Critical role of surface steps in the alloying of Ge on Si(001)

Using low-energy electron microscopy, we show that intermixing of Ge on Si(001) during growth is enhanced on stepped surfaces and is hindered on terraces where step flow does not occur. On large terraces we have identified a dramatic and unanticipated structural rearrangement that facilitates intermixing: Pairs of steps spontaneously form and migrate over the surface, leaving alloyed regions in their wake. The driving force for step formation is the entropy gain associated with the enhanced intermixing of Ge.