Anisotropic Interlayer Potentials in C₃N/Graphene and C₃N/h-BN Heterostructures

Two-dimensional carbon nitride (C3N) has emerged as a graphene analog with tunable electronic and thermal properties, offering unique opportunities for heterostructure engineering. Integrating C3N with graphene or hexagonal boron nitride (h-BN) leads to moiré superlattices with tailored functionalities. However, accurate and scalable modeling of these systems remains a significant challenge due to the high computational cost of density functional theory (DFT) and the limitations of conventional isotropic force fields. Here, we develop anisotropic interlayer potentials for C3N/graphene and C3N/h-BN heterostructures, parameterized against many-body dispersion-corrected DFT data. Our approach explicitly captures anisotropic van der Waals (vdW) interactions within these heterostructures, enabling large-scale molecular dynamics simulations with near-DFT accuracy. The resulting force fields reproduce key interfacial properties, including binding and sliding energetics, mechanical behavior, phonon spectra, and moiré superlattices of C3N/graphene and C3N/h-BN heterostructures. This work establishes an efficient and accurate computational framework for simulating C3N-based vdW heterostructures, deepening our understanding of their emergent properties and advancing their applications.