L. Simon et al., EPITAXIAL-GROWTH OF SI1-YCY ALLOYS CHARACTERIZED AS SELF-ORGANIZED, ORDERED, NANOMETER-SIZED C-RICH AGGREGATES IN MONOCRYSTALLINE SI, Physical review. B, Condensed matter, 54(15), 1996, pp. 10559-10564
Molecular-beam epitaxy deposition at 600 degrees C of Si in the presen
ce of a C precursor (C2H4) allows us to identify, in specific kinetic
conditions, a particular C accommodation mode in Si. By cross-sectiona
l transmission electron microscopy we observe a precipitation of nanom
etric, highly supersaturated C-rich aggregates (1-3 nm) excluding sili
con carbide or graphite formation. More surprisingly, these zero-dimen
sional aggregates are all self-organized in two-dimensional layers, pa
rallel to the growth surface, and reveal a periodicity of about 9 nm,
like in a ''natural'' superlattice. This indicates the occurrence of a
cyclic, growth-induced carbon precipitation into a defect-free epitax
ied Si matrix, forming a heterogeneous Si1-yCy alloy, in spite of cons
tant C and Si supplies all along the growth. The kinetic conditions go
verning this particular self-organization are specified in terms of Si
and C impinging rates at the growth surface. Moreover, by x-ray photo
electron diffraction on the C is core level, we demonstrate that a loc
al ordering, corresponding to that in the surrounding Si matrix, exist
s between the carbon atoms and their first Si neighbors inside the agg
regates. This result provides major arguments in favor of the existenc
e of the SinC phases recently predicted by ab initio calculations even
if the observation of structured electron, forward-scattering events
for next-nearest neighbors is hindered by probable distortions around
the C atoms due to high local strain. Finally, the periodic C precipit
ation is explained on the basis of recently developed concepts of surf
ace related C-solubility enhancements and sequential burying in C-enri
ched SinC phases of the accumulated C-rich surface layers. Such phases
could prove more stable than diluted carbon when forced to match sili
con.