In Situ Determination of the Nanoscale Chemistry and Behavior of Solid-Liquid Systems

Many fundamental questions in crystal-growth behavior remain unanswered because of the difficulties encountered in simultaneously observing phases and determining elemental concentrations and redistributions while crystals nucleate and grow at the nanoscale. We show that these obstacles can be overcome by performing energy-dispersive x-ray spectroscopy on partially molten Al-Si-Cu-Mg alloy particles during in situ heating in a transmission electron microscope. Using this technique, we were able to (i) determine that the aluminum and silicon concentrations change in a complementary and symmetric manner about the solid-liquid interface as a function of temperature; (ii) directly measure the solid- and liquid-phase compositions at equilibrium and in highly undercooled conditions for quantitative comparison with thermodynamic calculations of the liquidus and solidus phase boundaries; and (iii) provide direct evidence for homogeneous nucleation of the aluminum-rich solid. Crystal growth is an important technolog-ical process affecting fields from metal-lurgy to solid-state physics and applications ranging from the production of metal-alloy ingots for buildings and aircraft to single-crystal semi-conductors and oxides for electronic and optical devices (1, 2). It is also involved in everyday nat