Angle-resolved photoemission spectroscopy has been employed to study i
n situ intercalation of the layered compound VSe2 with Cs. The results
show that the valence band structure of VSe2, which initially is of 3
D character, is transformed to become essentially 2D upon Cs intercala
tion. The changes, which go far beyond the rigid-band model, are succe
ssfully reproduced by self-consistent linear-augmented-plane-wave calc
ulations. This is the first report of a UHV compatible system where th
e dimensionality of the electronic structure can be controlled in situ
.