Ab Initio Quantum Dynamics Simulation of the Impact of Graphene on the Carrier Lifetime of the ZnV 2 O 6 Photocatalyst.

We used a nonadiabatic molecular dynamics simulation to determine the carrier dynamics of a graphene/ZnV 2 O 6 heterostructure in the search for an effective photocatalyst material. The C-2p orbital promotes the wave function overlap, guiding electrons to move between graphene and ZnV 2 O 6 , successfully achieving good mixing with the valence and conduction bands in ZnV 2 O 6 materials, which is conducive to supporting carrier migration. The overlap between graphene/ZnV 2 O 6 electrons and hole wave functions is less than that of ZnV 2 O 6 , and there is small absolute nonadiabatic coupling. The charge separation caused by graphene increases the carrier lifetime and prevents nonradiative electron-hole recombination. This study reveals the microscopic mechanism of extending the carrier lifetime of ZnV 2 O 6 by introducing graphene, providing useful insights for regulating the electronic structure, promoting electron transfer and ultrafast electron and hole transfer. This strategy provides design considerations for advanced photocatalytic materials.