C lattice site distributions in metastable Ge1−yCy alloys grown on Ge(001) by molecular-beam epitaxy

Abstract

Epitaxial metastable Ge1−yCy alloy layers with y⩽0.045 were grown on Ge(001) by solid-source molecular-beam epitaxy (MBE) at temperatures Ts=200–400 °C. Using calculated strain coefficients and measured layer strains obtained from high-resolution reciprocal lattice maps (HR-RLMs), we determine C lattice site distributions as a function of Ts and total C concentration y. HR-RLMs show that all as-deposited alloys are fully coherent with their substrates. Ge1−yCy(001) layers grown at Ts⩽350 °C are in a state of in-plane tension and contain C in substitutional sites, giving rise to tensile strain, as well as in nanocluster sites which induce negligible lattice strain. Ts=400 °C layers are strain neutral with negligible substitutional C incorporation. Increasing y and/or Ts leads to a decrease in substitutional C concentration, consistent with Raman spectroscopy results, with a corresponding increase in the C fraction incorporated in nanocluster sites. The latter suggests that nanocluster formation is kinetically limited during film deposition by the C–C adatom encounter probability at the growth surface. Overall, the results show that it is not possible by MBE to obtain fully substitutional C incorporation in Ge1−yCy(001) alloys, irrespective of y and Ts. This is consistent with ab initio density functional calculations results showing that C incorporation in nanoclusters sites is energetically favored over incorporation in substitutional Ge lattice sites. Annealing the Ge1−yCy(001) layers at Ta=550 °C leads to a significant decrease in the substitutional C fraction and, hence, lower tensile strain. Layers annealed at 650 °C are strain free as all substitutional C has migrated to lower-energy nanocluster sites.