van der Waals two-dimensional
(2D) semiconductors have emerged
as a class of materials with promising device characteristics owing
to the intrinsic band gap. For realistic applications, the ideal is
to modify the band gap in a controlled manner by a mechanism that
can be generally applied to this class of materials. Here, we report
the observation of a universally tunable band gap in the family of
bulk 2H transition metal dichalcogenides (TMDs) by
in situ surface doping of Rb atoms. A series of angle-resolved photoemission
spectra unexceptionally shows that the band gap of TMDs at the zone
corners is modulated in the range of 0.8–2.0 eV, which covers
a wide spectral range from visible to near-infrared, with a tendency
from indirect to direct band gap. A key clue to understanding the
mechanism of this band-gap engineering is provided by the spectroscopic
signature of symmetry breaking and resultant spin-splitting, which
can be explained by the formation of 2D electric dipole layers within
the surface bilayer of TMDs. Our results establish the surface Stark
effect as a universal mechanism of band-gap engineering on the basis
of the strong 2D nature of van der Waals semiconductors.