An
atomic gradient passivation layer, (Ta,Mo)
x
(O,S)
y
, is designed to improve
the charge transportation and photoelectrochemical activity of CuInS2-based photoelectrodes. We found that Mo spontaneously diffused
to the a-TaO
x
layer during e-beam evaporation.
This result indicates that the gradient profile of MoO
x
/TaO
x
is formed in the
sublayer of (Ta,Mo)
x
(O,S)
y
. To understand the atomic-gradation effects of the
(Ta,Mo)
x
(O,S)
y
passive layer, the composition and (photo)electrochemical properties
have been characterized in detail. When this atomic gradient-passive
layer is applied to CuInS2-based photocathodes, promising
photocurrent and onset potential are seen without using Pt cocatalysts.
This is one of the highest activities among reported CuInS2 photocathodes, which are not combined with noble metal cocatalysts.
Excellent photoelectrochemical activity of the photoelectrode can
be mainly achieved by (1) the electron transient time improved due
to the conductive Mo-incorporated TaO
x
layer and (2) the boosted electrocatalytic activity by Mo
x
(O,S)
y
formation.