Plasmon Excited Ultrahot Carriers and Negative Differential Photoresponse in a Vertical Graphene van der Waals Heterostructure.

Photogenerated nonequilibrium hot carriers play a key role in graphene's intriguing optoelectronic properties. Compared to conventional photoexcitation, plasmon excitation can be engineered to enhance and control the generation and dynamics of hot carriers. Here, we report an unusual negative differential photoresponse of plasmon-induced "ultrahot" electrons in a graphene-boron nitride-graphene tunneling junction. We demonstrate nanocrescent gold plasmonic nanostructures that substantially enhance the absorption of long-wavelength photons whose energy is greatly below the tunneling barrier and significantly boost the electron thermalization in graphene. We further analyze the generation and transfer of ultrahot electrons under different bias and power conditions. We find that the competition among thermionic emission, the carrier-cooling effect, and the field effect results in a hitherto unusual negative differential photoresponse in the photocurrent-bias plot. Our results not only exemplify a promising platform for detecting low-energy photons, enhancing the photoresponse, and reducing the dark current but also reveal the critically coupled pathways for harvesting ultrahot carriers.