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运用基于密度泛函理论的第一性原理分子动力学和静态电子结构计算，研究了La65X35（X=Ni，Al）非晶合金体系原子结构随温度演化的规律及其相关电子结构特性.使用径向分布函数、Voronoi团簇以及键对分析等给出了从高温液体快速冷却到玻璃态过程中原子结构的演化规律.研究发现，该类合金体系的原子排布符合局域密堆模型，两体系中占比最大的特征多面体类型由溶质与溶剂原子半径比调控；两体系中高五次对称性局域结构随温度的下降而增加验证了其在抑制晶化方面的重要作用；利用投影态密度分析两体系电子结构之间的差异，指出La-5d与Ni-3d电子间强烈的杂化是LaNi 间键长缩短的电子结构起源，为理解成分相关的结构和物性提供了重要线索.The atomic-level structure of metallic glasses (MGs) is one of the most fundamental and challenging topics in condensed matter physics. Unlike crystalline metals or alloys, the MGs are lacking in a well-defined description of structure order, which is a major obstruction for relating its structure to physical properties. Obviously, it is vitally important to have an in-depth understanding of the atomic packing scheme in MGs. Due to the limitations of experimental characterization methods, it is hard to obtain the atomic packing scheme of MGs in experiment. Computational simulation on an atomic scale has become an important method of characterizing the atomic structure of MGs. The La-based LaNiAl glass forming system is well-known for its good glass-forming ability, distinctive relaxation peak that is well separated from relaxation, and liquid-liquid transition at a temperature around 1000 K. Many efforts have been made to investigate these novel properties. However, the atomic structure of this system is rarely studied. In this paper, the atomic structure evolution from liquids to glass states in La-based binary MGs La65Ni35 and La65Al35 are studied via ab initio molecular dynamics based on the density functional theory. The local structures are systematically analyzed by the radical distribution function, partial radical distribution function (PRDF), Voronoi tessellation method, and bond-type method in Honeycutt-Andersen. The results indicate that the PRDF of NiNi is much weaker than that of AlAl, which indicates the NiNi avoidance in La65Ni35. The major peaks of PRDFs are always smaller than the sum of efficient radius of the two kinds of atoms, especially for LaNi pairs. Atomic structure of the two systems are coincident with dense atomic packing scheme and the difference between major Voronoi polyhedron types (0, 3, 6, 0 for La65Ni35 and 0, 2, 8, 1, 0, 2, 8, 0 for La65Al35) in local structures is controlled by their ratio of solute to solvent atomic size. The high five-fold local symmetry structure gradually increases in both systems with the decrease of temperature, which validates its pivotal part in hindering crystallization. The electronic structure is studied with the partial density of states. It is found that the significant bond-shortening between La and Ni is due to the strong hybridization between Ni-3d and La-5d electrons and this result may play a key role in understanding composition related structure and properties in MGs.
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Keywords:
- metallic glass /
- atomic structure /
- ab initio calculation /
- electronic structure
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[1] Miracle D B 2004 Nature Mater. 3 697
[2] Greer A L, Ma E 2007 MRS Bull. 32 611
[3] Wang W H 2013 Prog. Phys. 33 177 (in Chinese)[汪卫华 2013 物理学进展 33 177]
[4] Liu Y H, Wang G, Wang R J, Pan M X, Wang W H 2007 Science 315 1385
[5] Guo G Q, Yang L, Zhang G Q 2011 Acta Phys. Sin. 60 016103 (in Chinese)[郭古青, 杨亮, 张国庆 2011 物理学报 60 016103]
[6] Bai H Y, Tang M B, Wang W H, Wang W L, Yu P 2005 Acta Phys. Sin. 54 3284 (in Chinese)[白海洋, 汤美波, 汪卫华, 王万录, 余鹏 2005 物理学报 54 3284]
[7] Sheng H W, Luo W K, Alamgir F M, Bai J M, Ma E 2006 Nature 439 419
[8] Wei H Q, Long Z L, Xu F, Zhang P, Tang Y 2014 Acta Phys. Sin. 63 118101 (in Chinese)[危洪清, 龙志林, 许福, 张平, 唐翌 2014 物理学报 63 118101]
[9] Wang W Y, Fang H Z, Shang S L, Zhang H, Wang Y, Hui X, Mathaudhu S, Liu Z K 2011 Physica B 406 3089
[10] Luo W K, Sheng H W, Ma E 2006 Appl. Phys. Lett. 89 131927
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[12] Sheng H W, Ma E, Liu H Z, Wen J 2006 Appl. Phys. Lett. 88 171906
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[15] Okumura H, Chen H S, Inoue A, Masumoto T 1991 Jpn. J. Appl. Phys. 30 2553
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[17] Xu W, Sandor M T, Yu Y, Ke H B, Zhang H P, Li M Z, Wang W H, Liu L, Wu Y 2015 Nat. Commun. 6 7696
[18] Kresse G, Furthmller J 1996 Phys. Rev. B 54 11169
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[22] Finney J L 1977 Nature 266 309
[23] Frank F C, Kasper J S 1958 Acta Crystallogr. 11 184
[24] Miracle D B 2006 Acta Mater. 54 4317
[25] Honeycutt J D, Andersen H C 1987 J. Phys. Chem. 91 4950
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