Interlayer multi-level orbital coupling in 2D materials: Beyond the two-level paradigm
Abstract
The interlayer orbital interaction (IOI) of two-dimensional (2D) materials and their heterostructures triggers diverse property modifications, driving advancements in interlayer engineering. Previous investigations into IOI have primarily relied on a two-level interlayer interaction framework (one energy level per layer), which is insufficient for fully capturing band edge evolutions—even in prototypical 2D materials transitioning from monolayers to multilayers. The underlying reason lies in the multi-level nature of orbitals: taking the MoS2 monolayer as a paradigm, the pz orbitals of the two sulfur atoms (which dominate interlayer IOI) contribute to the wavefunctions of three energy levels (rather than one), enabled by pz–dz2–pz coupling along the S–Mo–S chemical bonds. Consequently, these three energy levels within a single layer can interact with a target energy level of interest (e.g., a band edge) in adjacent layers, provided they share the same orbital character. This gives rise to the “n-act-on-one” IOI mechanism, the core of multi-level interlayer interaction. Notably, this multi-level characteristic is inherent to general 2D materials. To address this, we extend the interlayer interaction model to a multi-level framework. This multi-level perspective offers deeper insights into the properties of 2D materials and helps property tuning from a perspective of combining intra- and interlayer orbital interactions.
Article Details
Journal Info
The Journal of Chemical Physics
American Institute of Physics
Authors (9)
Nie-Wei Wang
Hebei Research Center of the Basic Discipline for Computational Physics, Key Laboratory of Optic-Electronic Information and Materials of Hebei Province, College of Physics Science and Technology, Hebei University , Baoding 071002,
Xiao-Lin Zhao
Hebei Research Center of the Basic Discipline for Computational Physics, Key Laboratory of Optic-Electronic Information and Materials of Hebei Province, College of Physics Science and Technology, Hebei University , Baoding 071002,
Yu-Meng Gao
Hebei Research Center of the Basic Discipline for Computational Physics, Key Laboratory of Optic-Electronic Information and Materials of Hebei Province, College of Physics Science and Technology, Hebei University , Baoding 071002,
Xiao-Huan Lv
Hebei Research Center of the Basic Discipline for Computational Physics, Key Laboratory of Optic-Electronic Information and Materials of Hebei Province, College of Physics Science and Technology, Hebei University , Baoding 071002,
Peng-Lai Gong
Hebei Research Center of the Basic Discipline for Computational Physics, Key Laboratory of Optic-Electronic Information and Materials of Hebei Province, College of Physics Science and Technology, Hebei University , Baoding 071002,
Chen-Dong Jin
Hebei Research Center of the Basic Discipline for Computational Physics, Key Laboratory of Optic-Electronic Information and Materials of Hebei Province, College of Physics Science and Technology, Hebei University , Baoding 071002,
Hu Zhang
State Key Laboratory of Integrated Optoelectronics, College of Electronic Science and Engineering
Jiang-Long Wang
Hebei Research Center of the Basic Discipline for Computational Physics, Key Laboratory of Optic-Electronic Information and Materials of Hebei Province, College of Physics Science and Technology, Hebei University , Baoding 071002,
Xing-Qiang Shi
Hebei Research Center of the Basic Discipline for Computational Physics, Key Laboratory of Optic-Electronic Information and Materials of Hebei Province, College of Physics Science and Technology, Hebei University , Baoding 071002,