Improved Carrier Separation and Recombination by Ferroelectric Polarization in the CuBiP2Se6/C2N Heterostructure: A Nonadiabatic Molecular Dynamics Study

The Journal of Physical Chemistry Letters. 2024. Vol. 15. No. 10. P. 2867–2875.

Jiang X., Tan J., Liu D., Feng Y., Chen K., Long R., Andrey S. Vasenko

The rapid recombination of photogenerated carriers heavily restrict the photocatalytic efficiency. Here, we propose a new strategy to improve catalytic efficiency based on ferroelectric van der Waals heterostructure (CuBiP2Se6/C2N). Combining density functional theory and nonadiabatic molecular dynamics (NAMD) method, we have systematically analyzed the ground state properties and carrier dynamics images in CuBiP2Se6/C2N heterostructure. Our calculations showed that the ferroelectric polarization of CuBiP2Se6 provides the internal driving force for the photogenerated carriers separation. NAMD results demonstrate that the excited state carrier transfer and recombination processes in the CuBiP2Se6/C2N are consistent with type-II mechanism. Meanwhile, construct the ferroelectric heterostructure can effectively prolong the carrier lifetime, from ~65.98 ps to ~124.54 ps. Moreover, the high quantum efficiency and tunable band edge positions mean that the CuBiP2Se6/C2N heterostructure is an excellent potential candidate material for photocatalytic water splitting.

Keywords: nonadiabatic molecular dynamics, Van der waals heterostructures, Ferroelectrics, Density functional theory (DFT), Water splitting, Photocatalytic performance

Publication based on the results of: Атомистическое моделирование динамики фотовозбуждённых состояний в новых материалах для солнечной энергетики (2024)