Onset of Cooperative Dynamics in an Equilibrium Glass-Forming Metallic Liquid

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• 作者：Abhishek Jaiswal ; Stephanie O’Keeffe ; Rebecca Mills ; Andrey Podlesynak ; Georg Ehlers ; Wojciech Dmowski ; Konstantin Lokshin ; Joseph Stevick ; Takeshi Egami ; Yang Zhang
• 刊名：Journal of Physical Chemistry B
• 出版年：2016
• 出版时间：February 18, 2016
• 年：2016
• 卷：120
• 期：6
• 页码：1142-1148
• 全文大小：492K
• ISSN：1520-5207

文摘

Onset of cooperative dynamics has been observed in many molecular liquids, colloids, and granular materials in the metastable regime on approaching their respective glass or jamming transition points, and is considered to play a significant role in the emergence of the slow dynamics. However, the nature of such dynamical cooperativity remains elusive in multicomponent metallic liquids characterized by complex many-body interactions and high mixing entropy. Herein, we report evidence of onset of cooperative dynamics in an equilibrium glass-forming metallic liquid (LM601: Zr₅₁Cu₃₆Ni₄Al₉). This is revealed by deviation of the mean effective diffusion coefficient from its high-temperature Arrhenius behavior below T_A ≈ 1300 K, i.e., a crossover from uncorrelated dynamics above T_A to landscape-influenced correlated dynamics below T_A. Furthermore, the onset/crossover temperature T_A in such a multicomponent bulk metallic glass-forming liquid is observed at approximately twice of its calorimetric glass transition temperature (T_g ≈ 697 K) and in its stable liquid phase, unlike many molecular liquids.