The thermal and photo-induced dissociation of H2S on the Ga-rich GaAs(
100) surface has been studied by synchrotron radiation soft X-ray phot
oelectron spectroscopy (SXPS), in conjunction with thermal desorption
spectroscopy (TDS) and low-energy electron diffraction (LEED). H2S ads
orbs in both molecular and dissociative forms at a surface temperature
of 90 K, with a saturation coverage of 0.57 ML. The molecularly adsor
bed H2S is unstable and desorbs/dissociates below 200 K; above 200 K,
only SH and atomic S species are left on the surface. The dissociation
of surface SH species is accompanied by the recombinative desorption
of H2S and H-2. This process is completed by similar to 450 K, above w
hich temperature surface sulfur atoms in two different chemical enviro
nments are observed. These sulfur atoms are attributed to Ga-S monomer
and dimer surface species, respectively. The former is converted to t
he latter upon annealing al 700-750 K. The annealed and dimerized GaAs
(100)/S surface shows a (2 x 1) LEED pattern in a broad sulfur coverag
e region. Both surface H2S and SH species dissociate readily upon UV l
aser or white light synchrotron radiation. At 193 nm, the initial phot
odissociation cross-sections for adsorbed H2S and SH species were esti
mated to be 6 x 10(-18) and 6 x 10(-19) cm(2), respectively. As a resu
lt of photodissociation, the amount of sulfur deposition can be signif
icantly increased. At sulfur coverages above 0.5 ML, annealing at 750
K results in two distinctively different sulfur states, which are attr
ibuted to surface and subsurface S, respectively. (C) 1997 Elsevier Sc
ience B.V.