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Pulsed-Laser-Induced Melting and Solidification of Thin Metallic Films

机译:脉冲激光诱导的金属薄膜熔化和凝固

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摘要

This thesis focused on investigating excimer-laser induced melting and solidification of thin metallic films on SiO2. Two distinct topics were pursued: (1) microstructural manipulation and optimization of Cu films via SLS of as-deposited Cu films on SiO2, and (2) investigation of oriented heterogeneous nucleation via complete melting and subsequent nucleation-initiated solidification of Ni films on SiO2. The work on SLS of Cu films is motivated in large part by the need to improve the properties of Cu films which, among other applications, constitute an essential element in the continued evolution of microelectronic products. The experiments we have conducted show clearly that the film can be, without much difficulty, melted and solidified using pulsed-laser irradiation. Based on the findings from a series of systematic single-shot experiments, we show that SLS can be properly implemented to obtain large-grained Cu films with controlled microstructures and restricted textures. The lateral growth distance was found to increase as a function of increasing incident energy density. This observation is consistent with the findings that were made previously using other materials, and basically indicates that lateral solidification continues until the interface is halted by the interfaces growing from nucleated solids, which are triggered within the liquid matrix ahead of the growing interface. Close examination of the laterally grown grains, which quickly develop 100 rolling direction crystallographic orientation texture due to occlusion of differently oriented grains, reveal, furthermore, that low-angle grain boundaries as well as twins can be generated during the growth. These intra-grain defects are found to appear in a systematic manner (as they are located at specific regions and observed under specific incident energy densities). Significantly longer lateral growth distances observed in Cu films (compared to that of Si films) was attributed to the fact that substantially higher growth rates are expected with simple metallic films at a given interfacial undercooling. The implementation of SLS using Cu films was accomplished quite effectively, as can be expected from the above lateral-growth-related results involving single-shot experiments. We were able to achieve a variety of large-grained, grain-boundary location and grain-orientation controlled Cu films via various SLS techniques. When performed optimally in accordance with the findings made in chapter 2, the resulting microstructure exhibits large grains, which are primarily devoid of intra-grain defects. For example, 2-shot SLS processed Cu films led to strong 100 rolling direction orientation, while avoiding the formation of low-angle grain boundaries and twin-boundaries. The highlight of SLS on Cu films correspond to a version of SLS (referred to as "2-Shot plus 2-Shot" SLS) in which the second 2-shot SLS is performed in the direction perpendicular to the first one. Through this approach, we were able to achieve grain-boundary-location controlled microstructure with a strong 100 orientation texture in all three dimensions (forming, effectively, an ultra-large quasi-single crystal material). Nucleation of solids in laser-quenched Ni films was investigated using EBSD analysis. The surface orientation analysis of nucleated grains obtained within the complete melting regime reveal a clear sign of texture. From these and additional findings from previous work involving Al films, we were able to conclude that systematic heterogeneous