和缺陷二十面体基本原子团为主体的非晶态结构;而在以以1×10~(12) K/s和1×10~(11) K/s的冷速凝固时,形成bcc晶体结构。形成非晶的临界冷速约为10~(13) K/s。不同熔体初始温度对凝固结构晶化程度有明显影响,这种影响随熔体初始温度的降低呈非线性变化关系,但影响程度存在一个上、下限的范围。发现在液固转变温度(T_g和T_c)以上,不同冷速和熔体初始温度热历史条件对微观结构的影响并不明显;但在液固转变温度以下,不同热历史条件对微观结构的影响就明显、充分地表现出来。根据这一特点,有可能建立另一种确定T_g和T_c的新方法。
进一步对包含50000个Na原子的较大体系的快速凝固过程进行了模拟,研究了快速凝固过程团簇结构的形成特性和演变机理。结果表明,液态金属Na和Al在快速凝固过程中,其团簇结构的演变有相似之处,又各有其特征。CTIM与H-A键型指数法相比,更能有效识别两者的差异所在。这展现了CTIM对识别和表征团簇结构的有效性,它将为研究液态金属凝固过程中团簇结构的形成和演变特性提供一条新途径。快速凝固结构中纳米团簇的形成经历了一个复杂的演变过程:从高温液态中极不稳定的较小尺度原子团,经历了过冷液态中相对较稳定的中等尺度原子团,到T_g以下中等尺度原子团相互兼并而形成。金属Na体系比Al更容易形成纳米团簇,并且这些纳米团簇的结构显著不同于那些由气相沉积、离子溅射等方法所获得的团簇结构。
对包含10000个Na原子体系的凝固结晶过程进行了模拟,跟踪研究了结晶过程晶核的形成机理。液态金属Na晶化过程中,体系微观结构的转变从过冷液态中二十面体和缺陷二十面体为主体的结构,经历了T_c附近的缺陷bcc结构,到最后的接近完整bcc结构。团簇的能量和几何因素对凝固过程中最有利形成的微观结构组态同时起关键性作用。体系中晶核的形成会经历很多不同的形核路径,团簇的内部结构和尺寸对临界晶核的形成同时起关键性作用,内部结构的差异会引起临界晶核尺寸的不同。临界晶核呈非球状形貌,并且包含部分亚稳态结构。由模拟所得到的临界晶核尺寸,与经典形核理论的预测差别不大。在过冷液态金属Na恒温晶化过程,通过团簇跟踪分析所获得的结晶量随时间的变化关系,满足Johnson-Mehl-Avrami (JMA)结晶动力学规律。这一方面从原子层次出发验证了基本凝固理论的正确性,另一方面也说明了基于CTIM的团簇跟踪分析方法的有效性。
对包含10000个原子的非晶态金属Na体系等温退火过程进行了模拟,跟踪研究了非晶态金属Na晶化过程形核和长大机理。非晶态金属Na等温退火形核过程中,经历了二十面体和缺陷二十面体团簇结构逐渐解体,接着具有bcc对称性结构的团簇逐渐形成的过程。同时只有当具有bcc对称性结构团簇的尺寸达到某一临界尺寸时,才能成为稳定晶核。非晶态金属Na的晶化过程与其深过冷熔体结晶过程类似,呈现形核、长大和晶粒粗化三个阶段特征。通过对比不同分析方法所得到的结果可见,基于CTIM的团簇跟踪分析更能准确区分晶化过程的不同阶段特征,并为DSC实验不能清楚区分非晶态金属晶化阶段的实验现象,提供了良好的微观解释。
In this thesis, with the molecular dynamics method, the solidification processes of liquid metal Na under different conditions are simulated. By means of the different microstructural description methods of the pair distribution function, bond-type index method, and cluster-type index method (CTIM), and the technique of tracing cluster based on the CTIM, the formation properties and evolution mechanisms of microstructures during the solidification processes of liquid metal under different conditions are deeply studied. According to the computer simulation results, some experimental phenomenons and solidification theories are explained on microstructural level.
