A locally preferred structure characterises all dynamical regimes of a supercooled liquid

preprint2016arXivOpen access

Abstract

Recent experimental results suggest that metallic liquids universally exhibit a high-temperature dynamical crossover, which is correlated with the glass transition temperature (TgT_{g}). We demonstrate, using molecular dynamics results for Cu64Zr36, that this temperature, TA≈2×TgT_{A} \approx 2 \times T_{g}, is linked with cooperative atomic rearrangements that produce domains of connected icosahedra. Supercooling to a new characteristic temperature, TDT_{D}, is shown to produce higher order cooperative rearrangements amongst connected icosahedra, leading to large-scale domain fluctuations and the onset of glassy dynamics. These extensive domains then abruptly stabilize above TgT_{g} and eventually percolate before the glass is formed. All characteristic temperatures (TAT_{A}, TDT_{D} and TgT_{g}) are thus connected by successive manifestations of the structural cooperativity that begins at TAT_{A}.

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