Integration of two-dimensional (2D) ferroelectric materials into van der Waals (vdW) heterostructures offers a promising strategy for enhancing photocatalytic efficiency. Herein, we reveal the electronic structures and photoexcited carrier dynamics in ${\mathrm{Cu}\mathrm{In}\mathrm{P}}_2{\mathrm{S}}_6/\mathrm{Si}\mathrm{C}$ heterostructures, using first-principles and nonadiabatic molecular dynamics simulations. Both the down- and up-polarization configurations exhibit a type-II charge-separation mechanism with ultrafast electron (hole) transfer within about 58 fs (110 fs), accompanied by long carrier lifetime scales of several nanoseconds. Notably, switching ${\mathrm{Cu}\mathrm{In}\mathrm{P}}_2{\mathrm{S}}_6$ ferroelectric polarization from up to down exhibits a low polarization-reversal energy barrier (0.32 eV) and reduces nonadiabatic coupling in the recombination process, due to weakened electron-phonon coupling and accelerated quantum decoherence, thereby suppressing electron-hole recombination and prolonging its lifetime from 1.04 to 3.44 ns. These findings demonstrate that ${\mathrm{Cu}\mathrm{In}\mathrm{P}}_2{\mathrm{S}}_6/\mathrm{Si}\mathrm{C}$ has great promise for photocatalysis using 2D ferroelectric vdW heterostructures.

Close

PrevNext

View figure in article

• Carrier dynamics
• Optoelectronics
• Photocatalysis
• Ferroelectrics
• Semiconductor compounds
• van der Waals systems
• Ab initio molecular dynamics
• High-throughput calculations