Persistent medium-range order and anomalous liquid properties of Al _1-xCu _x alloys

The development of short-to-medium-range order in atomic arrangements has generally been observed in noncrystalline solid systems such as metallic glasses. Whether such medium-range order (MRO) can exist in materials at well above their melting or glass-transition temperature has been a long-standing important scientific issue. Here, using ab initio molecular dynamics simulations, we show that a novel, persistent MRO exists in liquid Al-Cu alloys near the composition of CuAl ₃. The correlated atomic motions associated with the MRO give rise to a substantially enhanced viscosity in the vicinity of the composition. The component of the MRO liquid state gradually decreases with increasing temperature, and it disappears above a crossover temperature T _LLC. The continuous liquid-liquid crossover through a percolationlike transition leads to a pronounced heat capacity peak at T _LLC.