Tunable Electronic Structure and Carrier Dynamics Modulation via Ferroelectric Polarization in a CuInP2S6/C7N6 Heterostructure

Enhancing the transfer and separation efficiency of photogenerated carriers in heterostructures is critical for the development of high-efficiency photocatalysts. In this study, we propose a novel ferroelectric-based van der Waals heterostructure (CuInP2S6/C7N6) and investigate its electronic properties and carrier dynamics using first-principles calculations and nonadiabatic molecular dynamics (NAMD) simulations. The results revealed that the incorporation of CuInP2S6 significantly modulated the electronic structure and enabled efficient separation of photogenerated carriers. NAMD simulations indicated that carrier transfer and recombination in the CuInP2S6/C7N6 system followed a Type-II mechanism, with the Up-CuInP2S6/C7N6 configuration meeting the potential requirements for overall water splitting. Moreover, switching the polarization direction of CuInP2S6 effectively tunes its interfacial properties, electronic structure, and nonadiabatic coupling, thereby controlling the carrier transfer dynamics. Notably, the Up-CuInP2S6/C7N6 system exhibits superior photogenerated carrier separation efficiency, making it a promising candidate for photocatalytic applications. This work provides a novel strategy for regulating carrier dynamics and offers valuable insights into designing ferroelectric-based heterostructures for high-performance photocatalytic and optoelectronic devices.