Direct observation of ultrafast plasmonic hot electron transfer in the strong coupling regime

Achieving strong coupling between plasmonic oscillators can significantly modulate their intrinsic optical properties. Here, we report the direct observation of ultrafast plasmonic hot electron transfer from an Au grating array to an MoS 2 monolayer in the strong coupling regime between localized surface plasmons (LSPs) and surface plasmon polaritons (SPPs). By means of femtosecond pump-probe spectroscopy, the measured hot electron transfer time is approximately 40 fs with a maximum external quantum yield of 1.65%. Our results suggest that strong coupling between LSPs and SPPs has synergetic effects on the generation of plasmonic hot carriers, where SPPs with a unique nonradiative feature can act as an ‘energy recycle bin’ to reuse the radiative energy of LSPs and contribute to hot carrier generation. Coherent energy exchange between plasmonic modes in the strong coupling regime can further enhance the vertical electric field and promote the transfer of hot electrons between the Au grating and the MoS 2 monolayer. Our proposed plasmonic strong coupling configuration overcomes the challenge associated with utilizing hot carriers and is instructive in terms of improving the performance of plasmonic opto-electronic devices. Surface plasmons: Nanostructured sandwich stirs up hot electrons A device that taps into two types of surface plasmon waves offers new opportunities to transform light energy into speedy semiconductor charges. When surface plasmons are confined to nanoscale dimensions, they can rapidly decay and produce “hot” electrons with high kinetic energy. Zheyu Fang from Peking University in Beijing, China, and colleagues have constructed a metal–insulator–metal sandwich structure that improves harvesting of hot electrons for applications including photodetectors. To increase extraction under laser excitation, the team coated the insulator with an electron-attracting molybdenum disulfide monolayer. They also identified surface plasmon polaritons—mobile waves at the metal–insulator interface—in the sandwich structure using a gold grating with variable dimensions as the upper metal layer. Laser conditions that coupled mobile and localized plasmons promoted hot electron production instead of thermal dissipation.