Two-dimensional transition metal dichalcogenides, such
as MoS
2
, are intensely studied for applications in electronics.
However,
the difficulty of depositing large-area films of sufficient quality
under application-relevant conditions remains a major challenge. Herein,
we demonstrate deposition of polycrystalline, wafer-scale MoS
2
, TiS
2
, and WS
2
films of controlled
thickness at record-low temperatures down to 100 °C using plasma-enhanced
atomic layer deposition. We show that preventing excess sulfur incorporation
from H
2
S-based plasma is the key to deposition of crystalline
films, which can be achieved by adding H
2
to the plasma
feed gas. Film composition, crystallinity, growth, morphology, and
electrical properties of MoS
x
films prepared
within a broad range of deposition conditions have been systematically
characterized. Film characteristics are correlated with results of
field-effect transistors based on MoS
2
films deposited
at 100 °C. The capability to deposit MoS
2
on poly(ethylene
terephthalate) substrates showcases the potential of our process for
flexible devices. Furthermore, the composition control achieved by
tailoring plasma chemistry is relevant for all low-temperature plasma-enhanced
deposition processes of metal chalcogenides.