我室李剑锋教授在 ACIE 上发表论文：In situ Raman probing of hot-electron transfer at Au-graphene interfaces with atomic layer accuracy

摘要：Plasmonic metals under photoexcitation can generate energetic hot electrons to directly induce chemical reactions. However, the capability and fundamental insights of the transportation of these hot electrons at plasmonic metal-2D material interfaces remain unclear. Herein, hot-electron transfer at Au-graphene interfaces has been in situ studied using surface-enhanced Raman spectroscopy (SERS) with atomic layer accuracy. Combining in situ SERS studies with density functional theory calculations, it is proved that hot electrons can be injected from plasmonic Au nanoparticles to graphene and directly penetrate graphene to trigger photocatalytic reactions. With increasing graphene layers, the transportation of hot electrons decays rapidly and would be completely blocked after five layers of graphene. Moreover, the transfer of hot electrons can be modulated by applying an external electric field, and the hot-electron transfer efficiency under electrochemical conditions is improved by over three times in the presence of a monolayer of graphene. These fundamental understandings about hot-electron transfer provide insightful information to promote the design of more efficient plasmonic materials and devices.

文章链接：https://onlinelibrary.wiley.com/doi/10.1002/anie.202112749