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Quantum systems in confined geometries are host to novel physical phenomena.Examples include quantum Hall systems in semiconductors and Dirac electrons ingraphene. Interest in such systems has also been intensified by the recentdiscovery of a large enhancement in photoluminescence quantum efficiency and apotential route to valleytronics in atomically thin layers of transition metaldichalcogenides, MX2 (M = Mo, W; X = S, Se, Te), which are closely related tothe indirect to direct bandgap transition in monolayers. Here, we report thefirst direct observation of the transition from indirect to direct bandgap inmonolayer samples by using angle resolved photoemission spectroscopy onhigh-quality thin films of MoSe2 with variable thickness, grown by molecularbeam epitaxy. The band structure measured experimentally indicates a strongertendency of monolayer MoSe2 towards a direct bandgap, as well as a larger gapsize, than theoretically predicted. Moreover, our finding of a significantspin-splitting of 180 meV at the valence band maximum of a monolayer MoSe2 filmcould expand its possible application to spintronic devices.

Direct observation of the transition from indirect to direct bandgap in atomically thin epitaxial MoSe2