  A novel crystal configuration of sandwiched S-Mo-Se structure (Janus SMoSe)
at the monolayer limit has been synthesized and carefully characterized in this
work. By controlled sulfurization of monolayer MoSe2 the top layer of selenium
atoms are substituted by sulfur atoms while the bottom selenium layer remains
intact. The peculiar structure of this new material is systematically
investigated by Raman, photoluminescence and X-ray photoelectron spectroscopy
and confirmed by transmission-electron microscopy and time-of-flight secondary
ion mass spectrometry. Density-functional theory calculations are performed to
better understand the Raman vibration modes and electronic structures of the
Janus SMoSe monolayer, which are found to correlate well with corresponding
experimental results. Finally, high basal plane hydrogen evolution reaction
(HER) activity is discovered for the Janus monolayer and DFT calculation
implies that the activity originates from the synergistic effect of the
intrinsic defects and structural strain inherent in the Janus structure.