nucleation has taken place, and, furthermore, that oriented nucleation of the solids must have taken place. Although always suspected to be the case, it is typically extremely challenging to prove with certainty, in conventional nucleation experiments, that the mechanism of nucleation corresponds to that of a heterogeneous one. Furthermore, although it has been suspected theoretically for over 50 years, experimental results that clearly show that oriented nucleation actually transpires have not been obtained until our work involving Al films; the present findings involving Ni films further strengthen this conclusion as the Ni system removes some of the experimental uncertainties that are associated with Al films, and, furthermore, suggests that the process of oriented nucleation is a general and rather pervasive phenomenon. Additionally, it was observed that the selected orientation changed as a function of incident energy density; in the low energy density regime (above the completed melting threshold) {110}-surface texture was observed, while {111}-surface texture became more dominent at higher densities. Motivated by our experimental work involving Al and Ni that clearly indicates that oriented heterogeneous nucleation is a major path through which heterogeneous nucleation of solids occurs, we have also carried out a 2-dimensional Winterbottom-type thermodynamic analysis that can be used to obtain a better understanding of the phenomenon. In contrast to the previous work on the subject, we consider in our modelling the anisotropic nature of both the solid-liquid and solid-substrate interfacial energy; we advocate that this is the only physically consistent combination. The results show that oriented nucleation can be systematically accounted for as stemming from the expected anisotropic nature of the involved interfacial energies. Furthermore, the analysis also suggests possible reasons for observing a transition in surface texture from one orientation to another.
机译:本文主要研究准分子激光诱导的SiO2上金属薄膜的熔化和凝固。进行了两个不同的主题:(1)通过在SiO2上沉积的Cu膜的SLS通过SLS进行Cu膜的微观结构处理和优化,以及(2)通过在SiO2上Ni膜的完全熔化和随后的成核引发的凝固研究取向异相成核。 Cu膜SLS的工作很大程度上是由于需要改善Cu膜的性能而引起的,在其他应用中,Cu膜的性能构成了微电子产品持续发展的基本要素。我们进行的实验清楚地表明,使用脉冲激光辐照可以很容易地熔融和固化薄膜。基于一系列系统性单次实验的发现,我们表明SLS可以正确实施以获得具有可控的微观结构和受限制的织构的大晶粒Cu膜。发现横向生长距离随着入射能量密度的增加而增加。该观察结果与先前使用其他材料所获得的发现是一致的,并且基本上表明横向凝固一直持续到界面被有核固体生长的界面停止为止,该界面从有核固体中生长出来,而有核固体则在增长的界面之前在液体基质中被触发。对横向生长的晶粒进行仔细检查,由于不同取向晶粒的咬合,晶粒迅速形成了100个轧制方向的结晶取向织构,此外,还发现在生长过程中会产生低角度晶粒边界和孪晶。发现这些晶粒内缺陷以系统的方式出现(因为它们位于特定区域并在特定入射能量密度下观察到)。在铜膜中观察到的横向生长距离明显长于硅膜(与硅膜相比),这是由于在给定的界面过冷条件下,简单的金属膜的生长速度有望大大提高。从上述涉及单次实验的横向生长相关结果可以预期,使用铜膜的SLS实施非常有效。通过各种SLS技术,我们能够实现各种大晶粒,晶界位置和晶粒取向控制的Cu膜。当根据第2章中的发现进行最佳操作时,所得的显微组织会呈现出大晶粒,而这些晶粒主要没有晶粒内缺陷。例如,经2次SLS处理的Cu膜可产生强的100轧制方向取向,同时避免形成低角度晶界和孪晶界。 Cu膜上的SLS高光对应于SLS的一种版本(称为“ 2-Shot加2-Shot” SLS),其中第二个2-shot SLS在垂直于第一个的方向上执行。通过这种方法,我们能够在所有三个维度(有效地形成超大型准单晶材料)上实现具有强100取向织构的晶界位置可控的微观结构。使用EBSD分析研究了激光淬火Ni膜中的固体成核。在完全熔化过程中获得的有核晶粒的表面取向分析显示出明显的织构迹象。从涉及Al膜的先前工作的这些以及其他发现中,我们可以得出结论,已经发生了系统的异质成核,此外,固体的定向成核也已经发生。尽管总是被怀疑是这种情况,但是在常规成核实验中,要确定性地证明成核机理与异质成核机理相对应,通常很难确定。此外,尽管从理论上已经怀疑了50多年,但实验结果清楚地表明,直到我们涉及Al薄膜的工作才获得取向成核的实际效果。由于镍体系消除了与铝膜有关的一些实验不确定性,因此涉及镍膜的当前发现进一步证实了这一结论,并且进一步表明,取向成核过程是普遍且相当普遍的现象。另外,观察到所选取向随着入射能量密度的变化而变化。在低能量密度条件下(高于完全熔化阈值),观察到{110}-表面织构,而{111}-表面织构在较高密度下变得更占优势。受我们涉及Al和Ni的实验工作的启发,该研究清楚地表明,定向异相成核是固体异相成核发生的主要途径,我们还进行了二维Winterbottom型热力学分析,可以用来更好地了解这种现象。与先前有关该主题的工作相反,我们在建模时考虑了固液界面能和固相界面能的各向异性。我们主张这是唯一的物理上一致的组合。结果表明,定向成核可以系统地解释为源于所涉及界面能的预期各向异性。此外,分析还提出了观察表面纹理从一种取向向另一种取向转变的可能原因。

著录项

  • 作者

    Choi Min Hwan;

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  • 年度 2012
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  • 原文格式 PDF
  • 正文语种 {"code":"en","name":"English","id":9}
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