We report on the low-temperature
growth of crystalline Ga2O3 films on Si, sapphire,
and glass substrates using plasma-enhanced
atomic layer deposition (PEALD) featuring a hollow-cathode plasma
source. Films were deposited by using triethylgallium (TEG) and Ar/O2 plasma as metal precursor and oxygen co-reactant, respectively.
Growth experiments have been performed within 150–240 °C
substrate temperature and 30–300 W radio-frequency (rf) plasma
power ranges. Additionally, each unit AB-type ALD cycle was followed
by an in situ Ar plasma annealing treatment, which
consisted of an extra (50–300 W) Ar plasma exposure for 20
s ending just before the next TEG pulse. The growth per cycle (GPC)
of the films without Ar plasma annealing step ranged between 0.69
and 1.31 Å/cycle, and as-grown refractive indices were between
1.67 and 1.75 within the scanned plasma power range. X-ray diffraction
(XRD) measurements showed that Ga2O3 films grown
without in situ Ar plasma annealing exhibited amorphous
character irrespective of substrate temperature and rf power values.
With the incorporation of the in situ Ar plasma annealing
process, the GPC of Ga2O3 films ranged between
0.76 and 1.03 Å/cycle along with higher refractive index values
of 1.75–1.79. The increased refractive index (1.79) and slightly
reduced GPC (1.03 Å/cycle) at 250 W plasma annealing indicated
possible densification and crystallization of the films. Indeed, X-ray
measurements confirmed that in situ plasma annealed
films grow in a monoclinic β-Ga2O3 crystal
phase. The film crystallinity and density further enhance (from 5.11
to 5.60 g/cm3) by increasing the rf power value used during in situ Ar plasma annealing process. X-ray photoelectron
spectroscopy (XPS) measurement of the β-Ga2O3 sample grown under optimal in situ plasma
annealing power (250 W) revealed near-ideal film stoichiometry (O/Ga
of ∼1.44) with relatively low carbon content (∼5 at.
%), whereas 50 W rf power treated film was highly non-stoichiometric
(O/Ga of ∼2.31) with considerably elevated carbon content.
Our results demonstrate the effectiveness of in situ Ar plasma annealing process to transform amorphous wide bandgap
oxide semiconductors into crystalline films without needing high-temperature
post-deposition annealing treatment.