The solidification processes of liquid metal Na under different cooling rates and initial melt temperatures are simulated. The effects of different thermal history conditions on the microstructures during the solidification processes are investigated. The results show that the cooling rate plays a critical role in the transitions of microstructures. When the cooling rates are 1×10~(14) K/s and 1×10~(13) K/s, the amorphous structures are formed mainly with the icosahedron basic cluster and the defective icosahedron basic cluster. When the cooling rates are 1×10~(12) K/s and 1×10~(11)K/s, the bcc crystal structures are formed. The critical cooling rate for the formation of amorphous Na is about 10~(13) K/s. The initial melt temperature evidently affects the crystallinity of solidification structures. The influence degree is not linearly varying with the decrease of initial melt temperature, and has the upper and lower limits. It is still demonstrated that the effects of different cooling rates and initial melt temperatures on the microstructures of metal Na are very small above the liquid-solid transition temperature (T_g and T_c), but they are fully displayed near the liquid-solid transition points. According to this feature, it possibly provides a new method to determine the T_g and T_c.
The rapid solidification process of liquid metal Na with 50000 atoms is simulated. The formation properties and evolution mechanismes of cluster structures during the rapid solidification process are investigated. The results show that during the rapid solidification process of liquid metal Na and Al, there are some similar in their evolution features of cluster structures, meanwhile many differences. The CTIM can distinguish these differences more exactly than the H-A bond-type index method. The validity of CTIM in describing the cluster structures is confirmed, and it provides a new method of studing the formation properties of clusters during the solidification process. The formation and evolution of nano-clusters in the rapid solidification process have undergone a complicated evolution process: the small unstable cluster is formed in the liquid, through a middle-cluster in the supercooled liquid, and finally the nano-cluster is formed by combing several middle-clusters after T_g. The nano-clusters are formed more easily in liquid metal Na than in Al system, and the configurations of nano-clusters are also obviously different from those obtained by gaseous deposition, ionic spray methods and so on.
The crystallization process during the solidification of liquid metal Na with 10000 atoms is simulated. The formation mechanismes of crystal nuclei are investigated by tracing the evolution of clusters. The results show that during the crystallization process of liquid metal Na, the microstructures transform from the icosahedron or defective icosahedron structure in the supercooled liquid, through the defective bcc structure near the crystallization temperature, and finally to the perfect bcc structure. The energies of clusters and their geometrical constraints interplay the favorable microstructures during the nucleation process. The formation of nucleus may go along many different pathways. The size of cluster and its internal structure both play a crucial role in determining whether it is a critical nucleus. It is also found that the critical nucleus is non-spherical and may include some metastable structures. And the deviation of critical sizes in our simulations from the prediction of classical nucleation theory is not too much. The evolution of the volume fraction of crystal phases during the isothermal crystallization of the supercooled liquid metal Na satisfies the Johnson-Mehl-Avrami (JMA) theory. This verifes the validity of basic solidification theory from the microstructural level, on the other hand, the validity of the technique of tracing cluster based on the CTIM on studying the crystallization process is displayed.
The isothermal annealing process of amorphous metal Na with 10000 atoms is simulated. The formation and growth of nuclei in amorphous Na are traced. The results show the formations of nuclei undergo the shrink of clusters with icosahedron short-range order structure firstly, and then the bcc symmetric clusters are formed gradually. Only when the sizes of bcc symmetric clusters reach a critical size, they can turn into stable nuclei. The crystallization of amorphous Na exhibits three distinct stages three distinct stages of nucleation, subsequent growth of nuclei and coarsening of crystal grains. Through comparing the results obtained by different analysis methods, it is found that the CTIM can distinguish the different stages of crystallization processes. Our simulation results provide a reasonable explanation at atomic level for the experimental phenomenon that the DSC method cannot exactly reveal the crystallization stages of some amorphous metals.
引文
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