Proximity Engineering of the van der Waals Interaction in Multilayered Graphene

The van der Waals (vdW) interaction in two-dimensional (2D)-layered materials affects key characteristics of electronic devices, such as the contact resistance, with a vertical heterostructure geometry. While various functionalizations to manipulate the properties of 2D materials have shown issues such as defect generation or have a limited spatial range for the methods, engineering the vdW interaction in nondestructive ways for device applications has not been tried or properly achieved yet. Here, we introduce the proximity engineering of the vdW interaction in multilayered graphene, which is observed as modified interlayer distances and deviated stacking orders by Raman spectroscopy. A 2D electride, [Ca₂N]⁺·e^-, possessing a low-work function of 2.6 eV, was used to trigger an avalanche of electrons over tens of graphene layers, exceeding the conventional spatial-range limit (∼1 nm) by screening with a carrier density of 10¹⁴ cm^-2. Our proximity engineering reduces the vdW interaction in a nondestructive way and achieves a promising graphene-metal contact resistance of 500 ω·μm without using complicated edge contacts, which demonstrates a way to use moderately decoupled graphene layers for device applications.