Interlayer coupling between individual unit layers has played a critical role for layer-dependent properties in two-dimensional (2D) materials. While recent studies have revealed the significant degrees of interlayer interactions, the overall electronic structure of the 2D material has been mostly addressed by the intralayer interactions. Here, we report the direct observation of a highly dispersive single electronic band along the interlayer direction in puckered 2D PdSe2 as an experimental hallmark of strong interlayer couplings. Remarkably large band dispersion along kz-direction near Fermi level, which is even wider than the in-plane one, is observed by the angle-resolved photoemission spectroscopy measurement. Employing the X-ray absorption spectroscopy and density functional theory calculations, we reveal that the strong interlayer coupling in 2D PdSe2 originates from the unique directional bonding of Pd d orbitals associated with unexpected Pd 4d9 configuration, which consequently gives rise to the strong layer-dependency of the band gap.
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