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Recent studies have revealed that the interlayer interaction intwo-dimensional (2D) layered materials is not simply of van der Waals characterbut could coexist with quasi-bonding character. Here we classify the interlayerquasi-bonding interactions into two main categories (I: homo-occupancyinteraction, II: hetero-occupancy interaction) according to the occupancy ofthe involved energy bands near the Fermi level. Then we investigate thequasi-bonding-interaction-induced band structure evolution of severalrepresentative 2D materials based on density functional theory calculations.Further calculations confirm that this classification is applicable to generic2D layered materials and provides a unified understanding of the total strengthof interlayer interaction, which is a synergetic effect of the van der Waalsattraction and the quasi-bonding interaction. The latter is stabilizing in maincategory II and destabilizing in main category I. Thus, the total interlayerinteraction strength is relatively stronger in category II and weaker incategory I.

Interlayer Quasi-Bonding Interactions in 2D Layered Materials: A Classification According to the Occupancy of Involved Energy Bands