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Lack of directional bonding between two-dimensional crystals like graphene ormonolayer transition metal dichalcogenides provides unusual freedom inselection of components for vertical van der Waals heterostructures. However,even for identical layers, their stacking, in particular the relative anglebetween their crystallographic directions, modifies properties of thestructure. We demonstrate that the interatomic coupling between twotwo-dimensional crystals can be determined from angle-resolved photoemissionspectra of a trilayer structure with one aligned and one twisted interface.Each of the interfaces provides complementary information and together theyenable self-consistent determination of the coupling. We parametrizeinteratomic coupling for carbon atoms by studying twisted trilayer graphene andshow that the result can be applied to structures with different twists andnumber of layers. Our approach demonstrates how to extract fundamentalinformation about interlayer coupling in a stack of two-dimensional crystalsand can be applied to many other van der Waals interfaces.

Determination of interatomic coupling between two-dimensional crystals using angle-resolved photoemission spectroscopy