Abstract
Melting and solidification of as-deposited and recrystallized Bi crystallites, deposited on highly oriented 002-graphite at 423 K, were studied using reflection high-energy electron diffraction (RHEED). Films with mean thickness between 1.5 and 33 ML (monolayers) were studied. Ex situ atomic force microscopy was used to study the morphology and the size distribution of the formed nanocrystals. The as-deposited films grew in the form of three-dimensional crystallites with different shapes and sizes, while those recrystallized from the melt were formed in nearly similar shapes but different sizes. The change in the RHEED pattern with temperature was used to probe the melting and solidification of the crystallites. Melting started at temperatures below the bulk melting point of Bi, T-0=544.5 K, and extended over a temperature range that depended on the size distribution of the crystallites. The as-deposited 1.5 ML film started to melt at T-0-50 K and melted completely at T-0-20 K. For films with higher coverage, the size distribution was observed to spread over a wider range with a larger mean value, resulting in a shift in the melting temperature range towards higher temperatures. Due to the shift in size distribution to higher values upon recrystallization, the recrystallized Bi crystallites showed a melting temperature range higher than that of the as-deposited crystallites. For the investigated conditions, all films were completely melted below or at T-0 of Bi. The characteristic film melting point, defined as the temperature at which the film melting rate with temperature is the fastest, showed a linear dependence on the reciprocal of the average crystallite radius, consistent with theoretical models. Of these models, the surface-phonon instability model best fits the obtained results. During solidification, the Bi films showed high amount of supercooling relative to T-0 of Bi. The amount of liquid supercooling was found to decrease linearly with the reciprocal of the average crystallite size.