Abstract
Surface freezing, at temperatures up to a few degrees above the equilibrium melting point, has been observed for intermediate chain length (16≤ i≤ 50) n-alkanes [B. M. Ocko, X. Z. Wu, E. B. Sirota, S. K. Sinha, O. Gang and M. Deutsch, Phys. Rev. E, 1997, 55, 3164-3182]. Our recent experimental results suggest that surface freezing is also the first step when highly supercooled nanodroplets of n-octane crystallize. Our data yield surface and bulk nucleation rates on the order of ∼1015/cm2.s and ∼1022/cm3.s, respectively. Complementary molecular dynamics simulations also show that the surface of the droplet freezes almost immediately, and freezing of the remainder of the droplet progresses in a layer-by-layer manner.
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