We determined the enthalpic and entropic contributions to the thermodynamics of coherently strained nanocrystals grown via deposition of pure Ge on Si(001) surfaces at 600 and 700 degrees C by analyzing their composition profile and local strain. We found that the free energy associated with the entropy of mixing, which drives GexSi1-x alloy formation, was significantly larger than the relaxation enthalpy that produces the islands. Thus, entropy plays a significant role in the evolution of the size and shape of the islands during growth through the strong thermodynamic drive to form an alloy.
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