Kinetic Optimum of Volmer-Weber Growth

We find that the molecular beam epitaxy of Fe3Si on GaAs(001) observed by real-time x-ray diffraction begins by the abrupt formation of 3 monolayer (ML) high islands and approaches two-dimensional layer-by-layer growth at a thickness of 7 ML. A surface energy increase is confirmed by ab initio calculations and allows us to identify the growth as a strain-free Volmer-Weber transient. Kinetic Monte Carlo simulations incorporating this energy increase correctly reproduce the characteristic x-ray intensity oscillations found in the experiment. Simulations indicate an optimum growth rate for Volmer-Weber growth in between two limits, the appearance of trenches at slow growth and surface roughening at fast growth.