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Title: Role of string-like collective atomic motion on diffusion and structural relaxation in glass forming Cu-Zr alloys

We investigate Cu-Zr liquid alloys using molecular dynamics simulation and well-accepted embedded atom method potentials over a wide range of chemical composition and temperature as model metallic glass-forming (GF) liquids. As with other types of GF materials, the dynamics of these complex liquids are characterized by “dynamic heterogeneity” in the form of transient polymeric clusters of highly mobile atoms that are composed in turn of atomic clusters exhibiting string-like cooperative motion. In accordance with the string model of relaxation, an extension of the Adam-Gibbs (AG) model, changes in the activation free energy ΔG{sub a} with temperature of both the Cu and Zr diffusion coefficients D, and the alpha structural relaxation time τ{sub α} can be described to a good approximation by changes in the average string length, L. In particular, we confirm that the strings are a concrete realization of the abstract “cooperatively rearranging regions” of AG. We also find coexisting clusters of relatively “immobile” atoms that exhibit predominantly icosahedral local packing rather than the low symmetry packing of “mobile” atoms. These two distinct types of dynamic heterogeneity are then associated with different fluid structural states. Glass-forming liquids are thus analogous to polycrystalline materials where the icosahedrally packed regions correspondmore » to crystal grains, and the strings reside in the relatively disordered grain boundary-like regions exterior to these locally well-ordered regions. A dynamic equilibrium between localized (“immobile”) and wandering (“mobile”) particles exists in the liquid so that the dynamic heterogeneity can be considered to be type of self-assembly process. We also characterize changes in the local atomic free volume in the course of string-like atomic motion to better understand the initiation and propagation of these fluid excitations.« less
Authors:
 [1] ;  [2] ; ; ; ;  [1] ;  [3] ;  [4] ;  [5]
  1. International Center for New-Structured Materials (ICNSM), Zhejiang University and Laboratory of New-Structured Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027 (China)
  2. (Canada)
  3. (China)
  4. Materials Science and Engineering Division, National Institute of Standards and Technology, Gaithersburg, Maryland 20899 (United States)
  5. State Key Laboratory of Modern Optical Instrumentation, Zhejiang University, Hangzhou 310027 (China)
Publication Date:
OSTI Identifier:
22415715
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 142; Journal Issue: 16; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ATOMIC CLUSTERS; ATOMS; CHEMICAL COMPOSITION; COMPUTERIZED SIMULATION; CONCRETES; COPPER ALLOYS; DIFFUSION; EXCITATION; FREE ENERGY; GRAIN BOUNDARIES; LIQUIDS; METALLIC GLASSES; MOLECULAR DYNAMICS METHOD; POLYCRYSTALS; RELAXATION TIME; ZIRCONIUM ALLOYS