Novel
materials suitable for optoelectronics are of great interest
due to limited and diminishing energy resources and the movement toward
a green earth. We report a simple film growth method to tune the S
composition, x from 1 to 2 in semiconductor ultrathin
SnS
x
films on quartz substrates, that
is, single phase SnS, single phase SnS2, and mixed phases
of both SnS and SnS2 by varying the sulfurization temperature
from 150 to 500 °C. Due to the ultrathin nature of the SnS
x
films, their structural and optical properties
are characterized and cross-checked by multiple surface-sensitive
techniques. The grazing incidence X-ray diffraction (GIXRD) shows
that the single phase SnS forms at 150 °C, single phase SnS2 forms at 350 °C and higher, and mixed phases of SnS
and SnS2 form at temperature between. GIXRD shows structures
of SnS film and SnS2 film are orthorhombic and 2H hexagonal,
respectively. To complement the GIXRD, the reflection high energy
electron diffraction pattern analysis shows that both pure phases
are polycrystalline on the surface. Raman spectra support existence
of pure phase SnS, pure phase SnS2, and mixed phases of
SnS and SnS2. X-ray photoelectron spectroscopy reveals
that the near surface stoichiometry of both single phase SnS and single
phase SnS2 are close to Sn/S ratios of 1:1 and 1:2, respectively.
UV–vis spectroscopy shows the optical absorption coefficient
of SnS film is higher than 105 cm–1 above
the optical bandgap of 1.38 ± 0.02 eV, an ideal optical absorber.
A two-terminal device made of SnS film grown on SiO2 substrates
shows good photoresponse. The SnS2 has an optical bandgap
of 2.21 ± 0.02 eV. A photoluminescence (PL) peak of SnS2 film is observed at ∼542 nm. Time-resolved PL of the single
phase ultrathin SnS2 film indicates a carrier lifetime
of 1.62 ns, longer than sub nanosecond lifetime from multilayer SnS2. Our comprehensive results show that ultrathin SnS and SnS2 films have the required properties for potential photodetectors
and solar cell applications but consume much less material as compared
with current thin film devices.