We report the observation of a premelting transition at chemically sharp solid-liquid interfaces using molecular-dynamics simulations. The transition is observed in the solid-Al/liquid-Pb system and involves the formation of a liquid interfacial film of Al with a width that grows logarithmically as the bulk melting temperature is approached from below, consistent with current theories of premelting. The premelting behavior leads to a sharp change in the temperature dependence of the diffusion coefficient in the interfacial region, and could have important consequences for phenomena such as particle coalescence and shape equilibration, which are governed by interfacial kinetic processes.
2The term premelting refers to the formation of thermodynamically stable liquid films at solid interfaces subjected to temperatures below but near the bulk melting temperature (T m ). [1,2] Surface premelting (SP), the formation of a premelting layer at a solid-vapor interface, was first observed experimentally by Frenken and van der Veen [3] using proton scattering. Since then, advances in experimental techniques have provided powerful tools for direct atomicresolution observations of this surface phase transition. [4][5][6][7][8][9][10] These experimental studies have been complemented by a number of detailed atomistic simulations probing the existence and atomic-level mechanisms of SP (Refs. 11-18 and references therein). Premelting at solid-solid interfaces has also been reported in the literature and can take two basic forms: premelting at solid-solid heterophase boundaries and grain-boundary premelting (GBP). Examples of the former are found at interfaces between Pb and Al, [19] SiO and Al 2 O 3 , [20] as well as in ice at solid substrates, which plays a role in frost heave. [11,[21][22][23] Premelting at grain boundaries has been the subject of numerous continuum modeling studies, [24][25][26][27][28][29][30] In this work, we report molecular-dynamics (MD) simulation results on Al/Pb solid-liquid interfaces that predict the existence of a third class of premelting transition, namely, solid-liquid premelting (SLP). In this process a premelting liquid layer forms at a solid-liquid interface, below T m of the solid. Such a transition should, in principle, be possible at chemically heterogeneous solid-liquid interfaces in which the melt phase of the solid and the liquid phase are mutually immiscible, as is the case with Al and Pb near T m for Al. Solid-liquid premelting has not been previously reported under ambient pressures, either experimentally or by simulation -although some evidence of SLP has been reported in simulations of solid-liquid interfaces under extremely high pressures (diamond anvil). [32,33] As we will demonstrate, the process of SLP leads to a sharp change in the temperature dependence of the diffusion coefficient in the interfacial region, which is expected to have important consequences for the kinetics of interface-controlled processes such as particle shape equilibration or coalescence of liquid nanopar...