Jk. Wang et al., Vibrational dephasing dynamics at hydrogenated and deuterated semiconductor surfaces: Symmetry analysis, J CHEM PHYS, 113(12), 2000, pp. 5041-5052
Raman scattering has been performed on single crystal hydrogenated silicon
and germanium surfaces to investigate the temperature dependence of their v
ibrational spectral profiles. Based on a single-mode dephasing model for pu
re vibrational dephasing, the frequency shift and line broadening were anal
yzed to extract the following dephasing parameters: exchange mode frequency
, coupling strength, and friction parameter. The exchange modes for the XH
stretches on hydrogenated X(100) surfaces (X=Ge, Si, and C) are found to ma
tch their respective bending frequencies. The corresponding ones for hydrog
enated X(111) surfaces, on the other hand, are located within the bulk phon
on. This surface dependence of the exchange mode in surface vibrational dep
hasing dynamics is correlated with the structural relaxation and its associ
ated symmetry variation at surfaces. It is further confirmed by the experim
ents performed on deuterated semiconductor surfaces. A site-symmetry induce
d representation method is exploited to analyze the symmetry properties of
the surface vibrations on these two surfaces. This group-theoretical analys
is has revealed the selection rules of choosing the dominant exchange modes
on hydrogenated semiconductor surfaces. We have identified the exchange mo
des in the surface phonon spectra of these surfaces according to their symm
etry properties. (C) 2000 American Institute of Physics. [S0021-9606(00)701
36-X].